Atmospheric Chemistry and Physics

Journal: Atmospheric Chemistry and Physics

Abbreviation

Atmos. Chem. Phys.

Publisher

Copernicus

ISSN

1680-7324
1680-7375

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Publications 1 - 10 of 614

Water isotopic characterisation of the cloud-circulation coupling in the North Atlantic trades - Part 2: The imprint of the atmospheric circulation at different scales
Villiger, Leonie; Aemisegger, Franziska (2024)
Atmospheric Chemistry and Physics
Water vapour isotopes reflect the history of moist atmospheric processes encountered by the vapour since evaporating from the ocean, offering potential insights into the controls of shallow trade-wind cumuli. Given that these clouds, particularly their amount at the cloud base level, play an important role in the global radiative budget, improving our understanding of the hydrological cycle associated with them is crucial. This study examines the variability of water vapour isotopes at cloud base in the winter trades near Barbados and explores its connection to the atmospheric circulations ultimately governing cloud fraction. The analyses are based on nested COSMOiso simulations with explicit convection during the EUREC4A (Elucidating the role of clouds-circulation coupling in climate) field campaign. It is shown that the contrasting isotope and humidity characteristics in clear-sky versus cloudy environments at cloud base emerge due to vertical transport on timescales of 4 to 14h associated with local, convective circulations. In addition, the cloud base isotopes are sensitive to variations in the large-scale circulation on timescales of 4 to 6d, which shows on average a Hadley-type subsidence but occasionally much stronger descent related to extratropical dry intrusions. This investigation, based on high-resolution isotope-enabled simulations in combination with trajectory analyses, reveals how dynamical processes at different timescales act in concert to produce the observed humidity variations at the base of trade-wind cumuli.
Unveiling atmospheric transport and mixing mechanisms of ice-nucleating particles over the Alps
Wieder, Jörg; Mignani, Claudia; Schär, Mario; et al. (2022)
Atmospheric Chemistry and Physics
Precipitation over the mid-latitudes originates mostly from the ice phase within mixed-phase clouds, signifying the importance of initial ice crystal formation. Primary ice crystals are formed on ice-nucleating particles (INPs), which measurements suggest are sparsely populated in the troposphere. INPs are emitted by a large number of ground-based sources into the atmosphere, from where they can be lifted up to cloud heights. Therefore, it is vital to understand vertical INP transport mechanisms, which are particularly complex over orographic terrain. We investigate the vertical transport and mixing mechanisms of INPs over orographic terrain during cloudy conditions by simultaneous measurements of in situ INP concentration at a high valley and a mountaintop site in the Swiss Alps in late winter 2019. On the mountaintop, the INP concentrations were, on average, lower than in the high valley. However, a diurnal cycle in INP concentrations was observed at the mountaintop, which was absent in the high valley. The median mountaintop INP concentration equilibrated to the concentration found in the high valley towards the night. We found that, in nearly 70g% of the observed cases, INP-rich air masses were orographically lifted from low elevation upstream of the measurement site. In addition, we present evidence that, over the course of the day, air masses containing high INP concentrations were advected from the Swiss plateau towards the measurement sites, contributing to the diurnal cycle of INPs. Our results suggest a local INP concentration enhancement over the Alps during cloud events.
Online measurements of water-soluble organic acids in the gas and aerosol phase from the photooxidation of 1,3,5-trimethylbenzene
Praplan, Arnaud P.; Hegyi-Gaeggeler, K.; Barmet, P.; et al. (2014)
Atmospheric Chemistry and Physics
The formation of organic acids during photooxidation of 1,3,5-trimethylbenzene (TMB) in the presence of NOx was investigated with an online ion chromatography (IC) instrument coupled to a mass spectrometer (MS) at the Paul Scherrer Institute's smog chamber. Gas and aerosol phase were both sampled. Molecular formulas were attributed to 12 compounds with the help of high-resolution MS data from filter extracts (two compounds in the gas phase only, two in the aerosol phase only and eight in both). Seven of those species could be identified: formic acid, acetic acid, glycolic acid, butanoic acid, pyruvic acid, lactic acid and methylmaleic acid. While the organic acid fraction present in the aerosol phase does not strongly depend on the precursor concentration (6 to 20%), the presence of SO2 reduces this amount to less than 3% for both high and low precursor concentration scenarios. A large amount of acetic acid was injected during one experiment after aerosol formation, but no increase of acetic acid particle concentration could be observed. This indicates that the unexpected presence of volatile organic acids in the particle phase might not be due to partitioning effects, but to reactive uptake or to sampling artefact.
Stratospherically induced circulation changes under the extreme conditions of the no-Montreal-Protocol scenario
Zilker, Franziska; Sukhodolov, Timofei; Chiodo, Gabriel; et al. (2023)
Atmospheric Chemistry and Physics
