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Verdunstungsstudien
(1930)
Mit Hilfe von Apparaten wird es wohl niemals gelingen, die tatsachliche Verdunstung bestimmter Landflächen zu bestimmen, so wichtig eine derartige Ermittlung im Hinblick auf Klimaforschung, Wasserhaushalt der Erde und dergleichen sein mag. Es wurde daher schon aud die verschiedensten Arten versucht, wenigstens ein relatives Maß der Verdunstung - die sogenannte Verdunstungskraft zu bestimmen. Freie Wasserflächen für eine derartige Untersuchung zu verwenden, wäre das Einfachste ; jedoch sind hierbei die Möglichkeiten einer Störung besonders groß infolge von Einflüssen, die die gemessene Verdunstungskraft verändern, und so Fälschungen der Messungen verursachen. Es seien hier nur die Störiingon durch Regen, den Rand der Schale, Verunreinigungen der Oberflache und durch Wellenbildung erwähnt. Darum scheint es vorteilhafter, wie bereits Babinetl 1848 vorschlug, für derartige Messungen statt der freien Wasserfläche einen porösen Tonkörper zu verwenden. Mitscherlich und Livingstone begannen dann ziemlich gleichzeitig 1904 mit derartigen Tonkörpern zu arbeiten, und Livingstone trat bald mit seinen vor allem für die Botanik wichtigen Ergebnissen hervor. Aufgabe des Meteorologen ist, eine Methode zu schaffen, die eine stets wiederholbare Messung ermöglicht; jedoch muß man sich dessen befaßt sein, daß solche Messungen keinesfalls die Verdunstungswerte der Erdoberfläche mit oder ohne Vegetation oder die Wasserabgabe des Menschen angeben. Das Verhältnis dieser, der "natürlichen" Verdunstungswerte, zu dem durch jene im folgenden erörterte - Methode gefundenen "physikalischen" Werte bedarf noch der Ermittlung. Über die Sondergebiete der Verdunstung liegen bereits zahlreiche Arbeiten vor. In dieser Arbeit wird zuerst die verwendete Apparatur und die Meßanordnung besprochen, dann der Einfluß des Windes, der Temperatur und des äußeren Dampfdruckes auf die Verdunstung untersucht. Darauf wird die durch die Verdunstung selbst erzeugte Ventilation, die "Grundventilation" behandelt. Es schließt sich die Ermittliing des Strahlungseinflusses und die Eignung des Apparates zu Strahlungsmessungen an, und zum Schluß werden Vergleichsmessungen mit anderen Apparaten angeführt.
Ein Finite-Volumen-Modell des differentiell geheizten rotierenden Annulus wird verwendet, um die spontane Schwerewellenabstrahlung durch die großskalige, von baroklinen Wellen beherrschte Strömung zu untersuchen. Bei diesem Vorgang bilden barokline Wellen und der durch sie abgelenkte und verzerrte Strahlstrom, die sich näherungsweise im hydrostatischen und geostrophischen Gleichgewicht befinden, durch ihre Dynamik Ungleichgewichte aus, die sich als Schwerewellen ausbreiten. Neben der Anregung von Schwerewellen durch Prozesse wie Gebirgsüberströmung, Konvektion und Frontogenese, bildet dieser Vorgang vermutlich eine weitere wichtige Quelle von Schwerewellen in der Atmosphäre. Anders als für orographisch und konvektiv angeregte Schwerewellen gibt es für die spontane Schwerewellenabstrahlung bislang keine befriedigende Parametrisierung in Wettervorhersage- und Klimamodellen, die diesen Prozess nicht auflösen können. Die Durchführung von Messungen zur spontanen Schwerewellenabstrahlung in der Atmosphäre ist üblicherweise sehr aufwendig, sodass die Untersuchung dieses Vorganges in einem wiederholbaren und steuerbaren Laborexperiment reizvoll erscheint. Ob dafür möglicherweise das Experiment des differentiell geheizten rotierenden Annulus infrage kommt, untersuchen wir mit einem eigens dafür entwickelten numerischen Modell, dessen Tauglichkeit wir zunächst im Rahmen einer Validierung durch den Vergleich mit Labormessungen überprüfen. Damit die Ergebnisse zur Schwerewellendynamik im Annulus auf die Atmosphäre übertragbar sind, verwenden wir eine neue, atmosphärenähnliche Annuluskonfiguration. Im Gegensatz zu den klassischen Annuluskonfigurationen ist in der neuen Konfiguration die Brunt-Väisälä-Frequenz größer als der Coriolis-Parameter, sodass die Schwerewellen ein ähnliches Ausbreitungsverhalten zeigen sollten wie in der Atmosphäre. Deutliche Hinweise auf eine Schwerewellenaktivität in der atmosphärenähnlichen Konfiguration geben die horizontale Geschwindigkeitsdivergenz und eine Normalmodenzerlegung der kleinräumigen Strukturen der simulierten Strömung. Um der Herkunft der beobachteten Schwerewellen auf den Grund zu gehen, zerlegen wir die Strömung in den schwerewellenfreien quasigeostrophischen Anteil und den schwerewellenenthaltenden ageostrophischen Anteil. Bereiche innerhalb der baroklinen Welle, in denen ein erhöhter spontaner Antrieb des ageostrophischen Anteils durch die quasigeostrophische Strömung beobachtet wird, fallen mit Bereichen erhöhter Schwerewellenaktivität zusammen. Dies deutet darauf hin, dass die spontane Schwerewellenabstrahlung auch im Annulus zum Schwerewellenfeld beiträgt, sodass dieses Experiment als Labormodell dieser Schwerewellenquelle für deren weitere Erforschung geeignet erscheint.
Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase.
For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.
Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Tra ditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies. Only recently some feldspar species were identified to be ice-active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase.
For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands and the Sinai Peninsula). Additionally, eleven dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore we investigated how representative ice nucleation on surface-collected dust is for that in the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC set-up to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 - 250 K. Dust particles were collected in parallel on filters for offline cold stage ice nucleation experiments at 253 - 263 K. To help the interpretation of the results from the ice nucleation experiments the mineralogical composition of the dusts was investigated.We found that a higher ice nucleation activity in a given sample can be attributed at 253 K to the K-feldspar content present in this sample whereas at temperatures between 238 - 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content on the other hand is associated with a lower ice nucleation activity of a sample. This confirms the importance of feldspar at T > 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower T as found by earlier studies for monomineral dust surrogates. Furthermore, we find that milling may lead to a decrease in the ice nucleation ability of polymineral samples due to a change in mineralogical composition in the atmospherically relevant size fraction arising from the different hardness and cleavage of individual mineral phases. Comparison of our comprehensive data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modelling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key while other minerals are only of minor importance.
In this study we report the set-up of a novel twin chamber technique that uses the comparative method and establishes an appropriate connection of atmospheric and laboratory methods to broaden the tools for investigations. It is designed to study the impact of certain parameters and gases on ambient processes, such as particle formation online, and can be applied in a large variety of conditions. The characterisation of both chambers proved that both chambers operate identically, with a residence time xT (COMPASS1) = 26.5 ± 0.3 min and xT (COMPASS2) = 26.6 ± 0.4 min, at a typical flow rate of 15 L min−1 and a gas leak rate of (1.6 ± 0.8) × 10−5 s−1. Particle loss rates were found to be larger (due to the particles' stickiness to the chamber walls), with an extrapolated maximum of 1.8 × 10−3 s−1 at 1 nm, i.e. a hundredfold of the gas leak rate. This latter value is associated with sticky non-volatile gaseous compounds, too. Comparison measurement showed no significant differences. Therefore operation under atmospheric conditions is trustworthy. To indicate the applicability and the benefit of the system, a set of experiments was conducted under different conditions, i.e. urban and remote, enhanced ozone and terpenes as well as reduced sunlight. In order to do so, an ozone lamp was applied to enhance ozone in one of two chambers; the measurement chamber was protected from radiation by a first-aid cover and volatile organic compounds (VOCs) were added using a small additional flow and a temperature-controlled oven. During the elevated ozone period, ambient particle number and volume increased substantially at urban and remote conditions, but by a different intensity. Protection of solar radiation displayed a clear negative effect on particle number, while terpene addition did cause a distinct daily pattern. E.g. adding β pinene particle number concentration rose by 13% maximum at noontime, while no significant effect was observable during darkness. Therefore, the system is a useful tool for investigating local precursors and the details of ambient particle formation at surface locations as well as potential future feedback processes.
