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Chirkov, Maksym ; Stiller, Gabriele ; Laeng, Alexandra ; Kellmann, Sylvia ; Clarmann, Thomas von ; Boone, Chris D. ; Elkins, James William ; Engel, Andreas ; Glatthor, Norbert ; Grabowski, Udo ; Harth, Christina M. ; Kiefer, Michael ; Kolonjari, Felicia ; Krummel, Paul B. ; Linden, Andrea ; Lunder, Chris Rene ; Miller, Benjamin R. ; Montzka, Stephen A. ; Mühle, Jens ; O'Doherty, Simon ; Orphal, Johannes ; Prinn, Ronald G. ; Toon, Geoffrey C. ; Vollmer, Martin K. ; Walker, Kaley A. ; Weiss, Ray F. ; Wiegele, Andreas ; Young, Dickon
We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in the reduced spectral resolution nominal observation mode. The data cover the period from January 2005 to April 2012 and the altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of modelled spectra to the measured limb spectral radiances. The spectral ν4-band at 816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The rate of linear growth in the lower latitudes lower stratosphere was about 6 to 7 pptv year−1 in the period 2005–2012. The profiles obtained were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and cryosampler balloon measurements. Between 13 and 22 km, average agreement within −3 to +5 pptv (MIPAS – ACE) with ACE-FTS v3.5 profiles is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15–50 pptv below 24 km and less than 10 pptv above 28 km. MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from the NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data. This is attributed to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10°-latitude/1-to-2-km-altitude bins. The relative linear variation was always positive, with relative increases of 40–70 % decade−1 in the tropics and global lower stratosphere, and up to 120 % decade−1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. Asian HCFC-22 emissions have become the major source of global upper tropospheric HCFC-22. In the upper troposphere, monsoon air, rich in HCFC-22, is instantaneously mixed into the tropics. In the middle stratosphere, between 20 and 30 km, the observed trend is inconsistent with the trend at the surface (corrected for the age of stratospheric air), hinting at circulation changes. There exists a stronger positive trend in HCFC-22 in the Southern Hemisphere and a more muted positive trend in the Northern Hemisphere, implying a potential change in the stratospheric circulation over the observation period.
Chirkov, Maksym ; Stiller, Gabriele ; Laeng, Alexandra ; Kellmann, Sylvia ; Clarmann, Thomas von ; Boone, Chris D. ; Elkins, James William ; Engel, Andreas ; Glatthor, Norbert ; Grabowski, Udo ; Harth, Christina M. ; Kiefer, Michael ; Kolonjari, Felicia ; Krummel, Paul B. ; Linden, Andrea ; Lunder, Chris Rene ; Miller, Benjamin R. ; Montzka, Stephen A. ; Mühle, Jens ; O'Doherty, Simon ; Orphal, Johannes ; Prinn, Ronald G. ; Toon, Geoffrey C. ; Vollmer, Martin K. ; Walker, Kaley A. ; Weiss, Ray F. ; Wiegele, Andreas ; Young, Dickon
We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in reduced spectral resolution nominal mode in the period from January 2005 to April 2012 from version 5.02 level-1b spectral data and covering an altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of measured limb spectral radiances to modelled spectra. The spectral v4-band at 816.5 ± 13 cm-1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The linear growth rate in the lower latitudes lower stratosphere was about 6 to 7 pptv yr-1 in the period 2005–2012. The obtained profiles were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and in situ cryosampler balloon measurements. Between 13 and 22 km, average agreement within -3 to +5 pptv (MIPAS–ACE) with ACE-FTS v3.5 pro files is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15– 50 pptv below 24 km and less than 10 pptv above 28 km. Obtained MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data, probably due to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10° latitude/1 to 2 km altitude bins. The relative linear variation was always positive, with relative increases of 40–70%decade-1 in the tropics and global lower stratosphere, and up to 120%decade-1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. In the middle stratosphere between 20 and 30 km, the observed trend is not consistent with the age of stratospheric air-corrected trend at ground, but stronger positive at the Southern Hemisphere and less strong increasing in the Northern Hemisphere, hinting towards changes in the stratospheric circulation over the observation period.
Kingslake, Jonathan ; Dias, Rebecca ; Dawson, Gerard R. ; Simon, Judit ; Goodwin, Guy M. ; Harmer, Catherine J. ; Morriss, Richard ; Brown, Susan ; Guo, Boliang ; Dourish, Colin T. ; Ruhé, Henricus G. ; Lever, Anne G. ; Veltman, Dick J. ; Schaik, Anneke van ; Deckert, Jürgen ; Reif, Andreas ; Stäblein, Michael ; Menke, Andreas ; Gorwood, Philip ; Voegeli, Géraldine ; Pérez, Victor ; Browning, Michael
Background: Antidepressant medication is commonly used to treat depression. However, many patients do not respond to the first medication prescribed and improvements in symptoms are generally only detectable by clinicians 4–6 weeks after the medication has been initiated. As a result, there is often a long delay between the decision to initiate an antidepressant medication and the identification of an effective treatment regimen.
Previous work has demonstrated that antidepressant medications alter subtle measures of affective cognition in depressed patients, such as the appraisal of facial expression. Furthermore, these cognitive effects of antidepressants are apparent early in the course of treatment and can also predict later clinical response. This trial will assess whether an electronic test of affective cognition and symptoms (the Predicting Response to Depression Treatment Test; PReDicT Test) can be used to guide antidepressant treatment in depressed patients and, therefore, hasten treatment response compared to a control group of patients treated as usual.
Methods/design: The study is a randomised, two-arm, multi-centre, open-label, clinical investigation of a medical device, the PReDicT Test. It will be conducted in five European countries (UK, France, Spain, Germany and the Netherlands) in depressed patients who are commencing antidepressant medication. Patients will be randomised to treatment guided by the PReDicT Test (PReDicT arm) or to Treatment as Usual (TaU arm). Patients in the TaU arm will be treated as per current standard guidelines in their particular country. Patients in the PReDicT arm will complete the PReDicT Test after 1 (and if necessary, 2) weeks of treatment. If the test indicates non-response to the treatment, physicians will be advised to immediately alter the patient’s antidepressant therapy by dose escalation or switching to another compound. The primary outcome of the study is the proportion of patients showing a clinical response (defined as 50% or greater decrease in baseline scores of depression measured using the Quick Inventory of Depressive Symptoms – Self-Rated questionnaire) at week 8. Health economic and acceptability data will also be collected and analysed.
Discussion: This trial will test the clinical efficacy, cost-effectiveness and acceptability of using the novel PReDicT Test to guide antidepressant treatment selection in depressed patients.
Trial registration: ClinicalTrials.gov, ID: NCT02790970. Registered on 30 March 2016.
Harter, Philipp ; Hauke, Jan ; Heitz, Florian ; Reuss, Alexander ; Kommoss, Stefan ; Marmé, Frederik ; Heimbach, André ; Prieske, Katharina ; Richters, Lisa ; Burges, Alexander ; Neidhardt, Guido ; Gregorio, Nikolaus de ; Balat, Ahmed el- ; Hilpert, Felix ; Meier, Werner ; Kimmig, Rainer ; Kast, Karin ; Sehouli, Jalid ; Baumann, Klaus ; Jackisch, Christian ; Park-Simon, Tjoung-Won ; Hanker, Lars ; Kröber, Sandra ; Pfisterer, Jacobus ; Gevensleben, Heidrun ; Schnelzer, Andreas ; Dietrich, Dimo ; Neunhöffer, Tanja ; Krockenberger, Mathias Heinric ; Brucker, Sara ; Nürnberg, Peter ; Thiele, Holger ; Altmüller, Janine ; Lamla, Josefin ; Elser, Gabriele ; Du Bois, Andreas ; Hahnen, Eric Thomas ; Schmutzler, Rita Katharina
Background: Identification of families at risk for ovarian cancer offers the opportunity to consider prophylactic surgery thus reducing ovarian cancer mortality. So far, identification of potentially affected families in Germany was solely performed via family history and numbers of affected family members with breast or ovarian cancer. However, neither the prevalence of deleterious variants in BRCA1/2 in ovarian cancer in Germany nor the reliability of family history as trigger for genetic counselling has ever been evaluated.
Methods: Prospective counseling and germline testing of consecutive patients with primary diagnosis or with platinum-sensitive relapse of an invasive epithelial ovarian cancer. Testing included 25 candidate and established risk genes. Among these 25 genes, 16 genes (ATM, BRCA1, BRCA2, CDH1, CHEK2, MLH1, MSH2, MSH6, NBN, PMS2, PTEN, PALB2, RAD51C, RAD51D, STK11, TP53) were defined as established cancer risk genes. A positive family history was defined as at least one relative with breast cancer or ovarian cancer or breast cancer in personal history.
Results: In total, we analyzed 523 patients: 281 patients with primary diagnosis of ovarian cancer and 242 patients with relapsed disease. Median age at primary diagnosis was 58 years (range 16–93) and 406 patients (77.6%) had a high-grade serous ovarian cancer. In total, 27.9% of the patients showed at least one deleterious variant in all 25 investigated genes and 26.4% in the defined 16 risk genes. Deleterious variants were most prevalent in the BRCA1 (15.5%), BRCA2 (5.5%), RAD51C (2.5%) and PALB2 (1.1%) genes. The prevalence of deleterious variants did not differ significantly between patients at primary diagnosis and relapse. The prevalence of deleterious variants in BRCA1/2 (and in all 16 risk genes) in patients <60 years was 30.2% (33.2%) versus 10.6% (18.9%) in patients ≥60 years. Family history was positive in 43% of all patients. Patients with a positive family history had a prevalence of deleterious variants of 31.6% (36.0%) versus 11.4% (17.6%) and histologic subtype of high grade serous ovarian cancer versus other showed a prevalence of deleterious variants of 23.2% (29.1%) and 10.2% (14.8%), respectively. Testing only for BRCA1/2 would miss in our series more than 5% of the patients with a deleterious variant in established risk genes.
Conclusions: 26.4% of all patients harbor at least one deleterious variant in established risk genes. The threshold of 10% mutation rate which is accepted for reimbursement by health care providers in Germany was observed in all subgroups analyzed and neither age at primary diagnosis nor histo-type or family history sufficiently enough could identify a subgroup not eligible for genetic counselling and testing. Genetic testing should therefore be offered to every patient with invasive epithelial ovarian cancer and limiting testing to BRCA1/2 seems to be not sufficient.
Syndikus, Ina ; Petri, Marina ; Macchiavelli, Augusto O. ; Paschalis, Stefanos ; Bertulani, Carlos A. ; Aumann, Thomas ; Álvarez-Pol, Héctor ; Atar, Leyla ; Beceiro-Novo, Saul ; Benlliure Anaya, Jose Fernando ; Boillos Betete, Juan Manuel ; Boretzky, Konstanze ; Garcia Borge, Maria José ; Brown, B. Alex ; Caamaño, Manuel ; Caesar, Christoph ; Casarejos Ruiz, Enrique ; Catford, Wilton N. ; Cederkäll, Joakim ; Chakraborty, S. ; Chulkov, Leonid V. ; Cortina Gil, Dolores ; Cravo, Edgar ; Crespo, Raquel ; Datta Pramanik, Ushasi ; Dillmann, Iris ; Díaz Fernández, Paloma ; Elekes, Zoltán ; Enders, Joachim ; Farinon, Fabio ; Fraile Prieto, Luis Mario ; Galaviz Redondo, Daniel ; Geissel, Hans ; Gernhäuser, Roman ; Golubev, Pavel ; Göbel, Kathrin ; Heil, Michael ; Heine, Marcel ; Heinz, Andreas ; Henriques Correia, Ana Maria ; Holl, Matthias ; Johansson, Håkan T. ; Jonson, Björn ; Kalantar-Nayestanaki, Nasser ; Kanungo, Rituparna ; Kelic-Heil, Aleksandra ; Kröll, Thorsten ; Kurz, Nikolaus ; Langer, Christoph ; Le Bleis, Tudi ; Machado, Jorge ; Marganiec-Gałązka, Justyna ; Nácher González, Enrique ; Nilsson, Thomas ; Nociforo, Chiara ; Panin, Valerii ; Perea Martinez, Angel ; Pietri, Stephane ; Plag, Ralf ; Rahaman, Anisur ; Reifarth, René ; Revel, Aldric ; Ribeiro Jimenez, Guillermo ; Rigollet, Catherine ; Rossi, Dominic M. ; Savran, Deniz ; Scheit, Heiko ; Simon, Haik ; Sorlin, Olivier ; Tengblad, Olof ; Togano, Yasuhiro ; Vandebrouck, Marine ; Volkov, Vasily ; Wamers, Felix ; Wheldon, Carl ; Wilson, Gemma Louise ; Winfield, John S. ; Weick, Helmut ; Woods, Philip John ; Yakorev, Dmitry ; Zhukov, Mikhail V. ; Zilges, Andreas ; Zuber, Kai
The evolution of the traditional nuclear magic numbers away from the valley of stability is an active field of research. Experimental efforts focus on providing key spectroscopic information that will shed light into the structure of exotic nuclei and understanding the driving mechanism behind the shell evolution. In this work, we investigate the spin-orbit shell gap towards the neutron dripline. To do so, we employed (p,2p) quasi-free scattering reactions to measure the proton component of the state of 16,18,20C. The experimental findings support the notion of a moderate reduction of the proton spin-orbit splitting, at variance to recent claims for a prevalent magic number towards the neutron dripline.