The Montreal Protocol and its amendments (MPA) have been a huge success in preserving the stratospheric ozone layer from being destroyed by unabated chlorofluorocarbon (CFC) emissions. The phaseout of CFCs has not only prevented serious impacts on our health and climate, but also avoided strong alterations of atmospheric circulation patterns. With the Earth system model SOCOLv4, we study the dynamical and climatic impacts of a scenario with unabated CFC emissions by 2100, disentangling radiative and chemical (ozone-mediated) effects of CFCs. In the stratosphere, chemical effects of CFCs (i.e., the resulting ozone loss) are the main drivers of circulation changes, weakening wintertime polar vortices and speeding up the Brewer–Dobson circulation. These dynamical impacts during wintertime are due to low-latitude ozone depletion and the resulting reduction in the Equator-to-pole temperature gradient. Westerly winds in the lower stratosphere strengthen, which is for the Southern Hemisphere (SH) similar to the effects of the Antarctic ozone hole over the second half of the 20th century. Furthermore, the winter and spring stratospheric wind variability increases in the SH, whereas it decreases in summer and fall. This seasonal variation in wind speed in the stratosphere has substantial implications for the major modes of variability in the tropospheric circulation in the scenario without the MPA (No-MPA). We find coherent changes in the troposphere, such as patterns that are reminiscent of negative Southern and Northern Annular modes (SAM and NAM) and North Atlantic Oscillation (NAO) anomalies during seasons with a weakened vortex (winter and spring); the opposite occurs during seasons with strengthened westerlies in the lower stratosphere and troposphere (summer). In the troposphere, radiative heating by CFCs prevails throughout the year, shifting the SAM into a positive phase and canceling out the ozone-induced effects on the NAO, whereas the North Pacific sector shows an increase in the meridional sea-level pressure gradient as both CFC heating and ozone-induced effects reinforce each other there. Furthermore, global warming is amplified by 1.7 K with regionally up to a 12 K increase over eastern Canada and the western Arctic. Our study sheds light on the adverse effects of a non-adherence to the MPA on the global atmospheric circulation, uncovering the roles of the underlying physical mechanisms. In so doing, our study emphasizes the importance of the MPA for Earth's climate to avoid regional amplifications of negative climate impacts.
A perturbed parameter model ensemble to investigate Mt. Pinatubo's 1991 initial sulfur mass emission
Sheng, Jian-Xiong; Weisenstein, Debra K.; Luo, Beiping P.; et al. (2015)
Atmospheric Chemistry and Physics
We have performed more than 300 atmospheric simulations of the 1991 Pinatubo eruption using the AER 2-D sulfate aerosol model to optimize the initial sulfur mass injection as a function of altitude, which in previous modeling studies has often been chosen in an ad hoc manner (e.g., by applying a rectangular-shaped emission profile). Our simulations are generated by varying a four-parameter vertical mass distribution, which is determined by a total injection mass and a skew-normal distribution function. Our results suggest that (a) the initial mass loading of the Pinatubo eruption is approximately 14 Mt of SO2; (b) the injection vertical distribution is strongly skewed towards the lower stratosphere, leading to a peak mass sulfur injection at 18–21 km; (c) the injection magnitude and height affect early southward transport of the volcanic clouds as observed by SAGE II.
The 1986–1989 ENSO cycle in a chemical climate model
Brönnimann, Stefan; Schraner, Martin; Müller, B.; et al. (2006)
Atmospheric Chemistry and Physics
A pronounced ENSO cycle occurred from 1986 to 1989, accompanied by distinct dynamical and chemical anomalies in the global troposphere and stratosphere. Reproducing these effects with current climate models not only provides a model test but also contributes to our still limited understanding of ENSO's effect on stratosphere-troposphere coupling. We performed several sets of ensemble simulations with a chemical climate model (SOCOL) forced with global sea surface temperatures. Results were compared with observations and with large-ensemble simulations performed with an atmospheric general circulation model (MRF9). We focus our analysis on the extratropical stratosphere and its coupling with the troposphere. In this context, the circulation over the North Atlantic sector is particularly important. Relative to the La Niña winter 1989, observations for the El Niño winter 1987 show a negative North Atlantic Oscillation index with corresponding changes in temperature and precipitation patterns, a weak polar vortex, a warm Arctic middle stratosphere, negative and positive total ozone anomalies in the tropics and at middle to high latitudes, respectively, as well as anomalous upward and poleward Eliassen-Palm (EP) flux in the midlatitude lower stratosphere. Most of the tropospheric features are well reproduced in the ensemble means in both models, though the amplitudes are underestimated. In the stratosphere, the SOCOL simulations compare well with observations with respect to zonal wind, temperature, EP flux, meridional mass streamfunction, and ozone, but magnitudes are underestimated in the middle stratosphere. With respect to the mechanisms relating ENSO to stratospheric circulation, the results suggest that both, upward and poleward components of anomalous EP flux are important for obtaining the stratospheric signal and that an increase in strength of the Brewer-Dobson circulation is part of that signal.
The impact of cirrus clouds on tropical troposphere-to-stratosphere transport
Corti, Thierry; Luo, Beiping P.; Fu, Q.; et al. (2006)
Atmospheric Chemistry and Physics