The anthropogenic influence on climate and environment has increased strongly since industrialization about 150 yr ago. The consequences for the atmosphere became more and more apparent and nowadays affect our life quality on Earth progressively. Because of that it is very important to understand the atmospheric processes, on which these effects are based on, in detail. In this study we report the set-up of a novel twin chamber technique that uses the comparative method and establishes an appropriate connection of atmospheric and laboratory methods to broaden the tools for investigations. It is designed to study the impact of certain parameters and gases on ambient processes such as particle formation online and can be applied in a large variety of conditions. The characterisation of both chambers proved that both chambers operate identically with a residence time (xT (COMPASS 1) = 26.5 ± 0.3 min and xT (COMPASS 2) = 26.6 ± 0.4 min) at a typical flow rate of 15 L min−1 and a deposition rate (1.6 ± 0.8) × 10−5 s−1. Comparison measurement showed no significant differences. Therefore operation under atmospheric conditions is trustworthy. To indicate the applicability and the benefit of the system a set of experiments was conducted at different conditions, i.e. urban and remote, enhancing ozone and terpenes as well as reducing sunlight. In the ozone enhanced ambient particle number and volume increased substantially at urban and remote conditions in a different strength. Solar radiation displayed a clear positive effect on particle number as well as terpene addition did at remote conditions. Therefore the system is a useful tool to investigate local precursors, the details of ambient particle formation at surface locations as well as future feedback processes.
Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is described as a function of gaseous sulfuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites. Here we introduce a new nucleation parameter including ozone and water vapor concentrations as well as UV-B radiation as a proxy for OH radical formation. Applying this new parameter to field studies conducted at Finnish and German measurement sites it is found capable to predict the occurrence of nucleation events and their seasonal and annual variation indicating a significant role of organics. Extrapolation to possible future conditions of ozone, water vapor and organic concentrations leads to a significant potential increase in nucleation event number.
Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is either parameterised as a function of gaseous sulphuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites, or as a function of sulphuric acid and organic molecules. Here we introduce different nucleation parameters based on the interaction of sulphuric acid and terpene oxidation products and elucidate the individual importance. They include basic trace gas and meteorological measurements such as ozone and water vapour concentrations, temperature (for terpene emission) and UV B radiation as a proxy for OH radical formation. We apply these new parameters to field studies conducted at conducted at Finnish and German measurement sites and compare these to nucleation observations on a daily and annual scale. General agreement was found, although the specific compounds responsible for the nucleation process remain speculative. This can be interpreted as follows: During cooler seasons the emission of biogenic terpenes and the OH availability limits the new particle formation while towards warmer seasons the ratio of ozone and water vapour concentration seems to dominate the general behaviour. Therefore, organics seem to support ambient nucleation besides sulphuric acid or an OH-related compound. Using these nucleation parameters to extrapolate the current conditions to prognosed future concentrations of ozone, water vapour and organic concentrations leads to a significant potential increase in the nucleation event number.
The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany
(2013)
It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulphuric acid. However, the activation process of sulphuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus on the PARADE campaign measurements conducted during August/September 2011 at Mt. Kleiner Feldberg in central Germany. During this campaign a set of radicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulphuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilized Criegee intermediates (sCI). This novel laboratory derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during daytime and NO3 during nighttime. Because of the RO2s lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should to be taken into account when studying the impact of new particles in climate feedback cycles.