Thomas Peter


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Publications 1 - 10 of 102
  • Fahey, David W.; Gao, Ru-Shan; Möhler, Ottmar; et al. (2014)
    Atmospheric Measurement Techniques
    The AquaVIT-1 intercomparison of atmospheric water vapor measurement techniques was conducted at the aerosol and cloud simulation chamber AIDA (Aerosol Interaction and Dynamics in the Atmosphere) at the Karlsruhe Institute of Technology, Germany, in October 2007. The overall objective was to intercompare state-of-the-art and prototype atmospheric hygrometers with each other and with independent humidity standards under controlled conditions. This activity was conducted as a blind intercomparison with coordination by selected referees. The effort was motivated by persistent discrepancies found in atmospheric measurements involving multiple instruments operating on research aircraft and balloon platforms, particularly in the upper troposphere and lower stratosphere, where water vapor reaches its lowest atmospheric values (less than 10 ppm). With the AIDA chamber volume of 84 m3, multiple instruments analyzed air with a common water vapor mixing ratio, by extracting air into instrument flow systems, by locating instruments inside the chamber, or by sampling the chamber volume optically. The intercomparison was successfully conducted over 10 days during which pressure, temperature, and mixing ratio were systematically varied (50 to 500 hPa, 185 to 243 K, and 0.3 to 152 ppm). In the absence of an accepted reference instrument, the absolute accuracy of the instruments was not established. To evaluate the intercomparison, the reference value was taken to be the ensemble mean of a core subset of the measurements. For these core instruments, the agreement between 10 and 150 ppm of water vapor is considered good with variation about the reference value of about ±10% (±1σ). In the region of most interest between 1 and 10 ppm, the core subset agreement is fair with variation about the reference value of ±20% (±1σ). The upper limit of precision was also derived for each instrument from the reported data. The implication for atmospheric measurements is that the substantially larger differences observed during in-flight intercomparisons stem from other factors associated with the moving platforms or the non-laboratory environment. The success of AquaVIT-1 provides a template for future intercomparison efforts with water vapor or other species that are focused on improving the analytical quality of atmospheric measurements on moving platforms.
  • Vattioni, Sandro; Weber, Rahel; Feinberg, Aryeh; et al. (2024)
    Geoscientific Model Development
    Recent studies have suggested that injection of solid particles such as alumina and calcite particles for stratospheric aerosol injection (SAI) instead of sulfur-based injections could reduce some of the adverse side effects of SAI such as ozone depletion and stratospheric heating. Here, we present a version of the global aerosol–chemistry–climate model SOCOL-AERv2 and the Earth system model (ESM) SOCOLv4 which incorporate a solid-particle microphysics scheme for assessment of SAI of solid particles. Microphysical interactions of the solid particle with the stratospheric sulfur cycle were interactively coupled to the heterogeneous chemistry scheme and the radiative transfer code (RTC) for the first time within an ESM. Therefore, the model allows simulation of heterogeneous chemistry at the particle surface as well as feedbacks between microphysics, chemistry, radiation and climate. We show that sulfur-based SAI results in a doubling of the stratospheric aerosol burden compared to the same mass injection rate of calcite and alumina particles with a radius of 240 nm. Most of the sulfuric acid aerosol mass resulting from SO2 injection does not need to be lifted to the stratosphere but is formed after in situ oxidation and subsequent water uptake in the stratosphere. Therefore, to achieve the same radiative forcing, larger injection rates are needed for calcite and alumina particle injection than for sulfur-based SAI. The stratospheric sulfur cycle would be significantly perturbed, with a reduction in stratospheric sulfuric acid burden by 53 %, when injecting 5 Mt yr⁻¹ (megatons per year) of alumina or calcite particles of 240 nm radius. We show that alumina particles will acquire a sulfuric acid coating equivalent to about 10 nm thickness if the sulfuric acid is equally distributed over the whole available particle surface area in the lower stratosphere. However, due to the steep contact angle of sulfuric acid on alumina particles, the sulfuric acid coating would likely not cover the entire alumina surface, which would result in available surface for heterogeneous reactions other than the ones on sulfuric acid. When applying realistic uptake coefficients of 1.0, 10⁻⁵ and 10⁻⁴ for H₂SO₄, HCl and HNO₃, respectively, the same scenario with injections of calcite particles results in 94 % of the particle mass remaining in the form of CaCO₃. This likely keeps the optical properties of the calcite particles intact but could significantly alter the heterogeneous reactions occurring on the particle surfaces. The major process uncertainties of solid-particle SAI are (1) the solid-particle microphysics in the injection plume and degree of agglomeration of solid particles on the sub-ESM grid scale, (2) the scattering properties of the resulting agglomerates, (3) heterogeneous chemistry on the particle surface, and (4) aerosol–cloud interactions. These uncertainties can only be addressed with extensive, coordinated experimental and modelling research efforts. The model presented in this work offers a useful tool for sensitivity studies and incorporating new experimental results on SAI of solid particles.
