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Bajnai, David ; Guo, Weifu ; Spötl, Christoph ; Coplen, Tyler B. ; Methner, Katharina ; Löffler, Niklas ; Krsnik, Emilija ; Gischler, Eberhard ; Hansen, Maximilian ; Henkel, Daniela ; Price, Gregory D. ; Raddatz, Jacek ; Scholz, Denis ; Fiebig, Jens
Surface temperature is a fundamental parameter of Earth’s climate. Its evolution through time is commonly reconstructed using the oxygen isotope and the clumped isotope compositions of carbonate archives. However, reaction kinetics involved in the precipitation of carbonates can introduce inaccuracies in the derived temperatures. Here, we show that dual clumped isotope analyses, i.e., simultaneous ∆47 and ∆48 measurements on the single carbonate phase, can identify the origin and quantify the extent of these kinetic biases. Our results verify theoretical predictions and evidence that the isotopic disequilibrium commonly observed in speleothems and scleractinian coral skeletons is inherited from the dissolved inorganic carbon pool of their parent solutions. Further, we show that dual clumped isotope thermometry can achieve reliable palaeotemperature reconstructions, devoid of kinetic bias. Analysis of a belemnite rostrum implies that it precipitated near isotopic equilibrium and confirms the warmer-than-present temperatures during the Early Cretaceous at southern high latitudes.
Thoma, Markus ; Bachmeier, Franziska ; Gottwald, Felix Leonard ; Simon, Mario ; Vogel, Alexander Lucas
Particulate matter (PM) largely consists of secondary organic aerosol (SOA) that is formed via oxidation of biogenic and anthropogenic volatile organic compounds (VOCs). Unambiguous identification of SOA molecules and their assignment to their precursor vapors is a challenge that has so far only succeeded for a few SOA marker compounds, which are now well characterized and (partly) available as authentic standards. In this work, we resolve the complex composition of SOA by a top-down approach based on a newly created aerosolomics database, which is fed by non-target analysis results of filter samples from oxidation flow reactor experiments. We investigated the oxidation products from the five biogenic VOCs α-pinene, β-pinene, limonene, 3-carene, and trans-caryophyllene and from the four anthropogenic VOCs toluene, o-xylene, 1,2,4-trimethylbenzene, and naphthalene. Using ultra-high performance liquid chromatography coupled to a high-resolution (Orbitrap) mass spectrometer, we determine the molecular formula of 596 chromatographically separated compounds based on exact mass and isotopic pattern. We utilize retention time and fragmentation mass spectra as a basis for unambiguous attribution of the oxidation products to their parent VOCs. Based on the molecular-resolved application of the database, we are able to assign roughly half of the total signal of oxygenated hydrocarbons in ambient suburban PM2.5 to one of the nine studied VOCs. The application of the database enabled us to interpret the appearance of diurnal compound clusters that are formed by different oxidation processes. Furthermore, the application of a hierarchical cluster analysis (HCA) on the same set of filter samples enabled us to identify compound clusters that depend on sulfur dioxide mixing ratio and temperature. This study demonstrates how aerosolomics tools (database and HCA) applied on PM filter samples can improve our understanding of SOA sources, their formation pathways, and temperature-driven partitioning of SOA compounds.