Although it is well known that air enters the stratosphere preferentially through upwelling in the tropics, the exact mechanisms of troposphere-to-stratosphere transport (TST) are still unknown. Previously proposed mechanisms have been found either to be too slow (e.g., clear sky upwelling) to provide agreement with in situ tracer measurements, or to be insufficient in mass flux to act as a major supply for the Brewer-Dobson circulation (e.g., convective overshooting). In this study we evaluate whether the lofting of air via cirrus cloud-radiation interaction might offer an alternative path for TST, which is responsible for a significant fraction of the observed air mass transport. We find that a combination of deep convection and subsequent upwelling associated with cirrus clouds and clear sky can explain the supply of air for the Brewer-Dobson circulation. Thus, upwelling associated with cirrus clouds offers a mechanism for the missing second stage, which links the first stage of TST, deep convection, to the third stage, the Brewer-Dobson circulation.
Critical assessment of the current state of scientific knowledge, terminology, and research needs concerning the role of organic aerosols in the atmosphere, climate, and global change
Fuzzi, Sandro; Andreae, Meinrat O.; Huebert, Barry J.; et al. (2006)
Atmospheric Chemistry and Physics
In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines.
Intercomparing different devices for the investigation of ice nucleating particles using Snomax (R) as test substance
Wex, Heike; Augustin-Bauditz, Stefanie; Boose, Yvonne; et al. (2015)
Atmospheric Chemistry and Physics
Seven different instruments and measurement methods were used to examine the immersion freezing of bacterial ice nuclei from Snomax® (hereafter Snomax), a product containing ice-active protein complexes from non-viable Pseudomonas syringae bacteria. The experimental conditions were kept as similar as possible for the different measurements. Of the participating instruments, some examined droplets which had been made from suspensions directly, and the others examined droplets activated on previously generated Snomax particles, with particle diameters of mostly a few hundred nanometers and up to a few micrometers in some cases. Data were obtained in the temperature range from −2 to −38 °C, and it was found that all ice-active protein complexes were already activated above −12 °C. Droplets with different Snomax mass concentrations covering 10 orders of magnitude were examined. Some instruments had very short ice nucleation times down to below 1 s, while others had comparably slow cooling rates around 1 K min−1. Displaying data from the different instruments in terms of numbers of ice-active protein complexes per dry mass of Snomax, nm, showed that within their uncertainty, the data agree well with each other as well as to previously reported literature results. Two parameterizations were taken from literature for a direct comparison to our results, and these were a time-dependent approach based on a contact angle distribution (Niedermeier et al., 2014) and a modification of the parameterization presented in Hartmann et al. (2013) representing a time-independent approach. The agreement between these and the measured data were good; i.e., they agreed within a temperature range of 0.6 K or equivalently a range in nm of a factor of 2. From the results presented herein, we propose that Snomax, at least when carefully shared and prepared, is a suitable material to test and compare different instruments for their accuracy of measuring immersion freezing.
A global climatology of stratosphere-troposphere exchange using the ERA-Interim data set from 1979 to 2011
Škerlak, Bojan; Sprenger, Michael; Wernli, Heini (2014)
Atmospheric Chemistry and Physics
In this study we use the ERA-Interim reanalysis data set from the European Centre for Medium-Range Weather Forecasts (ECMWF) and a refined version of a previously developed Lagrangian methodology to compile a global 33 yr climatology of stratosphere–troposphere exchange (STE) from 1979 to 2011. Fluxes of mass and ozone are calculated across the tropopause, pressure surfaces in the troposphere, and the top of the planetary boundary layer (PBL). This climatology provides a state-of-the-art quantification of the geographical distribution of STE and the preferred transport pathways, as well as insight into the temporal evolution of STE during the last 33 yr. We confirm the distinct zonal and seasonal asymmetry found in previous studies using comparable methods. The subset of "deep STE", where stratospheric air reaches the PBL within 4 days or vice versa, shows especially strong geographical and seasonal variations. The global hotspots for deep STE are found along the west coast of North America and over the Tibetan Plateau, especially in boreal winter and spring. An analysis of the time series reveals significant positive trends of the net downward mass flux and of deep STE in both directions, which are particularly large over North America. The downward ozone flux across the tropopause is dominated by the seasonal cycle of ozone concentrations at the tropopause and peaks in summer, when the mass flux is nearly at its minimum. For the subset of deep STE events, the situation is reversed and the downward ozone flux into the PBL is dominated by the mass flux and peaks in early spring. Thus surface ozone concentration along the west coast of North America and around the Tibetan Plateau are likely to be influenced by deep stratospheric intrusions. We discuss the sensitivity of our results on the choice of the control surface representing the tropopause, the horizontal and vertical resolution of the trajectory starting grid, and the minimum residence time τ used to filter out transient STE trajectories.

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