Adams, John ; Adler, Clemens ; Ahammed, Zubayer ; Allgower, Chris ; Amonett, John ; Anderson, Bryon D. ; Anderson, Mike ; Averichev, Georgy S. ; Balewski, Jan ; Barannikova, Olga ; Barnby, Lee Stuart ; Baudot, Jérome ; Bekele, Selemon ; Belaga, Victoria Vladimirovna ; Bellwied, Rene ; Berger, Jens ; Bichsel, Hans ; Billmeier, Anja ; Bland, Leslie C. ; Blyth, Charles O. ; Bonner, Billy E. ; Boucham, Abdelkrim ; Brandin, Andrei V. ; Bravar, Alessandro ; Cadman, R. V. ; Caines, Helen Louise ; Calderón de la Barca Sánchez, Manuel ; Cardenas, Andrés ; Carroll, J. ; Castillo Castellanos, Javier Ernesto ; Castro, M. ; Cebra, Daniel A. ; Chaloupka, Petr ; Chattopadhyay, S. ; Chen, Y. ; Chernenko, S. P. ; Cherney, Michael Gerard ; Chikanian, Alexei ; Choi, B. ; Christie, William ; Coffin, Jean Pierre ; Cormier, Thomas Michael ; Corral, M. M. ; Cramer, John G. ; Crawford, Henry J. ; Derevschikov, Anatoly A. ; Didenko, Lidia ; Dietel, Thomas ; Draper, James E. ; Dunin, V. B. ; Dunlop, James C. ; Eckardt, Volker ; Efimov, Leonid G. ; Emelianov, V. ; Engelage, Jon M. ; Eppley, Geary Wareham ; Erazmus, Barbara Ewa ; Fachini, Patricia ; Faine, V. ; Faivre, Julien ; Fatemi, Renee H. ; Filimonov, Kirill ; Finch, Evan ; Fisyak, Yuri V. ; Flierl, Dominik Bernhard ; Foley, K. J. ; Fu, J. ; Gagliardi, Carl A. ; Gagunashvili, N. ; Gans, J. ; Gaudichet, L. ; Germain, Marie ; Geurts, Frank ; Ghazikhanian, Vahe ; Grachov, Oleg A. ; Grigoriev, Vladislav A. ; Guedon, M. ; Guertin, Steven M. ; Gushin, E. ; Hallman, Timothy J. ; Hardtke, David H. ; Harris, John W. ; Heinz, Mark Thomas ; Henry, Thomas W. ; Heppelmann, Steven Francis ; Herston, T. ; Hippolyte, Boris ; Hirsch, Andrew S. ; Hjort, Eric ; Hoffmann, Gerald W. ; Horsley, M. ; Huang, Huan Zhong ; Humanic, Thomas J. ; Igo, George J. ; Ishihara, A. ; Ivanshin, Yu. I. ; Jacobs, Peter Martin ; Jacobs, William W. ; Janik, Michał ; Johnson, I. ; Jones, Peter Graham ; Judd, Eleanor G. ; Kaneta, Kaneta ; Kaplan, Morton ; Keane, Declan ; Kiryluk, Joanna ; Kisiel, Adam Ryszard ; Klay, Jennifer Lynn ; Klein, Spencer Robert ; Klyachko, A. ; Kollegger, Thorsten ; Konstantinov, A. S. ; Kopytine, M. ; Kotchenda, L. ; Kovalenko, A. D. ; Kramer, M. ; Kravtsov, Peter ; Krueger, Keith William ; Kuhn, Christian Claude ; Kulikov, Anatoly I. ; Kunde, Gerd J. ; Kunz, Christopher Lee ; Kutuev, R. Kh. ; Kuznetsov, A. A. ; Lamont, Matthew A. C. ; Landgraf, Jeffery M. ; Lange, S. ; Lansdell, Curtis Patrick Leon ; Lasiuk, Brian ; Laue, Frank ; Lauret, Jerome ; Lebedev, Alexei ; Lednický, Richard ; Leontiev, V. M. ; LeVine, Micheal J. ; Li, Q. ; Lindenbaum, Sam J. ; Lisa, Michael A. ; Liu, F. ; Liu, L. ; Liu, Z. ; Liu, Q. J. ; Ljubicic, Tonko A. ; Llope, William Joseph ; Long, H. ; Longacre, Ronald S. ; Lopez-Noriega, M. ; Love, William A. ; Ludlam, Thomas ; Lynn, David ; Ma, Jing-guo ; Magestro, Daniel ; Majka, Richard Daniel ; Margetis, Spyridon ; Markert, Christina ; Martin, L. ; Marx, Jay N. ; Matis, Howard S. ; Matulenko, Yuri A. ; McShane, Tom S. ; Meissner, F. ; Melnick, Yu. ; Meščanin, Aleksei P. ; Messer, Matthias ; Miller, M. L. ; Milosevich, Z. ; Minaev, Nikolai G. ; Mitchell, J. ; Moore, C. F. ; Morozov, V. ; de Moura, M. M. ; Munhoz, Marcelo Gameiro ; Nelson, John M. ; Nevski, P. ; Nikitin, Vladimir A. ; Nogach, Larisa V. ; Norman, B. ; Nurušev, Sandibek B. ; Odyniec, Grazyna Janina ; Ogawa, Akio ; Okorokov, Vitaly A. ; Oldenburg, Markus D. ; Olson, Douglas L. ; Paic, Guy ; Pandey, S. U. ; Panebratsev, Yuri ; Panitkin, Sergei Yurievich ; Pavlinov, A. I. ; Pawlak, Tomasz Jan ; Perevoztchikov, V. ; Peryt, Wiktor Stanislaw ; Petrov, V. A ; Planinic, Mirko ; Pluta, Jan Marian ; Porile, Norbert T. ; Porter, Jeffrey Brent ; Poskanzer, Arthur M. ; Potrebenikova, E. ; Prindle, Duncan J. ; Pruneau, Claude A. ; Putschke, Jörn H. ; Rai, Gulshan ; Rakness, Gregory L. ; Ravel, Olivier ; Ray, Robert L. ; Razin, Sergej V. ; Reichhold, Dennis Michael ; Reid, Jeffrey G. ; Renault, G. ; Retiere, Fabrice ; Ridiger, Alexey ; Ritter, Hans Georg ; Roberts, Jabus B. ; Rogachevski, O. V. ; Romero, Juan L. ; Rose, A. ; Roy, Christelle Sophie ; Rykov, Vladimir L. ; Sakrejda, Iwona ; Salur, Sevil ; Sandweiss, Jack H. ; Savin, Igor A. ; Schambach, Joachim ; Scharenberg, Rolf Paul ; Schmitz, Norbert ; Schroeder, Lee S. ; Schüttauf, Andreas ; Schweda, Kai ; Seger, Janet Elizabeth ; Seliverstov, D. ; Seyboth, Peter ; Shahaliev, Ehtiram ; Shestermanov, Konstantin E. ; Shimanskii, S. S. ; Simon, F. ; Skoro, Goran P. ; Smirnov, Nikolai ; Snellings, Raimond ; Sorensen, Paul Richard ; Sowinski, James ; Spinka, Harold. M. ; Srivastava, Brijesh Kumar ; Stephenson, Edward J. ; Stock, Reinhard ; Stolpovsky, Alexander ; Strichanov, Michail Nikolaevič ; Stringfellow, Blair ; Struck, Christof ; Suaide, Alexandre Alarcon do Passo ; Sugarbaker, Evan R. ; Suire, Christophe Pierre ; Šumbera, Michal ; Surrow, Bernd ; Symons, Timothy James MacNeil ; de Toledo, A. Szanto ; Szarwas, Piotr ; Tai, An ; Takahashi, Jun ; Tang, Aihong ; Thein, Dylan ; Thomas, James H. ; Thompson, M. ; Tikhomirov, V. ; Tokarev, Mikhail V. ; Tonjes, Marguerite Belt ; Trainor, Thomas A. ; Trentalange, Stephen ; Tribble, Robert E. ; Trofimov, V. ; Tsai, Oleg D. ; Ullrich, Thomas ; Underwood, David G. ; Van Buren, Gene ; Molen, A. M. Vander ; Vasilevski, I. M. ; Vasiliev, Alexander Nikolaevich ; Vigdor, Steven E. ; Voloshin, Sergei ; Wang, F. ; Ward, H. ; Watson, J. W. ; Wells, R. ; Westfall, Gary D. ; Whitten, Charles A. ; Wieman, Howard ; Willson, Robert ; Wissink, Scott W. ; Witt, Richard ; Wood, J. ; Xu, N. ; Xu, Z. ; Yakutin, A. E. ; Yamamoto, E. ; Yang, J. ; Yepes, Pablo P. ; Yurevich, Vladimir Yurevich ; Zanevski, Y. V. ; Zborovský, I. ; Zhang, Haitao ; Zhang, W. M. ; Zoulkarneev, R. ; Zubarev, A. N.
The balance function is a new observable based on the principle that charge is locally conserved when particles are pair produced. Balance functions have been measured for charged particle pairs and identified charged pion pairs in Au+Au collisions at sqrt[sNN]=130 GeV at the Relativistic Heavy Ion Collider using STAR. Balance functions for peripheral collisions have widths consistent with model predictions based on a superposition of nucleon-nucleon scattering. Widths in central collisions are smaller, consistent with trends predicted by models incorporating late hadronization.