  • Stenke, Andrea; Schraner, Martin; Rozanov, Eugene; et al. (2012)
    Geoscientific Model Development
    We present the third generation of the coupled chemistry-climate model (CCM) SOCOL(modeling tools for studies of SOlar Climate Ozone Links). The most notable modifi-cations compared to the previous model version are: (1) the dynamical core has beenupdated with the fifth generation of the middle-atmosphere general circulation model5MA-ECHAM, and (2) the advection of the chemical species is now calculated by amass-conserving and shape-preserving flux-form transport scheme instead of the pre-viously used hybrid advection scheme. The whole chemistry code has been rewrittenaccording to the ECHAM5 infrastructure and transferred to Fortran95. In contrast to itspredecessors, SOCOLvs3 is now fully parallelized. The performance of the new SO-10COL version is evaluated on the basis of transient model simulations (1975–2004) withdifferent horizontal (T31 and T42) resolutions, following the approach of the CCMVal-1model validation activity. The advanced advection scheme significantly reduces the ar-tificial loss and accumulation of tracer mass in regions with strong gradients that wasobserved in previous model versions. Compared to its predecessors, SOCOLvs3 gen-15erally shows more realistic distributions of chemical trace species, especially of totalinorganic chlorine, in terms of the mean state, but also of the annual and interannualvariability. Advancements with respect to model dynamics are for example a better rep-resentation of the stratospheric mean state in spring, especially in the Southern Hemi-sphere, and a slowdown of the upward propagation in the tropical lower stratosphere.20Despite a large number of improvements model deficiencies still remain. Examples in-clude a too fast vertical ascent and/or horizontal mixing in the tropical stratosphere, thecold temperature bias in the lowermost polar stratosphere, and the overestimation ofpolar total ozone loss during Antarctic springtime.
  • Arsenovic, P.; Damiani, Alessandro; Rozanov, Eugene; et al. (2019)
    Atmospheric Chemistry and Physics
    Energetic particle precipitation (EPP) affects the chemistry of the polar middle atmosphere by producing reactive nitrogen (NOy) and hydrogen (HOx) species, which then catalytically destroy ozone. Recently, there have been major advances in constraining these particle impacts through a parametrization of NOy based on high-quality observations. Here we investigate the effects of low (auroral) and middle (radiation belt) energy range electrons, separately and in combination, on reactive nitrogen and hydrogen species as well as on ozone during Southern Hemisphere winters from 2002 to 2010 using the SOCOL3-MPIOM chemistry-climate model. Our results show that, in the absence of solar proton events, low-energy electrons produce the majority of NOy in the polar mesosphere and stratosphere. In the polar vortex, NOy subsides and affects ozone at lower altitudes, down to 10 hPa. Comparing a year with high electron precipitation with a quiescent period, we found large ozone depletion in the mesosphere; as the anomaly propagates downward, 15 % less ozone is found in the stratosphere during winter, which is confirmed by satellite observations. Only with both low- and middle-energy electrons does our model reproduce the observed stratospheric ozone anomaly.
  • Weydert, Serge; Girardin, Sophie; Cui, Xinnan; et al. (2019)
    Langmuir
  • Klumpp, Kristian; Marcolli, Claudia; Alonso-Hellweg, Ana; et al. (2023)
    Atmospheric Chemistry and Physics
    Heterogeneous ice nucleation on dust particles in the atmosphere is a key mechanism for ice formation in clouds. However, the conditions of a particle surface for efficient ice nucleation are poorly understood. In this study, we present results of immersion freezing experiments using differential scanning calorimetry on emulsified mineral dust suspensions, involving the two chemically identical, but morphologically different, kaolin minerals of kaolinite and halloysite. Kaolinite occurs in a platy morphology, while halloysites form predominantly tubular structures. We investigated six different halloysite and two different kaolinite samples. Our results show that, on average, the halloysite samples not only exhibit a higher ice nucleation (IN) activity than the kaolinite samples but also a higher diversity in terms of freezing onset temperatures and heterogeneously frozen fraction. Repeating the freezing experiments after shortly milling the samples led to a decrease in freezing onset temperatures and in the heterogeneously frozen fraction of the halloysite samples, bringing their IN activity closer to that of the kaolinites. To interpret these findings, the freezing experiments were complemented by dynamic vapor sorption (DVS), BET (Brunauer-Emmett-Teller) surface area measurements, pore ice melting experiments with slurries, and transmission electron microscopy (TEM) before and after milling. These measurements demonstrate an increase in surface area and the destruction of tubes by milling and provide evidence for the influence of the tubular structure of the halloysites on their IN activity. We identify the OH-Al-O-Si-OH functionalized edges as being the most likely site for ice nucleation, as the high geometric diversity of the edges best accounts for the high diversity in IN activity of halloysites. We hypothesize that the stacking of layers and the number of stacks in halloysite tubes and kaolinite platelets affect the freezing temperature, with thicker stacks having the potential to freeze water at higher temperatures. The notion that the edges constitute the IN-active part of kaolin minerals is further supported by comparing kaolin minerals with montmorillonites and feldspars, all of which exhibit enhanced IN activity in the presence of ammonia and ammonium-containing solutions. As OH-Al-O-Si-OH functionalized edge surfaces are the only surface type that kaolin particles have in common with montmorillonites and feldspars, the common feature of IN activity enhancement in ammoniated solutions can only be explained by ice nucleation occurring at the edges of kaolin minerals.