Thoma, Markus ; Bachmeier, Franziska ; Gottwald, Felix Leonard ; Simon, Mario ; Vogel, Alexander Lucas
Particulate matter (PM) largely consists of secondary organic aerosol (SOA) that is formed via oxidation of biogenic and anthropogenic volatile organic compounds (VOCs). Unambiguous identification of SOA molecules and their assignment to their precursor vapors are challenges that have so far only succeeded for a few SOA marker compounds, which are now well characterized and (partly) available as authentic standards. In this work, we resolve the complex composition of SOA by means of a top-down approach based on the newly created Aerosolomics database, which is fed by non-target analysis results of filter samples from oxidation flow reactor experiments. We investigated the oxidation products from the five biogenic VOCs α-pinene, β-pinene, limonene, 3-carene, and trans-caryophyllene and from the four anthropogenic VOCs toluene, o-xylene, 1,2,4-trimethylbenzene, and naphthalene. Using ultrahigh-performance liquid chromatography coupled to a high-resolution (Orbitrap) mass spectrometer, we determine the molecular formula of 596 chromatographically separated compounds based on exact mass and isotopic pattern. We utilize retention time and fragmentation mass spectra as a basis for unambiguous attribution of the oxidation products to their parent VOCs. Based on the molecular-resolved application of the database, we are able to assign roughly half of the total signal of oxygenated hydrocarbons in ambient suburban PM2.5 to one of the nine studied VOCs. The application of the database enabled us to interpret the appearance of diurnal compound clusters that are formed by different oxidation processes. Furthermore, by performing a hierarchical cluster analysis (HCA) on the same set of filter samples, we identified compound clusters that depend on sulfur dioxide mixing ratio and temperature. This study demonstrates how Aerosolomics tools (database and HCA) applied to PM filter samples can improve our understanding of SOA sources, their formation pathways, and temperature-driven partitioning of SOA compounds.
In the deep-sea, the interaction between benthic fauna and substrate mainly occurs through bioturbational processes which can be preserved as traces (i.e., lebensspuren). Lebensspuren are common features of deep seafloor landscapes and usually more abundant than the organism that produce them (i.e., tracemakers), rendering them promising proxies to infer biodiversity. The density and diversity relationships between lebensspuren and benthic fauna are to the present day unclear and contradicting hypotheses have been proposed suggesting negative, positive, or even null correlations. To test these hypotheses, in this study lebensspuren, tracemakers (specific epibenthic fauna that produce these traces), degrading fauna (benthic fauna that can erase lebensspuren), and fauna in general were characterized taxonomically at eight deep-sea stations in the Kuril Kamchatka Trench area. No general correlation (over-all study area) could be observed between diversities of lebensspuren, tracemakers, degrading fauna and fauna. However, a diversity correlation was observed between specific stations, showing both negative and positive correlations depending on: 1) the number of unknown tracemakers (especially significant for dwelling lebensspuren); and 2) the lebensspuren with multiple origins; and 3) tracemakers that can produce different lebensspuren. Lebensspuren and faunal density were not correlated. However, lebensspuren density was either positively or negatively correlated with tracemaker densities, depending on the lebensspuren morphotypes. A positive correlation was observed for resting lebensspuren (e.g., ophiuroid impressions, Actinaria circular impressions), while negative correlations were observed for locomotion-feeding lebensspuren (e.g., echinoid trails). In conclusion, lebensspuren diversity may be a good proxy for tracemaker biodiversity when the lebensspuren-tracemaker tandem can be reliable characterized; and lebensspuren-density correlations vary depending the specific lebensspuren residence time, tracemaker density and associated behaviour (rate of movement), but on a global scale abiotic and other biotic 42 factors may also play an important role.
In the deep sea, interactions between benthic fauna and seafloor sediment primarily occur through bioturbation that can be preserved as traces (i.e. lebensspuren). Lebensspuren are common features of deep-sea landscapes and are more abundant than the organisms that produce them (i.e. tracemakers), rendering lebensspuren promising proxies for inferring biodiversity. The density and diversity relationships between lebensspuren and benthic fauna remain unclear, and contradicting correlations have been proposed (i.e. negative, positive, or even null correlations). To approach these variable correlations, lebensspuren and benthic fauna were characterized taxonomically at eight deep-sea stations in the Kuril-Kamchatka Trench area, together with two novel categories: tracemakers (specific epibenthic fauna that produce these traces) and degrading fauna (benthic fauna that can erase lebensspuren). No general correlation (overall study area) was observed between diversities of lebensspuren, tracemakers, degrading fauna, and fauna. However, a diversity correlation was observed at specific stations, showing both negative and positive correlations depending on: (1) the number of unknown tracemakers (especially significant for dwelling lebensspuren); (2) the lebensspuren with multiple origins; and (3) tracemakers that can produce different lebensspuren. Lebensspuren and faunal density were not correlated. However, lebensspuren density was either positively or negatively correlated with tracemaker densities, depending on the lebensspuren morphotypes. A positive correlation was observed for resting lebensspuren (e.g. ophiuroid impressions, Actiniaria circular impressions), while negative correlations were observed for locomotion-feeding lebensspuren (e.g. echinoid trails). In conclusion, lebensspuren diversity may be a good proxy for tracemaker biodiversity when the lebensspuren–tracemaker relationship can be reliable characterized. Lebensspuren–density correlations vary depending on the specific lebensspuren residence time, tracemaker density, and associated behaviour (rate of movement). Overall, we suggest that lebensspuren density and diversity correlations should be studied with tracemakers rather than with general benthic fauna. On a global scale, abiotic (e.g. hydrodynamics, substrate consistency) and other biotic factors (e.g. microbial degradation) may also play an important role.