Adler, Clemens ; Ahammed, Zubayer ; Allgower, Chris ; Amonett, John ; Anderson, Bryon D. ; Anderson, Mike ; Averichev, Georgy S. ; Balewski, Jan ; Barannikova, Olga ; Barnby, Lee Stuart ; Baudot, Jérome ; Bekele, Selemon ; Belaga, Victoria Vladimirovna ; Bellwied, Rene ; Berger, Jens ; Bichsel, Hans ; Billmeier, Anja ; Bland, Leslie C. ; Blyth, Charles O. ; Bonner, Billy E. ; Boucham, Abdelkrim ; Brandin, Andrei V. ; Bravar, Alessandro ; Cadman, R. V. ; Caines, Helen Louise ; Calderón de la Barca Sánchez, Manuel ; Cardenas, Andrés ; Carroll, J. ; Castillo Castellanos, Javier Ernesto ; Castro, M. ; Cebra, Daniel A. ; Chaloupka, Petr ; Chattopadhyay, S. ; Chen, Y. ; Chernenko, S. P. ; Cherney, Michael Gerard ; Chikanian, Alexei ; Choi, B. ; Christie, William ; Coffin, Jean Pierre ; Cormier, Thomas Michael ; Corral, M. M. ; Cramer, John G. ; Crawford, Henry J. ; Derevschikov, Anatoly A. ; Didenko, Lidia ; Dietel, Thomas ; Draper, James E. ; Dunin, V. B. ; Dunlop, James C. ; Eckardt, Volker ; Efimov, Leonid G. ; Emelianov, V. ; Engelage, Jon M. ; Eppley, Geary Wareham ; Erazmus, Barbara Ewa ; Fachini, Patricia ; Faine, V. ; Faivre, Julien ; Fatemi, Renee H. ; Filimonov, Kirill ; Finch, Evan ; Fisyak, Yuri V. ; Flierl, Dominik Bernhard ; Foley, K. J. ; Fu, J. ; Gagliardi, Carl A. ; Gagunashvili, N. ; Gans, J. ; Gaudichet, L. ; Germain, Marie ; Geurts, Frank ; Ghazikhanian, Vahe ; Grachov, Oleg A. ; Grigoriev, Vladislav A. ; Guedon, M. ; Gushin, E. ; Hallman, Timothy J. ; Hardtke, David H. ; Harris, John W. ; Henry, Thomas W. ; Heppelmann, Steven Francis ; Herston, T. ; Hippolyte, Boris ; Hirsch, Andrew S. ; Hjort, Eric ; Hoffmann, Gerald W. ; Horsley, M. ; Huang, Huan Zhong ; Humanic, Thomas J. ; Igo, George J. ; Ishihara, A. ; Ivanshin, Yu. I. ; Jacobs, Peter Martin ; Jacobs, William W. ; Janik, Michał ; Johnson, I. ; Jones, Peter Graham ; Judd, Eleanor G. ; Kaneta, Kaneta ; Kaplan, Morton ; Keane, Declan ; Kiryluk, Joanna ; Kisiel, Adam Ryszard ; Klay, Jennifer Lynn ; Klein, Spencer Robert ; Klyachko, A. ; Kollegger, Thorsten ; Konstantinov, A. S. ; Kopytine, M. ; Kotchenda, L. ; Kovalenko, A. D. ; Kramer, M. ; Kravtsov, Peter ; Krueger, Keith William ; Kuhn, Christian Claude ; Kulikov, Anatoly I. ; Kunde, Gerd J. ; Kunz, Christopher Lee ; Kutuev, R. Kh. ; Kuznetsov, A. A. ; Lakehal-Ayat, L. ; Lamont, Matthew A. C. ; Landgraf, Jeffery M. ; Lange, S. ; Lansdell, Curtis Patrick Leon ; Lasiuk, Brian ; Laue, Frank ; Lauret, Jerome ; Lebedev, Alexei ; Lednický, Richard ; Leontiev, V. M. ; LeVine, Micheal J. ; Li, Q. ; Lindenbaum, Sam J. ; Lisa, Michael A. ; Liu, F. ; Liu, L. ; Liu, Z. ; Liu, Q. J. ; Ljubicic, Tonko A. ; Llope, William Joseph ; LoCurto, G. ; Long, H. ; Longacre, Ronald S. ; Lopez-Noriega, M. ; Love, William A. ; Ludlam, Thomas ; Lynn, David ; Ma, Jing-guo ; Magestro, Daniel ; Majka, Richard Daniel ; Margetis, Spyridon ; Markert, Christina ; Martin, L. ; Marx, Jay N. ; Matis, Howard S. ; Matulenko, Yuri A. ; McShane, Tom S. ; Meissner, F. ; Melnick, Yu. ; Meščanin, Aleksei P. ; Messer, Matthias ; Miller, M. L. ; Milosevich, Z. ; Minaev, Nikolai G. ; Mitchell, J. ; Moore, C. F. ; Morozov, V. ; de Moura, M. M. ; Munhoz, Marcelo Gameiro ; Nelson, John M. ; Nevski, P. ; Nikitin, Vladimir A. ; Nogach, Larisa V. ; Norman, B. ; Nurušev, Sandibek B. ; Odyniec, Grazyna Janina ; Ogawa, Akio ; Okorokov, Vitaly A. ; Oldenburg, Markus D. ; Olson, Douglas L. ; Paic, Guy ; Pandey, S. U. ; Panebratsev, Yuri ; Panitkin, Sergei Yurievich ; Pavlinov, A. I. ; Pawlak, Tomasz Jan ; Perevoztchikov, V. ; Peryt, Wiktor Stanislaw ; Petrov, V. A ; Planinic, Mirko ; Pluta, Jan Marian ; Porile, Norbert T. ; Porter, Jeffrey Brent ; Poskanzer, Arthur M. ; Potrebenikova, E. ; Prindle, Duncan J. ; Pruneau, Claude A. ; Putschke, Jörn H. ; Rai, Gulshan ; Rakness, Gregory L. ; Ravel, Olivier ; Ray, Robert L. ; Razin, Sergej V. ; Reichhold, Dennis Michael ; Reid, Jeffrey G. ; Renault, G. ; Retiere, Fabrice ; Ridiger, Alexey ; Ritter, Hans Georg ; Roberts, Jabus B. ; Rogachevski, O. V. ; Romero, Juan L. ; Rose, A. ; Roy, Christelle Sophie ; Rykov, Vladimir L. ; Sakrejda, Iwona ; Salur, Sevil ; Sandweiss, Jack H. ; Savin, Igor A. ; Schambach, Joachim ; Scharenberg, Rolf Paul ; Schmitz, Norbert ; Schroeder, Lee S. ; Schüttauf, Andreas ; Schweda, Kai ; Seger, Janet Elizabeth ; Seliverstov, D. ; Seyboth, Peter ; Shahaliev, Ehtiram ; Shestermanov, Konstantin E. ; Shimanskii, S. S. ; Simon, F. ; Skoro, Goran P. ; Smirnov, Nikolai ; Snellings, Raimond ; Sorensen, Paul Richard ; Sowinski, James ; Spinka, Harold. M. ; Srivastava, Brijesh Kumar ; Stephenson, Edward J. ; Stock, Reinhard ; Stolpovsky, Alexander ; Strichanov, Michail Nikolaevič ; Stringfellow, Blair ; Struck, Christof ; Suaide, Alexandre Alarcon do Passo ; Sugarbaker, Evan R. ; Suire, Christophe Pierre ; Šumbera, Michal ; Surrow, Bernd ; Symons, Timothy James MacNeil ; Toledo, Alejandro Szanto de ; Szarwas, Piotr ; Tai, An ; Takahashi, Jun ; Tang, Aihong ; Thein, Dylan ; Thomas, James H. ; Thompson, M. ; Tikhomirov, V. ; Tokarev, Mikhail V. ; Tonjes, Marguerite Belt ; Trainor, Thomas A. ; Trentalange, Stephen ; Tribble, Robert E. ; Trofimov, V. ; Tsai, Oleg D. ; Ullrich, Thomas ; Underwood, David G. ; Van Buren, Gene ; VanderMolen, A. M. ; Vasilevski, I. M. ; Vasiliev, Alexander Nikolaevich ; Vigdor, Steven E. ; Voloshin, Sergei ; Wang, F. ; Ward, H. ; Watson, J. W. ; Wells, R. ; Westfall, Gary D. ; Whitten, Charles A. ; Wieman, Howard ; Willson, Robert ; Wissink, Scott W. ; Witt, Richard ; Wood, J. ; Xu, N. ; Xu, Z. ; Yakutin, A. E. ; Yamamoto, E. ; Yang, J. ; Yepes, Pablo P. ; Yurevich, Vladimir Yurevich ; Zanevski, Y. V. ; Zborovský, I. ; Zhang, Haitao ; Zhang, W. M. ; Zoulkarneev, R. ; Zubarev, A. N.
Azimuthal anisotropy (v2) and two-particle angular correlations of high pT charged hadrons have been measured in Au+Au collisions at sqrt[sNN]=130 GeV for transverse momenta up to 6 GeV/c, where hard processes are expected to contribute significantly. The two-particle angular correlations exhibit elliptic flow and a structure suggestive of fragmentation of high pT partons. The monotonic rise of v2(pT) for pT<2 GeV/c is consistent with collective hydrodynamical flow calculations. At pT>3 GeV/c, a saturation of v2 is observed which persists up to pT=6 GeV/c.
Castagnola, Elio ; Bagnasco, Francesca ; Mesini, Alessio ; Agyeman, Philipp K. A. ; Ammann, Roland A. ; Carlesse, Fabianne ; Pablo, Maria Elena Santolaya de ; Groll, Andreas H. ; Haeusler, Gabrielle M. ; Lehrnbecher, Thomas ; Simon, Arne ; D'Amico, Maria Rosaria ; Duong, Austin ; Idelevich, Evgeny A. ; Luckowitsch, Marie ; Meli, Mariaclaudia ; Menna, Giuseppe ; Palmert, Sasha ; Russo, Giovanna ; Sarno, Marco ; Solopova, Galina ; Tondo, Annalisa ; Traubici, Yona ; Sung, Lillian
Bloodstream infections (BSI) are a severe complication of antineoplastic chemotherapy or hematopoietic stem cell transplantation (HSCT), especially in the presence of antibiotic resistance (AR). A multinational, multicenter retrospective study in patients aged ≤ 18 years, treated with chemotherapy or HSCT from 2015 to 2017 was implemented to analyze AR among non-common skin commensals BSI. Risk factors associated with AR, intensive care unit (ICU) admission and mortality were analyzed by multilevel mixed effects or standard logistic regressions. A total of 1291 BSIs with 1379 strains were reported in 1031 patients. Among Gram-negatives more than 20% were resistant to ceftazidime, cefepime, piperacillin-tazobactam and ciprofloxacin while 9% was resistant to meropenem. Methicillin-resistance was observed in 17% of S. aureus and vancomycin resistance in 40% of E. faecium. Previous exposure to antibiotics, especially to carbapenems, was significantly associated with resistant Gram-negative BSI while previous colonization with methicillin-resistant S. aureus was associated with BSI due to this pathogen. Hematological malignancies, neutropenia and Gram-negatives resistant to >3 antibiotics were significantly associated with higher risk of ICU admission. Underlying disease in relapse/progression, previous exposure to antibiotics, and need of ICU admission were significantly associated with mortality. Center-level variation showed a greater impact on AR, while patient-level variation had more effect on ICU admission and mortality. Previous exposure to antibiotics or colonization by resistant pathogens can be the cause of AR BSI. Resistant Gram-negatives are significantly associated with ICU admission and mortality, with a significant role for the treating center too. The significant evidence of center-level variations on AR, ICU admission and mortality, stress the need for careful local antibiotic stewardship and infection control programs.
Dietrich, Sascha ; Oleś, Małgorzata ; Lu, Junyan ; Sellner, Leopold ; Anders, Simon ; Velten, Britta ; Wu, Bian ; Hüllein, Jennifer ; Silva Liberio, Michelle da ; Walther, Tatjana ; Wagner, Lena ; Rabe, Sophie ; Ghidelli-Disse, Sonja ; Bantscheff, Marcus ; Oleś, Andrzej K. ; Słabicki, Mikołaj ; Mock, Andreas ; Oakes, Christopher C. ; Wang, Shihui ; Oppermann, Sina ; Lukas, Marina ; Kim, Vladislav ; Sill, Martin ; Benner, Axel ; Jauch, Anna ; Sutton, Lesley-Ann ; Young, Emma ; Rosenquist, Richard ; Liu, Xiyang ; Jethwa, Alexander ; Lee, Kwang Seok ; Lewis, Joe ; Putzker, Kerstin ; Lutz, Christoph ; Rossi, Davide ; Mokhir, Andriy ; Oellerich, Thomas ; Zirlik, Katja ; Herling, Marco ; Nguyen-Khac, Florence ; Plass, Christoph ; Andersson, Emma ; Mustjoki, Satu ; Kalle, Christof von ; Ho, Anthony Dick ; Hensel, Manfred ; Dürig, Jan ; Ringshausen, Ingo ; Zapatka, Marc ; Huber, Wolfgang ; Zenz, Thorsten
As new generations of targeted therapies emerge and tumor genome sequencing discovers increasingly comprehensive mutation repertoires, the functional relationships of mutations to tumor phenotypes remain largely unknown. Here, we measured ex vivo sensitivity of 246 blood cancers to 63 drugs alongside genome, transcriptome, and DNA methylome analysis to understand determinants of drug response. We assembled a primary blood cancer cell encyclopedia data set that revealed disease-specific sensitivities for each cancer. Within chronic lymphocytic leukemia (CLL), responses to 62% of drugs were associated with 2 or more mutations, and linked the B cell receptor (BCR) pathway to trisomy 12, an important driver of CLL. Based on drug responses, the disease could be organized into phenotypic subgroups characterized by exploitable dependencies on BCR, mTOR, or MEK signaling and associated with mutations, gene expression, and DNA methylation. Fourteen percent of CLLs were driven by mTOR signaling in a non–BCR-dependent manner. Multivariate modeling revealed immunoglobulin heavy chain variable gene (IGHV) mutation status and trisomy 12 as the most important modulators of response to kinase inhibitors in CLL. Ex vivo drug responses were associated with outcome. This study overcomes the perception that most mutations do not influence drug response of cancer, and points to an updated approach to understanding tumor biology, with implications for biomarker discovery and cancer care.