  • Stenke, Andrea; Schraner, Martin; Rozanov, Eugene; et al. (2013)
    Geoscientific Model Development
    We present the third generation of the coupled chemistry–climate model (CCM) SOCOL (modeling tools for studies of SOlar Climate Ozone Links). The most notable modifications compared to the previous model version are (1) the dynamical core has been updated with the fifth generation of the middle-atmosphere general circulation model MA-ECHAM (European Centre/HAMburg climate model), and (2) the advection of the chemical species is now calculated by a mass-conserving and shape-preserving flux-form transport scheme instead of the previously used hybrid advection scheme. The whole chemistry code has been rewritten according to the ECHAM5 infrastructure and transferred to Fortran95. In contrast to its predecessors, SOCOLvs3 is now fully parallelized. The performance of the new SOCOL version is evaluated on the basis of transient model simulations (1975–2004) with different horizontal (T31 and T42) resolutions, following the approach of the CCMVal-1 model validation activity. The advanced advection scheme significantly reduces the artificial loss and accumulation of tracer mass in regions with strong gradients that was observed in previous model versions. Compared to its predecessors, SOCOLvs3 generally shows more realistic distributions of chemical trace species, especially of total inorganic chlorine, in terms of the mean state, but also of the annual and interannual variability. Advancements with respect to model dynamics are for example a better representation of the stratospheric mean state in spring, especially in the Southern Hemisphere, and a slowdown of the upward propagation in the tropical lower stratosphere. Despite a large number of improvements model deficiencies still remain. Examples include a too-fast vertical ascent and/or horizontal mixing in the tropical stratosphere, the cold temperature bias in the lowermost polar stratosphere, and the overestimation of polar total ozone loss during Antarctic springtime.
  • Motos, Ghislain; Schaub, Aline; David, Shannon C.; et al. (2024)
    Frontiers in Microbiology
    We describe a novel biosafety aerosol chamber equipped with state-of-the-art instrumentation for bubble-bursting aerosol generation, size distribution measurement, and condensation-growth collection to minimize sampling artifacts when measuring virus infectivity in aerosol particles. Using this facility, we investigated the effect of relative humidity (RH) in very clean air without trace gases (except ∼400 ppm CO₂) on the preservation of influenza A virus (IAV) infectivity in saline aerosol particles. We characterized infectivity in terms of 99%-inactivation time, t₉₉, a metric we consider most relevant to airborne virus transmission. The viruses remained infectious for a long time, namely t₉₉ > 5 h, if RH < 30% and the particles effloresced. Under intermediate conditions of humidity (40% < RH < 70%), the loss of infectivity was the most rapid (t₉₉ ≈ 15–20 min, and up to t₉₉ ≈ 35 min at 95% RH). This is more than an order of magnitude faster than suggested by many previous studies of aerosol-borne IAV, possibly due to the use of matrices containing organic molecules, such as proteins, with protective effects for the virus. We tested this hypothesis by adding sucrose to our aerosolization medium and, indeed, observed protection of IAV at intermediate RH (55%). Interestingly, the t₉₉ of our measurements are also systematically lower than those in 1-μL droplet measurements of organic-free saline solutions, which cannot be explained by particle size effects alone.
  • Kleinheins, Judith; Shardt, Nadia; El Haber, Manuella; et al. (2023)
    Physical Chemistry Chemical Physics
    The liquid–air surface tension of aqueous solutions is a fundamental quantity in multi-phase thermodynamics and fluid dynamics and thus relevant in many scientific and engineering fields. Various models have been proposed for its quantitative description. This Perspective gives an overview of the most popular models and their ability to reproduce experimental data of ten binary aqueous solutions of electrolytes and organic molecules chosen to be representative of different solute types. In addition{,} we propose a new model which reproduces sigmoidal curve shapes (Sigmoid model) to empirically fit experimental surface tension data. The surface tension of weakly surface-active substances is well reproduced by all models. In contrast{,} only few models successfully model the surface tension of aqueous solutions with strongly surface-active substances. For substances with a solubility limit{,} usually no experimental data is available for the surface tension of supersaturated solutions and the pure liquid solute. We discuss ways in which these can be estimated and emphasize the need for further research. The newly developed Sigmoid model best reproduces the surface tension of all tested solutions and can be recommended as a model for a broad range of binary mixtures and over the entire concentration range.
Publications 1 - 10 of 102