Measurements of vertical velocity from vertically pointing Doppler lidars are used to derive the profiles of vertical velocity variance. Observations were taken during the FESSTVaL (Field Experiment on Submesoscale Spatio-Temporal Variability in Lindenberg) campaign during the warm seasons of 2020 and 2021. Normalized by the square of convective velocity scale, the average vertical velocity variance profile follows the universal profile of Lenschow et al. (1980), however, daily profiles still show a high day-to-day variability. We found that moisture transport and the content of moisture in the boundary layer could explain the remaining variability of the normalized vertical velocity variance. The magnitude of the normalized vertical velocity variance is highest on clear-sky days, and decreases as the relative humidity increase and surface latent heat flux decrease in cloud-topped and rainy days. This suggests that moisture content and moisture transport are limiting factors for the intensity of turbulence in the convective boundary layer. We also found that the intensity of turbulence decreases with an increase in boundary layer cloud fraction during FESSTVaL, while the latent heating in the cloud layer was not a relevant source of turbulence in this case. We conclude that a new vertical velocity scale has to be defined that would take into account the moist processes in the convective boundary layer.
Measurements of vertical velocity from vertically pointing Doppler lidars are used to derive the profiles of normalized vertical velocity variance. Observations were taken during the FESSTVaL (Field Experiment on Submesoscale Spatio-Temporal Variability in Lindenberg) campaign during the warm seasons of 2020 and 2021. Normalized by the square of the convective velocity scale, the average vertical velocity variance profile follows the universal profile of Lenschow et al. (1980). However, daily profiles still show a high day-to-day variability. We found that moisture transport and the content of moisture in the boundary layer could explain the remaining variability of the normalized vertical velocity variance. The magnitude of the normalized vertical velocity variance is highest on clear-sky days and decreases as the absolute humidity increases and surface latent heat flux decreases on cloud-topped days. This suggests that moisture content and moisture transport are limiting factors for the intensity of turbulence in the convective boundary layer. We also found that the intensity of turbulence decreases with an increase in the boundary layer cloud fraction during FESSTVaL, while the latent heating in the cloud layer was not a relevant source of turbulence in this case. We conclude that a new vertical velocity scale has to be defined that would take into account the moist processes in the convective boundary layer.
Haussühl, Eiken ; Reichmann, Hans Josef ; Schreuer, Jürgen ; Friedrich, Alexandra ; Hirschle, Christian ; Bayarjargal, Lkhamsuren ; Winkler, Björn ; Alencar, Igor ; Wiehl, Leonore ; Ganschow, Steffen
A comprehensive study of sillenite Bi12SiO20 single-crystal properties, including elastic stiffness and piezoelectric coefficients, dielectric permittivity, thermal expansion and molar heat capacity, is presented. Brillouin-interferometry measurements (up to 27 GPa), which were performed at high pressures for the first time, and ab initio calculations based on density functional theory (up to 50 GPa) show the stability of the sillenite structure in the investigated pressure range, in agreement with previous studies. Elastic stiffness coefficients c11 and c12 are found to increase continuously with pressure while c44 increases slightly for lower pressures and remains nearly constant above 15 GPa. Heat-capacity measurements were performed with a quasi-adiabatic calorimeter employing the relaxation method between 2 K and 395 K. No phase transition could be observed in this temperature interval. Standard molar entropy, enthalpy change and Debye temperature are extracted from the data. The results are found to be roughly half of the previous values reported in the literature. The discrepancy is attributed to the overestimation of the Debye temperature which was extracted from high-temperature data. Additionally, Debye temperatures obtained from mean sound velocities derived by Voigt-Reuss averaging are in agreement with our heat-capacity results. Finally, a complete set of electromechanical coefficients was deduced from the application of resonant ultrasound spectroscopy between 103 K and 733 K. No discontinuities in the temperature dependence of the coefficients are observed. High-temperature (up to 1100 K) resonant ultrasound spectra recorded for Bi12MO20 crystals revealed strong and reversible acoustic dissipation effects at 870 K, 960 K and 550 K for M = Si, Ge and Ti, respectively. Resonances with small contributions from the elastic shear stiffness c44 and the piezoelectric stress coefficient e123 are almost unaffected by this dissipation.