Wenzel, Mike ; Welte, Maria-Noemi ; Grossmann, Lina ; Preißer, Felix Martin ; Theißen, Lena Hermine ; Humke, Clara Julia ; Deuker, Marina ; Bernatz, Simon ; Gild, Philipp ; Ahyai, Sascha ; Karakiewicz, Pierre I. ; Bodelle, Boris ; Kluth, Luis A. ; Chun, Felix ; Mandel, Philipp ; Becker, Andreas
Objective: To investigate the value of standard [digital rectal examination (DRE), PSA] and advanced (mpMRI, prostate biopsy) clinical evaluation for prostate cancer (PCa) detection in contemporary patients with clinical bladder outlet obstruction (BOO) scheduled for Holmium laser enucleation of the prostate (HoLEP).
Material and Methods: We retrospectively analyzed 397 patients, who were referred to our tertiary care laser center for HoLEP due to BOO between 11/2017 and 07/2020. Of those, 83 (20.7%) underwent further advanced clinical PCa evaluation with mpMRI and/or prostate biopsy due to elevated PSA and/or lowered PSA ratio and/or suspicious DRE. Logistic regression and binary regression tree models were applied to identify PCa in BOO patients.
Results: An mpMRI was conducted in 56 (66%) of 83 patients and revealed PIRADS 4/5 lesions in 14 (25%) patients. Subsequently, a combined systematic randomized and MRI-fusion biopsy was performed in 19 (23%) patients and revealed in PCa detection in four patients (5%). A randomized prostate biopsy was performed in 31 (37%) patients and revealed in PCa detection in three patients (4%). All seven patients (9%) with PCa detection underwent radical prostatectomy with 29% exhibiting non-organ confined disease. Incidental PCa after HoLEP (n = 76) was found in nine patients (12%) with advanced clinical PCa evaluation preoperatively. In univariable logistic regression analyses, PSA, fPSA ratio, and PSA density failed to identify patients with PCa detection. Conversely, patients with a lower International Prostate Symptom Score (IPSS) and PIRADs 4/5 lesion in mpMRI were at higher risk for PCa detection. In multivariable adjusted analyses, PIRADS 4/5 lesions were confirmed as an independent risk factor (OR 9.91, p = 0.04), while IPSS did not reach significance (p = 0.052).
Conclusion: In advanced clinical PCa evaluation mpMRI should be considered in patients with elevated total PSA or low fPSA ratio scheduled for BOO treatment with HoLEP. Patients with low IPSS or PIRADS 4/5 lesions in mpMRI are at highest risk for PCa detection. In patients with a history of two or more sets of negative prostate biopsies, advanced clinical PCa evaluation might be omitted.
Safety requirements and the need of low‐migration UV inks have received increasing attention in the packaging industry. Crucial for the development and design of low‐migration UV inkjet inks for migration‐sensitive applications is the polymerization degree. In this study, curing‐behavior of a black, high purity packaging ink (HPP‐ink) was monitored using ATR‐FTIR spectroscopy. UV irradiation of HPP‐ink led to changes in specific absorption bands of the FTIR spectra due to crosslinking reaction of double bonds. Changes in absorptions bands at 1,408 and 1,321 cm−1 permitted the determination of CC conversion of acrylic and vinyl double bond, independently of one another. In addition, a method was developed which allows the investigation of surface‐cure and deep‐cure behavior, separately.
Riecke, Kerstin ; Müller, Volkmar ; Weide, Rudolf ; Schmidt, Marcus ; Park-Simon, Tjoung-Won ; Möbus, Volker ; Mundhenke, Christoph ; Polasik, Arkadius ; Lübbe, Kristina ; Hesse, Tobias ; Laakmann, Elena ; Thill, Marc ; Fasching, Peter Andreas ; Denkert, Carsten ; Fehm, Tanja ; Nekljudova, Valentina ; Rey, Julia ; Loibl, Sibylle ; Witzel, Isabell
Simple Summary: The incidence of brain metastases from breast cancer is increasing and the treatment is still a major challenge. Several scores have been developed in order to estimate the prognosis of patients with brain metastases by objective criteria. Here, we validated all three published graded-prognostic-assessment (GPA)-scores in a subcohort of 882 breast cancer patients with brain metastases in the Brain Metastases in the German Breast Cancer (BMBC) registry. Although all three available GPA-scores were associated with OS, they all show limitations mainly in predicting short-term (below 3 months) survival but also in long-term (above 12 months) survival. We discuss the test performances of all scores in our work and provide evidence how physicians should use them as a tool to select patients for different treatment options.
Abstract: Several scores have been developed in order to estimate the prognosis of patients with brain metastases (BM) by objective criteria. The aim of this analysis was to validate all three published graded-prognostic-assessment (GPA)-scores in a subcohort of 882 breast cancer (BC) patients with BM in the Brain Metastases in the German Breast Cancer (BMBC) registry. The median age at diagnosis of BM was 57 years. All in all, 22.3% of patients (n = 197) had triple-negative, 33.4% (n = 295) luminal A like, 25.1% (n = 221) luminal B/HER2-enriched like and 19.2% (n = 169) HER2 positive like BC. Age ≥60 years, evidence of extracranial metastases (ECM), higher number of BM, triple-negative subtype and low Karnofsky-Performance-Status (KPS) were all associated with worse overall survival (OS) in univariate analysis (p < 0.001 each). All three GPA-scores were associated with OS. The breast-GPA showed the highest probability of classifying patients with survival above 12 months in the best prognostic group (specificity 68.7% compared with 48.1% for the updated breast-GPA and 21.8% for the original GPA). Sensitivities for predicting 3 months survival were very low for all scores. In this analysis, all GPA-scores showed only moderate diagnostic accuracy in predicting the OS of BC patients with BM.
Characteristics and clinical outcome of breast cancer patients with asymptomatic brain metastases
(2020)
Laakmann, Elena ; Witzel, Isabell ; Neunhöffer, Tanja ; Weide, Rudolf ; Schmidt, Marcus ; Park-Simon, Tjoung-Won ; Möbus, Volker ; Mundhenke, Christoph ; Polasik, Arkadius ; Lübbe, Kristina ; Hesse, Tobias ; Riecke, Kerstin ; Thill, Marc ; Fasching, Peter Andreas ; Denkert, Carsten ; Fehm, Tanja ; Nekljudova, Valentina ; Rey, Julia ; Loibl, Sibylle ; Müller, Volkmar
Simple Summary: The prognosis for patients with breast cancer that has spread to the brain is poor, and survival for these women hasn’t improved over the last few decades. We do not currently test for asymptomatic brain metastases in breast cancer patients, although this does happen in some other types of cancer. In this study we wanted to find out more about breast cancer that has spread to the brain and in particular to see whether there might be any advantage to spotting brain metastases before the development of neurological symptoms. Overall, our results suggest that women could be better off if their brain metastases are diagnosed before they begin to cause symptoms. We now need to carry out a clinical trial to see what happens if we screen high-risk breast cancer patients for brain metastases. This will verify whether doing so could increase survival, symptom control or quality of life.
Abstract: Background: Brain metastases (BM) have become a major challenge in patients with metastatic breast cancer. Methods: The aim of this analysis was to characterize patients with asymptomatic BM (n = 580) in the overall cohort of 2589 patients with BM from our Brain Metastases in Breast Cancer Network Germany (BMBC) registry. Results: Compared to symptomatic patients, asymptomatic patients were slightly younger at diagnosis (median age: 55.5 vs. 57.0 years, p = 0.01), had a better performance status at diagnosis (Karnofsky index 80–100%: 68.4% vs. 57%, p < 0.001), a lower number of BM (>1 BM: 56% vs. 70%, p = 0.027), and a slightly smaller diameter of BM (median: 1.5 vs. 2.2 cm, p < 0.001). Asymptomatic patients were more likely to have extracranial metastases (86.7% vs. 81.5%, p = 0.003) but were less likely to have leptomeningeal metastasis (6.3% vs. 10.9%, p < 0.001). Asymptomatic patients underwent less intensive BM therapy but had a longer median overall survival (statistically significant for a cohort of HER2-positive patients) compared to symptomatic patients (10.4 vs. 6.9 months, p < 0.001). Conclusions: These analyses show a trend that asymptomatic patients have less severe metastatic brain disease and despite less intensive local BM therapy still have a better outcome (statistically significant for a cohort of HER2-positive patients) than patients who present with symptomatic BM, although a lead time bias of the earlier diagnosis cannot be ruled out. Our analysis is of clinical relevance in the context of potential trials examining the benefit of early detection and treatment of BM.
Koch, Elias Andreas Thomas ; Petzold, Anne ; Wessely, Anja ; Dippel, Edgar ; Gesierich, Anja Heike ; Gutzmer, Ralf ; Hassel, Jessica C. ; Haferkamp, Sebastian ; Hohberger, Bettina ; Kähler, Katharina C. ; Knorr, Harald ; Kreuzberg-Brenner, Nicole ; Leiter-Stöppke, Ulrike ; Loquai, Carmen ; Meier, Friedegund ; Meissner, Markus ; Mohr, Peter ; Pföhler, Claudia Ursula ; Rahimi, Farnaz ; Schadendorf, Dirk ; Schell, Beatrice ; Schlaak, Max Simon ; Terheyden, Patrick ; Thoms, Kai-Martin ; Schuler-Thurner, Beatrice ; Ugurel, Selma ; Ulrich, Jens ; Utikal, Jochen ; Weichenthal, Michael ; Ziller, Fabian ; Berking, Carola ; Heppt, Markus V.
Background: Since there is no standardized and effective treatment for advanced uveal melanoma (UM), the prognosis is dismal once metastases develop. Due to the availability of immune checkpoint blockade (ICB) in the real-world setting, the prognosis of metastatic UM has improved. However, it is unclear how the presence of hepatic and extrahepatic metastasis impacts the response and survival after ICB. Methods: A total of 178 patients with metastatic UM treated with ICB were included in this analysis. Patients were recruited from German skin cancer centers and the German national skin cancer registry (ADOReg). To investigate the impact of hepatic metastasis, two cohorts were compared: patients with liver metastasis only (cohort A, n = 55) versus those with both liver and extra-hepatic metastasis (cohort B, n = 123). Data were analyzed in both cohorts for response to treatment, progression-free survival (PFS), and overall survival (OS). The survival and progression probabilities were calculated with the Kaplan–Meier method. Log-rank tests, χ2 tests, and t-tests were performed to detect significant differences between both cohorts. Results: The median OS of the overall population was 16 months (95% CI 13.4–23.7) and the median PFS, 2.8 months (95% CI 2.5–3.0). The median OS was longer in cohort B than in cohort A (18.2 vs. 6.1 months; p = 0.071). The best objective response rate to dual ICB was 13.8% and to anti-PD-1 monotherapy 8.9% in the entire population. Patients with liver metastases only had a lower response to dual ICB, yet without significance (cohort A 8.7% vs. cohort B 16.7%; p = 0.45). Adverse events (AE) occurred in 41.6%. Severe AE were observed in 26.3% and evenly distributed between both cohorts. Conclusion: The survival of this large cohort of patients with advanced UM was more favorable than reported in previous benchmark studies. Patients with both hepatic and extrahepatic metastasis showed more favorable survival and higher response to dual ICB than those with hepatic metastasis only.
Bernatz, Simon ; Ackermann, Jörg ; Mandel, Philipp ; Kaltenbach, Benjamin ; Zhdanovich, Yauheniya ; Harter, Patrick Nikolaus ; Döring, Claudia ; Hammerstingl, Renate Maria ; Bodelle, Boris ; Smith, Kevin ; Bucher, Andreas ; Albrecht, Moritz Hans Ernst ; Rosbach, Nicolas ; Basten, Lajos Maximilian ; Yel, Ibrahim ; Wenzel, Mike ; Bankov, Katrin ; Koch, Ina ; Chun, Felix ; Köllermann, Jens ; Wild, Peter Johannes ; Vogl, Thomas J.
Objectives: To analyze the performance of radiological assessment categories and quantitative computational analysis of apparent diffusion coefficient (ADC) maps using variant machine learning algorithms to differentiate clinically significant versus insignificant prostate cancer (PCa). Methods: Retrospectively, 73 patients were included in the study. The patients (mean age, 66.3 ± 7.6 years) were examined with multiparametric MRI (mpMRI) prior to radical prostatectomy (n = 33) or targeted biopsy (n = 40). The index lesion was annotated in MRI ADC and the equivalent histologic slides according to the highest Gleason Grade Group (GrG). Volumes of interest (VOIs) were determined for each lesion and normal-appearing peripheral zone. VOIs were processed by radiomic analysis. For the classification of lesions according to their clinical significance (GrG ≥ 3), principal component (PC) analysis, univariate analysis (UA) with consecutive support vector machines, neural networks, and random forest analysis were performed. Results: PC analysis discriminated between benign and malignant prostate tissue. PC evaluation yielded no stratification of PCa lesions according to their clinical significance, but UA revealed differences in clinical assessment categories and radiomic features. We trained three classification models with fifteen feature subsets. We identified a subset of shape features which improved the diagnostic accuracy of the clinical assessment categories (maximum increase in diagnostic accuracy ΔAUC = + 0.05, p < 0.001) while also identifying combinations of features and models which reduced overall accuracy. Conclusions: The impact of radiomic features to differentiate PCa lesions according to their clinical significance remains controversial. It depends on feature selection and the employed machine learning algorithms. It can result in improvement or reduction of diagnostic performance.
RECENTLY, PASSIVE ETFS AND INDEX FUNDS HAVE BECOME POPULAR AMONG INDIVIDUAL INVESTORS. IN OUR STUDY, WE INVESTIGATE WHETHER INDIVIDUAL INVESTORS BENEFIT FROM USING THEM. WITH DATA FROM ONE OF THE LARGEST BROKERAGES IN GERMANY, WE FIND THAT INDIVIDUAL INVESTORS WORSEN THEIR PORTFOLIO PERFORMANCE AFTER USING THESE PRODUCTS IN COMPARISON TO NON-USERS. SINCE THESE SECURITIES MAKE MARKET TIMING EASIER, FURTHER ANALYSIS REVEALS THAT THE DECREASE IN USERS’ PORTFOLIO PERFORMANCE IS PRIMARILY DUE TO BAD MARKET TIMING.
THIS STUDY INVESTIGATES WHAT HAPPENS WHEN RETAIL CUSTOMERS ARE OFFERED FREE AND UNBIASED ADVICE. USING A LARGE FIELD EXPERIMENT IT SHOWS THAT THOSE WHO ACCEPT THE OFFER (5%) ARE MORE LIKELY TO BE MALE, OLDER, WEALTHIER, MORE EXPERIENCED AND MORE FINANCIALLY SOPHISTICATED. HOWEVER, EVEN THOUGH THE ADVICE WOULD HAVE HELPED, IT ACTUALLY LARGELY FAILED TO HELP BECAUSE THE CUSTOMERS DID NOT LISTEN TO IT. OVERALL, OUR RESULTS SUGGEST THAT THE MERE AVAILABILITY OF UNBIASED FINANCIAL ADVICE IS A NECESSARY BUT NOT SUFFICIENT CONDITION FOR BENEFITING RETAIL CUSTOMERS.
Manning, Alistair J. ; Redington, Alison L. ; Say, Daniel ; O'Doherty, Simon ; Young, Dickon ; Simmonds, Peter G. ; Vollmer, Martin K. ; Mühle, Jens ; Arduini, Jgor ; Spain, Gerard ; Wisher, Adam ; Maione, Michela ; Schuck, Tanja J. ; Stanley, Kieran ; Reimann, Stefan ; Engel, Andreas ; Krummel, Paul B. ; Fraser, Paul J. ; Harth, Christina M. ; Salameh, Peter K. ; Weiss, Ray F. ; Gluckman, Ray ; Brown, Peter N. ; Watterson, John D. ; Arnold, Tim
National greenhouse gas inventories (GHGIs) are submitted annually to the United Nations Framework Convention on Climate Change (UNFCCC). They are estimated in compliance with Intergovernmental Panel on Climate Change (IPCC) methodological guidance using activity data, emission factors and facility-level measurements. For some sources, the outputs from these calculations are very uncertain. Inverse modelling techniques that use high-quality, long-term measurements of atmospheric gases have been developed to provide independent verification of national GHGIs. This is considered good practice by the IPCC as it helps national inventory compilers to verify reported emissions and to reduce emission uncertainty. Emission estimates from the InTEM (Inversion Technique for Emission Modelling) model are presented for the UK for the hydrofluorocarbons (HFCs) reported to the UNFCCC (HFC-125, HFC-134a, HFC-143a, HFC-152a, HFC-23, HFC-32, HFC-227ea, HFC-245fa, HFC-43-10mee and HFC-365mfc). These HFCs have high global warming potentials (GWPs), and the global background mole fractions of all but two are increasing, thus highlighting their relevance to the climate and a need for increasing the accuracy of emission estimation for regulatory purposes. This study presents evidence that the long-term annual increase in growth of HFC-134a has stopped and is now decreasing. For HFC-32 there is an early indication, its rapid global growth period has ended, and there is evidence that the annual increase in global growth for HFC-125 has slowed from 2018. The inverse modelling results indicate that the UK implementation of European Union regulation of HFC emissions has been successful in initiating a decline in UK emissions from 2018. Comparison of the total InTEM UK HFC emissions in 2020 with the average from 2009–2012 shows a drop of 35 %, indicating progress toward the target of a 79 % decrease in sales by 2030. The total InTEM HFC emission estimates (2008–2018) are on average 73 (62–83) % of, or 4.3 (2.7–5.9) Tg CO2-eq yr−1 lower than, the total HFC emission estimates from the UK GHGI. There are also significant discrepancies between the two estimates for the individual HFCs.
Manning, Alistair J. ; Redington, Alison L. ; Say, Daniel ; O'Doherty, Simon ; Young, Dickon ; Simonsen, Peter G. ; Vollmer, Martin K. ; Mühle, Jens ; Arduini, Jgor ; Spain, Gerard ; Wisher, Adam ; Maione, Michela ; Schuck, Tanja J. ; Stanley, Kieran ; Reimann, Stefan ; Engel, Andreas ; Krummel, Paul B. ; Fraser, Paul J. ; Harth, Christina M. ; Salameh, Peter K. ; Weiss, Ray F. ; Gluckman, Ray ; Brown, Peter N. ; Watterson, John D. ; Arnold, Tim
National Greenhouse Gas Inventories (GHGI) are submitted annually to the United Nations Framework Convention on Climate Change (UNFCCC). They are estimated in compliance with Intergovernmental Panel on Climate Change (IPCC) methodological guidance using activity data, emission factors and facility-level measurements. For some sources, the outputs from these calculations are very uncertain. Inverse modelling techniques that use high-quality, long-term measurements of atmospheric gases have been developed to provide independent verification of national GHGI. This is considered good practice by the IPCC as it helps national inventory compilers to verify reported emissions and to reduce emission uncertainty. Emission estimates from the InTEM (Inversion Technique for Emissions Modelling) model are presented for the UK for the hydrofluorocarbons (HFCs) reported to the UNFCCC (HFC-125, HFC-134a, HFC-143a, HFC-152a, HFC-23, HFC-32, HFC-227ea, HFC-245fa, HFC-43-10mee and HFC-365mfc). These HFCs have high Global Warming Potentials (GWPs) and the global background mole fractions of all but two are increasing, thus highlighting their relevance to the climate and a need for increasing the accuracy of emission estimation for regulatory purposes. This study presents evidence that the long-term annual increase in growth of HFC-134a has stopped and is now decreasing. For HFC-32 there is an early indication its rapid global growth period has ended, and there is evidence that the annual increase in global growth for HFC-125 has slowed from 2018. The inverse modelling results indicate that the UK implementation of European Union regulation of HFC emissions has been successful in initiating a decline in UK emissions in the since 2018. Comparison of the total InTEM UK HFC emissions in 2020 with the average from 2009–2012 shows a drop of 35%, indicating progress toward the target of a 79% decrease in sales by 2030. The total InTEM HFC emission estimates (2008–2018) are on average 73 (62–83)% of, or 4.3 (2.7–5.9) Tg CO2-eq yr−1 lower than, the total HFC emission estimates from the UK GHGI inventory. There are also significant discrepancies between the two estimates for the individual HFCs.
Wang, Mingyi ; Xiao, Mao ; Bertozzi, Barbara ; Marie, Guillaume ; Rörup, Birte ; Schulze, Benjamin ; Bardakov, Roman ; He, Xu-Cheng ; Shen, Jiali ; Scholz, Wiebke ; Marten, Ruby ; Dada, Lubna ; Baalbaki, Rima ; Lopez, Brandon ; Lamkaddam, Houssni ; Manninen, Hanna E. ; Amorim, Antonio ; Ataei, Farnoush ; Bogert, Pia ; Brasseur, Zoé ; Caudillo, Lucía ; De Menezes, Louis-Philippe ; Duplissy, Jonathan ; Ekman, Annica M. L. ; Finkenzeller, Henning ; Gonzalez Carracedo, Loïc ; Granzin, Manuel ; Guida, Roberto ; Heinritzi, Martin ; Hofbauer, Victoria ; Höhler, Kristina ; Korhonen, Kimmo ; Krechmer, Jordan E. ; Kürten, Christoph Andreas ; Lehtipalo, Katrianne ; Mahfouz, Naser G. A. ; Makhmutov, Vladimir ; Massabò, Dario ; Mathot, Serge ; Mauldin, Roy L. ; Mentler, Bernhard ; Müller, Tatjana ; Onnela, Antti ; Petäjä, Tuukka ; Philippov, Maxim ; Piedehierro, Ana A. ; Pozzer, Andrea ; Ranjithkumar, Ananth ; Schervish, Meredith ; Schobesberger, Siegfried ; Simon, Mario ; Stozhkov, Yuri ; Tomé, António ; Umo, Nsikanabasi Silas ; Vogel, Franziska ; Wagner, Robert ; Wang, Dongyu S. ; Weber, Stefan K. ; Welti, André ; Wu, Yusheng ; Zauner-Wieczorek, Marcel ; Sipilä, Mikko ; Winkler, Paul M. ; Hansel, Armin ; Baltensperger, Urs ; Kulmala, Markku ; Flagan, Richard C. ; Curtius, Joachim ; Riipinen, Ilona ; Gordon, Hamish ; Lelieveld, Jos ; El Haddad, Imad ; Volkamer, Rainer ; Worsnop, Douglas R. ; Christoudias, Theodoros ; Kirkby, Jasper ; Möhler, Ottmar ; Donahue, Neil McPherson
New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)1,2,3,4. However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region5,6. Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles—comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3–H2SO4–NH3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
Wang, Mingyi ; Kong, Weimeng ; Marten, Ruby ; He, Xu-Cheng ; Chen, Dexian ; Pfeifer, Joschka ; Heitto, Arto ; Kontkanen, Jenni ; Dada, Lubna ; Kürten, Christoph Andreas ; Yli-Juuti, Taina ; Manninen, Hanna Elina ; Amanatidis, Stavros ; Amorim, Antonio ; Baalbaki, Rima ; Baccarini, Andrea ; Bell, David M. ; Bertozzi, Barbara ; Bräkling, Steffen ; Brilke, Sophia ; Murillo, Lucía Caudillo ; Chiu, Randall ; Chu, Biwu ; De Menezes, Louis-Philippe ; Duplissy, Jonathan ; Finkenzeller, Henning ; Gonzalez Carracedo, Loic ; Granzin, Manuel ; Guida, Roberto ; Hansel, Armin ; Hofbauer, Victoria ; Krechmer, Jordan ; Lehtipalo, Katrianne ; Lamkaddam, Houssni ; Lampimäki, Marku ; Lee, Chuan Ping ; Makhmutov, Vladimir ; Marie, Guillaume ; Mathot, Serge ; Mauldin, Roy Lee ; Mentler, Bernhard ; Müller, Tatjana ; Onnela, Antti ; Partoll, Eva ; Petäjä, Tuukka ; Philippov, Maxim ; Pospisilova, Veronika ; Ranjithkumar, Ananth ; Rissanen, Matti P. ; Rörup, Birte ; Scholz, Wiebke ; Shen, Jiali ; Simon, Mario ; Sipilä, Mikko ; Steiner, Gerhard ; Stolzenburg, Dominik ; Tham, Yee Jun ; Tomé, António ; Wagner, Andrea Christine ; Wang, Dongyu S. ; Wang, Yonghong ; Weber, Stefan K. ; Winkler, Paul M. ; Wlasits, Peter J. ; Wu, Yusheng ; Xiao, Mao ; Ye, Qing ; Zauner-Wieczorek, Marcel ; Zhou, Xueqin ; Volkamer, Rainer ; Riipinen, Ilona ; Dommen, Josef ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Worsnop, Douglas R. ; Kirkby, Jasper ; Seinfeld, John H. ; El Haddad, Imad ; Flagan, Richard C. ; Donahue, Neil McPherson
A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog, but how it occurs in cities is often puzzling. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms.