Harrison, Sandy P. ; Villegas-Diaz, Roberto ; Cruz-Silva, Esmeralda ; Gallagher, Daniel ; Kesner, David ; Lincoln, Paul ; Shen, Yicheng ; Sweeney, Luke ; Colombaroli, Daniele ; Ali, Adam ; Barhoumi, Chéïma ; Bergeron, Yves ; Blyakharchuk, Tatiana ; Bobek, Přemysl ; Bradshaw, Richard ; Clear, Jennifer L. ; Czerwiński, Sambor ; Daniau, Anne-Laure ; Dodson, John ; Edwards, Kevin J. ; Edwards, Mary E. ; Feurdean, Angelica ; Foster, David ; Gajewski, Konrad ; Gałka, Mariusz ; Garneau, Michelle ; Giesecke, Thomas ; Gil Romera, Graciela ; Girardin, Martin P. ; Höfer, Dana ; Huang, Kangyou ; Inoue, Jun ; Jamrichová, Eva ; Jasiunas, Nauris ; Jiang, Wenying ; Jiménez-Moreno, Gonzalo ; Karpińska-Kołaczek, Monika ; Kołaczek, Piotr ; Kuosmanen, Niina ; Lamentowicz, Mariusz ; Lavoie, Martin ; Li, Fang ; Li, Jianyong ; Lisitsyna, Olga ; López-Sáez, José Antonio ; Luelmo-Lautenschlaeger, María de los Reyes ; Magnan, Gabriel ; Magyari, Eniko Katalin ; Maksims, Alekss ; Marcisz, Katarzyna ; Marinova, Elena ; Marlon, Jenn ; Mensing, Scott ; Miroslaw-Grabowska, Joanna ; Oswald, Wyatt ; Pérez-Dı́az, Sebastián ; Pérez-Obiol, Ramón ; Piilo, Sanna ; Poska, Anneli ; Qin, Xiaoguang ; Remy, Cécile ; Richard, Pierre J. H. ; Salonen, Sakari ; Sasaki, Naoko ; Schneider, Heike ; Shotyk, William ; Stančikaitė, Migle ; Šteinberga, Dace ; Stivriņš, Normunds ; Takahara, Hikaru ; Tan, Zhihai ; Trasune, Liva ; Umbanhowar, Charles E. ; Väliranta, Minna ; Vassiljev, Jüri ; Xiao, Xiayun ; Xu, Qinghai ; Xu, Xin ; Zawisza, Edyta ; Zhao, Yan ; Zhou, Zheng ; Paillard, Jordan
Sedimentary charcoal records are widely used to reconstruct regional changes in fire regimes through time in the geological past. Existing global compilations are not geographically comprehensive and do not provide consistent metadata for all sites. Furthermore, the age models provided for these records are not harmonised and many are based on older calibrations of the radiocarbon ages. These issues limit the use of existing compilations for research into past fire regimes. Here, we present an expanded database of charcoal records, accompanied by new age models based on recalibration of radiocarbon ages using IntCal20 and Bayesian age-modelling software. We document the structure and contents of the database, the construction of the age models, and the quality control measures applied. We also record the expansion of geographical coverage relative to previous charcoal compilations and the expansion of metadata that can be used to inform analyses. This first version of the Reading Palaeofire Database contains 1676 records (entities) from 1480 sites worldwide. The database (RPDv1b – Harrison et al., 2021) is available at https://doi.org/10.17864/1947.000345.