Kürten, Christoph Andreas ; Bergen, Anton ; Heinritzi, Martin ; Leiminger, Markus ; Lorenz, Verena ; Piel, Felix ; Simon, Mario ; Sitals, Robert ; Wagner, Andrea Christine ; Curtius, Joachim
The exact mechanisms for new particle formation (NPF) under different boundary layer conditions are not known yet. One important question is whether amines and sulfuric acid lead to efficient NPF in the atmosphere. Furthermore, it is not clear to what extent highly oxidized organic molecules (HOMs) are involved in NPF. We conducted field measurements at a rural site in central Germany in the proximity of three larger dairy farms to investigate whether there is a connection between NPF and the presence of amines and/or ammonia due to the local emissions from the farms. Comprehensive measurements using a nitrate chemical ionization–atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer, a proton-transfer-reaction mass spectrometer (PTR-MS), particle counters and differential mobility analyzers (DMAs), as well as measurements of trace gases and meteorological parameters, were performed. We demonstrate here that the nitrate CI-APi-TOF is suitable for sensitive measurements of sulfuric acid, amines, a nitrosamine, ammonia, iodic acid and HOMs. NPF was found to correlate with sulfuric acid, while an anti-correlation with RH, amines and ammonia is observed. The anti-correlation between NPF and amines could be due to the efficient uptake of these compounds by nucleating clusters and small particles. Much higher HOM dimer (C19/C20 compounds) concentrations during the night than during the day indicate that these HOMs do not efficiently self-nucleate as no nighttime NPF is observed. Observed iodic acid probably originates from an iodine-containing reservoir substance, but the iodine signals are very likely too low to have a significant effect on NPF.
Kürten, Christoph Andreas ; Bergen, Anton ; Heinritzi, Martin ; Leiminger, Markus ; Lorenz, Verena ; Piel, Felix ; Simon, Mario ; Sitals, Robert ; Wagner, Andrea Christine ; Curtius, Joachim
The exact mechanisms for new particle formation (NPF) under different boundary layer conditions are not known yet. One important question is if amines and sulfuric acid lead to efficient NPF in the atmosphere. Furthermore, it is not clear to what extent highly oxidized organic molecules (HOM) are involved in NPF. We conducted field measurements at a rural site in central Germany in the proximity of three larger dairy farms to investigate if there is a connection between NPF and the presence of amines and/or ammonia due to the local emissions from the farms. Comprehensive measurements using a nitrate Chemical Ionization-Atmospheric Pressure interface-Time Of Flight (CI-APi-TOF) mass spectrometer, a Proton Transfer Reaction-Mass Spectrometer (PTR-MS), particle counters and Differential Mobility Analyzers (DMAs) as well as measurements of trace gases and meteorological parameters were performed. It is shown that the nitrate CI-APi-TOF is suitable for sensitive measurements of sulfuric acid, amines, a nitrosamine, ammonia, iodic acid and HOM. NPF was found to correlate with sulfuric acid, while an anti-correlation with RH, amines and ammonia is observed. The anti-correlation between NPF and amines could be due to the efficient uptake of these compounds by nucleating clusters and small particles. Much higher HOM dimer (C19/C20 compounds) concentrations during the night than during the day indicate that these HOM do not efficiently self-nucleate as no night-time NPF is observed. Observed iodic acid probably originates from an iodine-containing reservoir substance but the iodine signals are very likely too low to have a significant effect on NPF.
Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.
Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid-base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10-30 nm VMD particles. This behavior is not consistent with present nanoparticle physico-chemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base:acid ratios lower than 1:1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient that suggests a change to a mixed-phase state as the particles grew beyond this size. The reasons for the very acidic composition remain uncertain, but a possible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid-base pairs in particles as small as 10 nm.
Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
(2015)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter Κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In 20 particular, when the concentrations of sulfuric acid was 5.1 x 106 molecules cm exp -3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured Κ of 15nm particles was 0.3 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (Κ DMAS ~ 0.28). Furthermore, the difference in Κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The Κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth already at 10nm sizes.
Hygroscopicity of nanoparticles produced from homogeneous
nucleation in the CLOUD experiments
(2016)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid–dimethylamine, and sulfuric acid–organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (κDMAS ∼ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid–imethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
Heinritzi, Martin ; Simon, Mario ; Steiner, Gerhard ; Wagner, Andrea Christine ; Kürten, Christoph Andreas ; Hansel, Armin ; Curtius, Joachim
Knowledge about mass discrimination effects in a chemical ionization mass spectrometer (CIMS) is crucial for quantifying, e.g., the recently discovered extremely low volatile organic compounds (ELVOCs) and other compounds for which no calibration standard exists so far. Here, we present a simple way of estimating mass discrimination effects of a nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer. Characterization of the mass discrimination is achieved by adding different perfluorinated acids to the mass spectrometer in amounts sufficient to deplete the primary ions significantly. The relative transmission efficiency can then be determined by comparing the decrease of signals from the primary ions and the increase of signals from the perfluorinated acids at higher masses. This method is in use already for PTR-MS; however, its application to a CI-APi-TOF brings additional difficulties, namely clustering and fragmentation of the measured compounds, which can be treated with statistical analysis of the measured data, leading to self-consistent results. We also compare this method to a transmission estimation obtained with a setup using an electrospray ion source, a high-resolution differential mobility analyzer and an electrometer, which estimates the transmission of the instrument without the CI source. Both methods give different transmission curves, indicating non-negligible mass discrimination effects of the CI source. The absolute transmission of the instrument without the CI source was estimated with the HR-DMA method to plateau between the m∕z range of 127 and 568 Th at around 1.5 %; however, for the CI source included, the depletion method showed a steady increase in relative transmission efficiency from the m∕z range of the primary ion (mainly at 62 Th) to around 550 Th by a factor of around 5. The main advantages of the depletion method are that the instrument is used in the same operation mode as during standard measurements and no knowledge of the absolute amount of the measured substance is necessary, which results in a simple setup.
Heinritzi, Martin ; Simon, Mario ; Steiner, Gerhard ; Wagner, Andrea Christine ; Kürten, Christoph Andreas ; Hansel, Armin ; Curtius, Joachim
Knowledge about mass discrimination effects in a chemical ionization mass spectrometer (CIMS) is crucial for quantifying, e.g., the recently discovered extremely low volatile organic compounds (ELVOCs) and other compounds for which no calibration standard exists so far. Here, we present a simple way of estimating mass discrimination effects of a nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer. Characterization of the mass discrimination is achieved by adding different perfluorinated acids to the mass spectrometer in amounts sufficient to deplete the primary ions significantly. The relative transmission efficiency can then be determined by comparing the decrease of signals from the primary ions and the increase of signals from the perfluorinated acids at higher masses. This method is in use already for PTR-MS; however, its application to a CI-APi-TOF brings additional difficulties, namely clustering and fragmentation of the measured compounds, which can be treated with statistical analysis of the measured data, leading to selfconsistent results. We also compare this method to a transmission estimation obtained with a setup using an electrospray ion source, a high-resolution differential mobility analyzer and an electrometer, which estimates the transmission of the instrument without the CI source. Both methods give different transmission curves, indicating non-negligible mass discrimination effects of the CI source. The absolute transmission of the instrument without the CI source was estimated with the HR-DMA method to plateau between the m=z range of 127 and 568 Th at around 1.5 %; however, for the CI source included, the depletion method showed a steady increase in relative transmission efficiency from the m=z range of the primary ion (mainly at 62 Th) to around 550 Th by a factor of around 5. The main advantages of the depletion method are that the instrument is used in the same operation mode as during standard measurements and no knowledge of the absolute amount of the measured substance is necessary, which results in a simple setup.
Keskinen, Helmi ; Virtanen, Annele ; Joutsensaari, Jorma ; Tsagkogeorgas, Georgios ; Duplissy, Jonathan ; Schobesberger, Siegfried ; Gysel, Martin ; Riccobono, Francesco ; Slowik, Jay G. ; Bianchi, Federico ; Yli-Juuti, Taina ; Lehtipalo, Katrianne ; Rondo, Linda ; Breitenlechner, Martin ; Kupc, Agnieszka ; Almeida, Joao ; Amorin, António ; Dunne, Eimear M. ; Downward, Andrew J. ; Ehrhart, Sebastian ; Franchin, Alessandro ; Kajos, Maija K. ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Nieminen, Tuomo ; Makhmutov, Vladimir ; Mathot, Serge ; Miettinen, Pasi ; Onnela, Antti ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Santos, Filipe Duarte ; Schallhart, Simon ; Sipilä, Mikko ; Stozhkov, Yuri ; Tomé, Antonio ; Vaattovaara, Petri ; Wimmer, Daniela ; Prévôt, André Stephan Henry ; Dommen, Josef ; Donahue, Neil McPherson ; Flagan, Richard C. ; Weingartner, Ernest ; Viisanen, Yrjö ; Riipinen, Ilona ; Hansel, Armin ; Curtius, Joachim ; Kulmala, Markku ; Worsnop, Douglas R. ; Baltensperger, Urs ; Wex, Heike ; Stratmann, Frank ; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD chamber experiments at CERN. The investigation is carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovski-Stokes-Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ∼0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Keskinen, Helmi ; Virtanen, Annele ; Joutsensaari, Jorma ; Tsagkogeorgas, Georgios ; Duplissy, Jonathan ; Schobesberger, Siegfried ; Gysel, Martin ; Riccobono, Francesco ; Slowik, Jay G. ; Bianchi, Federico ; Yli-Juuti, Taina ; Lehtipalo, Katrianne ; Rondo, Linda ; Breitenlechner, Martin ; Kupc, Agnieszka ; Almeida, Joao ; Amorin, António ; Dunne, Eimear M. ; Downward, Andrew J. ; Ehrhart, Sebastian ; Franchin, Alessandro ; Kajos, Maija K. ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Nieminen, Tuomo ; Makhmutov, Vladimir ; Mathot, Serge ; Miettinen, Pasi ; Onnela, Antti ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Santos, Filipe Duarte ; Schallhart, Simon ; Sipilä, Mikko ; Stozhkov, Yuri ; Tomé, Antonio ; Vaattovaara, Petri ; Wimmer, Daniela ; Prévôt, André Stephan Henry ; Dommen, Josef ; Donahue, Neil McPherson ; Flagan, Richard C. ; Weingartner, Ernest ; Viisanen, Yrjö ; Riipinen, Ilona ; Hansel, Armin ; Curtius, Joachim ; Kulmala, Markku ; Worsnop, Douglas R. ; Baltensperger, Urs ; Wex, Heike ; Stratmann, Frank ; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Kürten, Christoph Andreas ; Li, Chenxi ; Bianchi, Federico ; Curtius, Joachim ; Dias, Antonio ; Donahue, Neil McPherson ; Duplissy, Jonathan ; Flagan, Richard C. ; Hakala, Jani ; Jokinen, Tuija ; Kirkby, Jasper ; Kulmala, Markku ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Makhmutov, Vladimir ; Onnela, Antti ; Rissanen, Matti P. ; Simon, Mario ; Sipilä, Mikko ; Stozhkov, Yuri ; Tröstl, Jasmin ; Ye, Penglin ; McMurry, Peter H.
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (∼ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm−3, and dimethylamine mixing ratio of ∼ 40 pptv, i.e., 1 × 109 cm−3).
Kürten, Christoph Andreas ; Li, Chenxi ; Bianchi, Federico ; Curtius, Joachim ; Dias, Antonio ; Donahue, Neil McPherson ; Duplissy, Jonathan ; Flagan, Richard C. ; Hakala, Jani ; Jokinen, Tuija ; Kirkby, Jasper ; Kulmala, Markku ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Makhmutov, Vladimir ; Onnela, Antti ; Rissanen, Matti P. ; Simon, Mario ; Sipilä, Mikko ; Stozhkov, Yuri ; Tröstl, Jasmin ; Ye, Penglin ; McMurry, Peter H.
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently, and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are re-analyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 nm and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically-controlled) new particle formation for the conditions during the CLOUD7 experiment (278 K, 38% RH, sulfuric acid concentration between 1×106 and 3×107 cm-3 and dimethylamine mixing ratio of ~40 pptv). Finally, the simulation of atmospheric new particle formation reveals that even tiny mixing ratios of dimethylamine (0.1 pptv) yield NPF rates that could explain significant boundary layer particle formation. This highlights the need for improved speciation and quantification techniques for atmospheric gas-phase amine measurements.
Simon, Mario ; Heinritzi, Martin ; Herzog, Stephan ; Leiminger, Markus ; Bianchi, Federico ; Praplan, Arnaud Patrick ; Dommen, Josef ; Curtius, Joachim ; Kürten, Christoph Andreas
Amines are potentially important for atmospheric new particle formation, but their concentrations are usually low with typical mixing ratios in the pptv range or even smaller. Therefore, the demand for highly sensitive gas-phase amine measurements has emerged in the last several years. Nitrate chemical ionization mass spectrometry (CIMS) is routinely used for the measurement of gas-phase sulfuric acid in the sub-pptv range. Furthermore, extremely low volatile organic compounds (ELVOCs) can be detected with a nitrate CIMS. In this study we demonstrate that a nitrate CIMS can also be used for the sensitive measurement of dimethylamine (DMA, (CH3)2NH) using the NO3−•(HNO3)1 − 2• (DMA) cluster ion signal. Calibration measurements were made at the CLOUD chamber during two different measurement campaigns. Good linearity between 0 and ∼ 120 pptv of DMA as well as a sub-pptv detection limit of 0.7 pptv for a 10 min integration time are demonstrated at 278 K and 38 % RH.
Hall, Brad D. ; Engel, Andreas ; Mühle, Jens ; Elkins, James William ; Artuso, Florinda ; Atlas, Elliot L. ; Aydin, Murat ; Blake, Donald R. ; Brunke, Ernst-Günther ; Chiavarini, Salvatore ; Fraser, Paul J. ; Happell, James D. ; Krummel, Paul B. ; Levin, Ingeborg ; Loewenstein, Max ; Maione, Michela ; Montzka, Stephen A. ; O'Doherty, Simon ; Reimann, Stefan ; Rhoderick, George J. ; Saltzman, Eric S. ; Scheel, Hans-Eckhart ; Steele, L. Paul ; Vollmer, Martin K. ; Weiss, Ray F. ; Worthy, Douglas E. ; Yokouchi, Yoko
The International Halocarbons in Air Comparison Experiment (IHALACE) was conducted to document relationships between calibration scales among various laboratories that measure atmospheric greenhouse and ozone depleting gases. Six stainless steel cylinders containing natural and modified natural air samples were circulated among 19 laboratories. Results from this experiment reveal relatively good agreement among commonly used calibration scales for a number of trace gases present in the unpolluted atmosphere at pmol mol−1 (parts per trillion) levels, such as chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). Some scale relationships were found to be consistent with those derived from bi-lateral experiments or from analysis of atmospheric data, while others revealed discrepancies. The transfer of calibration scales among laboratories was found to be problematic in many cases, meaning that measurements tied to a common scale may not, in fact, be compatible. These results reveal substantial improvements in calibration over previous comparisons. However there is room for improvement in communication and coordination of calibration activities with respect to the measurement of halogenated and related trace gases.
Yver, Camille E. ; Pison, Isabelle C. ; Fortems-Cheiney, Audrey ; Schmidt, Martina ; Chevallier, Frédéric ; Ramonet, Michel ; Jordan, Armin ; Søvde, Ole Amund ; Engel, Andreas ; Fisher, Rebecca E. ; Lowry, David ; Nisbet, Euan G. ; Levin, Ingeborg ; Hammer, Samuel ; Necki, Jaroslaw ; Bartyzel, Jakub ; Reimann, Stefan ; Vollmer, Martin ; Steinbacher, Martin ; Aalto, Tuula ; Maione, Michela ; Arduini, Jgor ; O'Doherty, Simon ; Grant, Aoife ; Sturges, William T. ; Forster, Grant L. ; Lunder, Chris Rene ; Privalov, Viacheslav I. ; Paramonova, Nina N.
This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, soil uptake distinct from surface emissions and finally, soil uptake, biomass burning, anthropogenic emissions and N2 fixation-related emissions separately were inverted in several scenarios. The various inversions generate an estimate for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and 8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on soil uptake measurements. Our estimate of global H2 soil uptake is −59 ± 4.0 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions considering their respective uncertainties. To constrain a more robust partition of H2 sources and sinks would need additional constraints, such as isotopic measurements.
Pison, Isabelle C. ; Fortems-Cheiney, Audrey ; Schmidt, Martina ; Chevallier, Frédéric ; Ramonet, Michel ; Jordan, Armin ; Søvde, Ole Amund ; Engel, Andreas ; Fisher, Rebecca E. ; Lowry, David ; Nisbet, Euan G. ; Levin, Ingeborg ; Hammer, Samuel ; Necki, Jaroslaw ; Bartyzel, J. ; Reimann, Stefan ; Vollmer, Martin K. ; Steinbacher, Martin ; Aalto, Tuula ; Maione, Michela ; Arduini, Jgor ; O'Doherty, Simon ; Grant, Aoife ; Sturges, William T. ; Forster, Grant L. ; Lunder, Chris Rene ; Privalov, Viacheslav I. ; Paramonova, Nina N. ; Werner, A. ; Bousquet, Philippe
This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between −8 and +8 Tg yr−1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is −59±9 Tg yr−1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks.
Caudillo-Plath, Lucía ; Rörup, Birte ; Heinritzi, Martin ; Marie, Guillaume ; Simon, Mario ; Wagner, Andrea C. ; Müller, Tatjana ; Granzin, Manuel ; Amorim, António ; Ataei, Farnoush ; Baalbaki, Rima ; Bertozzi, Barbara ; Brasseur, Zoé ; Chiu, Randall ; Chu, Biwu ; Dada, Lubna ; Duplissy, Jonathan ; Finkenzeller, Henning ; Gonzalez Carracedo, Loïc ; He, Xu-Cheng ; Hofbauer, Victoria ; Kong, Weimeng ; Lamkaddam, Houssni ; Lee, Chuan P. ; Lopez, Brandon ; Mahfouz, Naser G. A. ; Makhmutov, Vladimir ; Manninen, Hanna E. ; Marten, Ruby ; Massabò, Dario ; Mauldin, Roy L. ; Mentler, Bernhard ; Molteni, Ugo ; Onnela, Antti ; Pfeifer, Joschka ; Philippov, Maxim ; Piedehierro, Ana A. ; Schervish, Meredith ; Scholz, Wiebke ; Schulze, Benjamin ; Shen, Jiali ; Stolzenburg, Dominik ; Stožkov, Ju. I. ; Surdu, Mihnea ; Tauber, Christian ; Tham, Yee Jun ; Tian, Ping ; Tomé, António ; Vogt, Steffen ; Wang, Mingyi ; Wang, Dongyu S. ; Weber, Stefan K. ; Welti, André ; Yonghong, Wang ; Yusheng, Wu ; Zauner-Wieczorek, Marcel ; Baltensperger, Urs ; El Haddad, Imad ; Flagan, Richard C. ; Hansel, Armin ; Höhler, Kristina ; Kirkby, Jasper ; Kulmala, Markku ; Lehtipalo, Katrianne ; Möhler, Ottmar ; Saathoff, Harald ; Volkamer, Rainer ; Winkler, Paul M. ; Donahue, Neil M. ; Kürten, Christoph Andreas ; Curtius, Joachim
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
Caudillo-Plath, Lucı́a ; Rörup, Birte ; Heinritzi, Martin ; Marie, Guillaume ; Simon, Mario ; Wagner, Andrea C. ; Müller, Tatjana ; Granzin, Manuel ; Amorim, Antonio ; Ataei, Farnoush ; Baalbaki, Rima ; Bertozzi, Barbara ; Brasseur, Zoé ; Chiu, Randall ; Chu, Biwu ; Dada, Lubna ; Duplissy, Jonathan ; Finkenzeller, Henning ; Gonzalez Carracedo, Loïc ; He, Xu-Cheng ; Hofbauer, Victoria ; Kong, Weimeng ; Lamkaddam, Houssni ; Lee, Chuan P ; Lopez, Brandon ; Mahfouz, Naser G. A. ; Makhmutov, Vladimir ; Manninen, Hanna E. ; Marten, Ruby ; Massabò, Dario ; Mauldin, Roy L. ; Mentler, Bernhard ; Molteni, Ugo ; Onnela, Antti ; Pfeifer, Joschka ; Philippov, Maxim ; Piedehierro, Ana A. ; Schervish, Meredith ; Scholz, Wiebke ; Schulze, Benjamin ; Shen, Jiali ; Stolzenburg, Dominik ; Stožkov, Ju. I. ; Surdu, Mihnea ; Tauber, Christian ; Tham, Yee Jun ; Tian, Ping ; Tomé, António ; Vogt, Steffen ; Wang, Mingyi ; Wang, Dongyu S. ; Weber, Stefan K. ; Welti, André ; Yonghong, Wang ; Yusheng, Wu ; Zauner-Wieczorek, Marcel ; Baltensperger, Urs ; El Haddad, Imad ; Flagan, Richard C. ; Hansel, Armin ; Höhler, Kristina ; Kirkby, Jasper ; Kulmala, Markku ; Lehtipalo, Katrianne ; Möhler, Ottmar ; Saathoff, Harald ; Volkamer, Rainer ; Winkler, Paul M. ; Donahue, Neil M. ; Kürten, Christoph Andreas ; Curtius, Joachim
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
Pinter, Andreas ; Schwarz, Peter ; Gerdes, Sascha ; Simon, Jan C. ; Saalbach, Anja ; Rush, James ; Melzer, Nima ; Kramps, Thomas ; Häberle, Benjamin ; Reinhardt, Maximilian
Inflammatory diseases including psoriasis are associated with metabolic and cardiovascular comorbidities, including obesity and metabolic syndrome. Obesity is associated with greater psoriasis disease severity and reduced response to treatment. Therefore, targeting metabolic comorbidities could improve patients’ health status and psoriasis-specific outcomes. METABOLyx is a randomized controlled trial evaluating the combination of a lifestyle intervention program with secukinumab treatment in psoriasis. Here, the rationale, methodology and baseline patient characteristics of METABOLyx are presented. A total of 768 patients with concomitant moderate to severe plaque psoriasis and metabolic syndrome were randomized to secukinumab 300 mg, or secukinumab 300 mg plus a tailored lifestyle intervention program, over 24 weeks. A substudy of immunologic and metabolic biomarkers is ongoing. The primary endpoint of METABOLyx is PASI90 response at week 24. Other endpoints include patient-reported outcomes and safety. METABOLyx represents the first large scale clinical trial of an immunomodulatory biologic in combination with a standardized lifestyle intervention.
Kirkby, Jasper ; Duplissy, Jonathan ; Sengupta, Kamalika ; Frege, Carla ; Gordon, Hamish ; Williamson, Christina ; Heinritzi, Martin ; Simon, Mario ; Yan, Chao ; Almeida, Joao ; Tröstl, Jasmin ; Nieminen, Tuomo ; Ortega, Ismael K. ; Wagner, Robert ; Adamov, Alexey ; Amorim, Antonio ; Bernhammer, Anne-Kathrin ; Bianchi, Federico ; Breitenlechner, Martin ; Brilke, Sophia ; Chen, Xuemeng ; Craven, Jill ; Dias, Antonio ; Ehrhart, Sebastian ; Flagan, Richard C. ; Franchin, Alessandro ; Fuchs, Claudia ; Guida, Roberto ; Hakala, Jani ; Hoyle, Christopher Robert ; Jokinen, Tuija ; Junninen, Heikki ; Kangasluoma, Juha ; Kim, Jaeseok ; Krapf, Manuel ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Makhmutov, Vladimir ; Mathot, Serge ; Molteni, Ugo ; Onnela, Antti ; Peräkylä, Otso ; Piel, Felix ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Pringle, Kirsty ; Rap, Alexandru ; Richards, Nigel A. D. ; Riipinen, Ilona ; Rissanen, Matti P. ; Rondo, Linda ; Sarnela, Nina ; Schobesberger, Siegfried ; Scott, Catherine E. ; Seinfeld, John H. ; Sipilä, Mikko ; Steiner, Gerhard ; Stozhkov, Yuri ; Stratmann, Frank ; Tomé, Antonio ; Virtanen, Annele ; Vogel, Alexander L. ; Wagner, Andrea Christine ; Wagner, Paul E. ; Weingartner, Ernest ; Wimmer, Daniela ; Winkler, Paul M. ; Ye, Penglin ; Zhang, Xuan ; Hansel, Armin ; Dommen, Josef ; Donahue, Neil McPherson ; Worsnop, Douglas R. ; Baltensperger, Urs ; Kulmala, Markku ; Carslaw, Kenneth S. ; Curtius, Joachim
Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood1. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours2. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere3,4, and that ions have a relatively minor role5. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded6,7. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
Tröstl, Jasmin ; Chuang, Wayne K. ; Gordon, Hamish ; Heinritzi, Martin ; Yan, Chao ; Molteni, Ugo ; Ahlm, Lars ; Frege, Carla ; Bianchi, Federico ; Wagner, Robert ; Simon, Mario ; Lehtipalo, Katrianne ; Williamson, Christina ; Craven, Jill ; Duplissy, Jonathan ; Adamov, Alexey ; Almeida, Joao ; Bernhammer, Anne-Kathrin ; Breitenlechner, Martin ; Brilke, Sophia ; Dias, Antonio ; Ehrhart, Sebastian ; Flagan, Richard C. ; Franchin, Alessandro ; Fuchs, Claudia ; Guida, Roberto ; Gysel, Martin ; Hansel, Armin ; Hoyle, Christopher Robert ; Jokinen, Tuija ; Junninen, Heikki ; Kangasluoma, Juha ; Keskinen, Helmi ; Kim, Jaeseok ; Krapf, Manuel ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lawler, Michael Joseph ; Leiminger, Markus ; Mathot, Serge ; Möhler, Ottmar ; Nieminen, Tuomo ; Onnela, Antti ; Petäjä, Tuukka ; Piel, Felix ; Miettinen, Pasi ; Rissanen, Matti P. ; Rondo, Linda ; Sarnela, Nina ; Schobesberger, Siegfried ; Sengupta, Kamalika ; Sipilä, Mikko ; Smith, James N. ; Steiner, Gerhard ; Tomé, Antonio ; Virtanen, Annele ; Wagner, Andrea Christine ; Weingartner, Ernest ; Wimmer, Daniela ; Winkler, Paul M. ; Ye, Penglin ; Carslaw, Kenneth S. ; Curtius, Joachim ; Dommen, Josef ; Kirkby, Jasper ; Kulmala, Markku ; Riipinen, Ilona ; Worsnop, Douglas R. ; Donahue, Neil McPherson ; Baltensperger, Urs
About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday1. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres2,3. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles4, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth5,6, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer7,8,9,10. Although recent studies11,12,13 predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon2, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory)2,14, has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown15 that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10−4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10−4.5 to 10−0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.
Wagner, Andrea Christine ; Bergen, Anton ; Brilke, Sophia ; Fuchs, Claudia ; Ernst, Markus ; Hoker, Jesica ; Heinritzi, Martin ; Simon, Mario ; Bühner, Bertram ; Curtius, Joachim ; Kürten, Christoph Andreas
A new method for size-resolved chemical analysis of nucleation mode aerosol particles (size range from ∼10 to ∼30 nm) is presented. The Thermal Desorption Differential Mobility Analyzer (TD-DMA) uses an online, discontinuous principle. The particles are charged, a specific size is selected by differential mobility analysis and they are collected on a filament by electrostatic precipitation. Subsequently, the sampled mass is evaporated in a clean carrier gas and analyzed by a chemical ionization mass spectrometer. Gas-phase measurements are performed with the same mass spectrometer during the sampling of particles. The characterization shows reproducible results, with a particle size resolution of 1.19 and the transmission efficiency for 15 nm particles being slightly above 50 %. The signal from the evaporation of a test substance can be detected starting from 0.01 ng and shows a linear response in the mass spectrometer. Instrument operation in the range of pg m−3 is demonstrated by an example measurement of 15 nm particles produced by nucleation from dimethylamine, sulfuric acid and water.
Wagner, Andrea Christine ; Bergen, Anton ; Brilke, Sophia ; Fuchs, Claudia ; Ernst, Markus ; Hoker, Jesica ; Heinritzi, Martin ; Simon, Mario ; Bühner, Bertram ; Curtius, Joachim ; Kürten, Christoph Andreas
A new method for size resolved chemical analysis of nucleation mode aerosol particles (size range from ~10 to ~30 nm) is presented. The Thermal Desorption Differential Mobility Analyzer (TD-DMA) uses an online, discontinuous principle. The particles are charged, a specific size is selected by differential mobility analysis and they are collected on a filament by electrostatic precipitation. Subsequently, the sampled mass is evaporated in a clean carrier gas and analyzed by a chemical ionization mass spectrometer. Gas phase measurements are performed with the same mass spectrometer during the sampling of particles. The characterization shows reproducible results, with a particle size resolution of 1.19 and the transmission efficiency for 15 nm particles being slightly above 50 %. The signal from the evaporation of a test substance can be detected starting from 0.01 ng and shows a linear response in the mass spectrometer. Instrument operation in the range of pg/m3 is demonstrated by an example measurement of 15 nm particles produced by nucleation from dimethylamine, sulfuric acid and water.
Simon, Mario ; Heinritzi, Martin ; Herzog, Stephan ; Leiminger, Markus ; Bianchi, Federico ; Praplan, Arnaud Patrick ; Dommen, Josef ; Curtius, Joachim ; Kürten, Christoph Andreas
Amines are potentially important for atmospheric new particle formation, but their concentrations are usually low with typical mixing ratios in the pptv range or even smaller. Therefore, the demand for highly sensitive gas-phase amine measurements has emerged in the last several years. Nitrate chemical ionization mass spectrometry (CIMS) is routinely used for the measurement of gasphase sulfuric acid in the sub-pptv range. Furthermore, extremely low volatile organic compounds (ELVOCs) can be detected with a nitrate CIMS. In this study we demonstrate that a nitrate CIMS can also be used for the sensitive measurement of dimethylamine (DMA, (CH3/2NH) using the NO3−•(HNO3)1 − 2• (DMA) cluster ion signal. Calibration measurements were made at the CLOUD chamber during two different measurement campaigns. Good linearity between 0 and ~120 pptv of DMA as well as a sub-pptv detection limit of 0.7 pptv for a 10 min integration time are demonstrated at 278K and 38% RH.
We present a compact and versatile cryofocusing– thermodesorption unit, which we developed for quantitative analysis of halogenated trace gases in ambient air. Possible applications include aircraft-based in situ measurements, in situ monitoring and laboratory operation for the analysis of flask samples. Analytes are trapped on adsorptive material cooled by a Stirling cooler to low temperatures (e.g. -80°C) and subsequently desorbed by rapid heating of the adsorptive material (e.g. 200°C). The set-up involves neither the exchange of adsorption tubes nor any further condensation or refocusing steps. No moving parts are used that would require vacuum insulation. This allows for a simple and robust design. Reliable operation is ensured by the Stirling cooler, which neither contains a liquid refrigerant nor requires refilling a cryogen. At the same time, it allows for significantly lower adsorption temperatures compared to commonly used Peltier elements. We use gas chromatography – mass spectrometry (GC–MS) for separation and detection of the preconcentrated analytes after splitless injection. A substance boiling point range of approximately -80 to +150°C and a substance mixing ratio range of less than 1 ppt (pmol mol−1)to more than 500 ppt in preconcentrated sample volumes of 0.1 to 10 L of ambient air is covered, depending on the application and its analytical demands. We present the instrumental design of the preconcentration unit and demonstrate capabilities and performance through the examination of analyte breakthrough during adsorption, repeatability of desorption and analyte residues in blank tests. Examples of application are taken from the analysis of flask samples collected at Mace Head Atmospheric Research Station in Ireland using our laboratory GC–MS instruments and by data obtained during a research flight with our in situ aircraft instrument GhOSTMS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer).
We present a compact and versatile cryofocusing–thermodesorption unit, which we developed for quantitative analysis of halogenated trace gases in ambient air. Possible applications include aircraft-based in situ measurements, in situ monitoring and laboratory operation for the analysis of flask samples. Analytes are trapped on adsorptive material cooled by a Stirling cooler to low temperatures (e.g. −80 °C) and subsequently desorbed by rapid heating of the adsorptive material (e.g. +200 °C). The set-up involves neither the exchange of adsorption tubes nor any further condensation or refocusing steps. No moving parts are used that would require vacuum insulation. This allows for a simple and robust design. Reliable operation is ensured by the Stirling cooler, which neither contains a liquid refrigerant nor requires refilling a cryogen. At the same time, it allows for significantly lower adsorption temperatures compared to commonly used Peltier elements. We use gas chromatography – mass spectrometry (GC–MS) for separation and detection of the preconcentrated analytes after splitless injection. A substance boiling point range of approximately −80 to +150 °C and a substance mixing ratio range of less than 1 ppt (pmol mol−1) to more than 500 ppt in preconcentrated sample volumes of 0.1 to 10 L of ambient air is covered, depending on the application and its analytical demands. We present the instrumental design of the preconcentration unit and demonstrate capabilities and performance through the examination of analyte breakthrough during adsorption, repeatability of desorption and analyte residues in blank tests. Examples of application are taken from the analysis of flask samples collected at Mace Head Atmospheric Research Station in Ireland using our laboratory GC–MS instruments and by data obtained during a research flight with our in situ aircraft instrument GhOST-MS (Gas chromatograph for the Observation of Tracers – coupled with a Mass Spectrometer).
Baumeister, Sarah ; Mößnang, Carolin Ulrike ; Bast, Nico ; Hohmann, Sarah ; Tillmann, Julian ; Goyard, David ; Charman, Tony ; Ambrosino, Sara ; Baron-Cohen, Simon ; Beckmann, Christian F. ; Bölte, Sven ; Bourgeron, Thomas ; Rausch, Annika ; Crawley, Daisy ; Dell'Acqua, Flavio ; Dumas, Guillaume ; Durston, Sarah ; Ecker, Christine ; Floris, Dorothea L. ; Frouin, Vincent ; Hayward, Hannah ; Holt, Rosemary ; Johnson, Mark H. ; Jones, Emily J. H. ; Lai, Meng-Chuan ; Lombardo, Michael V. ; Mason, Luke ; Oldehinkel, Marianne ; Persico, Tony ; San José Cáceres, Antonia ; Wolfers, Thomas ; Spooren, Willibrordus Philippus Johannes Maria ; Loth, Eva ; Murphy, Declan G. M. ; Buitelaar, Jan K. ; Tost, Heike ; Meyer-Lindenberg, Andreas ; Banaschewski, Tobias ; Brandeis, Daniel
Background Reward processing has been proposed to underpin atypical social behavior, a core feature of autism spectrum disorder (ASD). However, previous neuroimaging studies have yielded inconsistent results regarding the specificity of atypicalities for social rewards in ASD. Utilizing a large sample, we aimed to assess altered reward processing in response to reward type (social, monetary) and reward phase (anticipation, delivery) in ASD.
Methods Functional magnetic resonance imaging during social and monetary reward anticipation and delivery was performed in 212 individuals with ASD (7.6-30.5 years) and 181 typically developing (TD) participants (7.6-30.8 years).
Results Across social and monetary reward anticipation, whole-brain analyses (p<0.05, family-wise error-corrected) showed hypoactivation of the right ventral striatum (VS) in ASD. Further, region of interest (ROI) analysis across both reward types yielded hypoactivation in ASD in both the left and right VS. Across delivery of social and monetary reward, hyperactivation of the VS in individuals with ASD did not survive correction for multiple comparisons. Reward type by diagnostic group interactions, and a dimensional analysis of autism trait scores were not significant during anticipation or delivery. Levels of attention-deficit/hyperactivity disorder (ADHD) symptoms did not affect reward processing in ASD.
Conclusions Our results do not support current theories linking atypical social interaction in ASD to specific alterations in processing of social rewards. Instead, they point towards a generalized hypoactivity of VS in ASD during anticipation of both social and monetary rewards. We suggest that this indicates attenuated subjective reward value in ASD independent of social content and ADHD symptoms.