Atmospheric Chemistry and Physics

Journal: Atmospheric Chemistry and Physics

Abbreviation

Atmos. Chem. Phys.

Publisher

European Geophysical Society

ISSN

1680-7324
1680-7375

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Publications 1 - 10 of 54

In situ measurements of perturbations to stratospheric aerosol and modeled ozone and radiative impacts following the 2021 La Soufrière eruption
Li, Yaowei; Pedersen, Corey; Dykema, John; et al. (2023)
Atmospheric Chemistry and Physics
Stratospheric aerosols play important roles in Earth’s radiative budget and in heterogeneous chemistry. Volcanic eruptions modulate the stratospheric aerosol layer by injecting particles and particle precursors like sulfur dioxide (SO2) into the stratosphere. Beginning on 9 April 2021, La Soufrière erupted, injecting SO2 into the tropical upper troposphere and lower stratosphere, yielding a peak SO2 loading of 0.3–0.4 Tg. The resulting volcanic aerosol plumes dispersed predominately over the Northern Hemisphere (NH), as indicated by the CALIOP/CALIPSO satellite observations and model simulations. From June to August 2021 and May to July 2022, the NASA ER-2 high-altitude aircraft extensively sampled the stratospheric aerosol layer over the continental United States during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) mission. These in situ aerosol measurements provide detailed insights into the number concentration, size distribution, and spatiotemporal variations of particles within volcanic plumes. Notably, aerosol surface area density and number density in 2021 were enhanced by a factor of 2–4 between 380–500 K potential temperature compared to the 2022 DCOTSS observations, which were minimally influenced by volcanic activity. Within the volcanic plume, the observed aerosol number density exhibited significant meridional and zonal variations, while the mode and shape of aerosol size distributions did not vary. The La Soufrière eruption led to an increase in the number concentration of small particles (<400 nm), resulting in a smaller aerosol effective diameter during the summer of 2021 compared to the baseline conditions in the summer of 2022, as observed in regular ER-2 profiles over Salina, Kansas. A similar reduction in aerosol effective diameter was not observed in ER-2 profiles over Palmdale, California, possibly due to the values that were already smaller in that region during the limited sampling period in 2022. Additionally, we modeled the eruption with the SOCOL-AERv2 aerosol–chemistry–climate model. The modeled aerosol enhancement aligned well with DCOTSS observations, although the direct comparison was complicated by issues related to the model’s background aerosol burden. This study indicates that the La Soufrière eruption contributed approximately 0.6 % to Arctic and Antarctic ozone column depletion in both 2021 and 2022, which is well within the range of natural variability. The modeled top-of-atmosphere 1-year global average radiative forcing was −0.08 W m−2 clear-sky and −0.04 W m−2 all-sky. The radiative effects were concentrated in the tropics and NH midlatitudes and diminished to near-baseline levels after 1 year.
The vapor pressures and activities of dicarboxylic acids reconsidered: the impact of the physical state of the aerosol
Soonsin, Vacharaporn; Zardini, Alessandro A.; Marcolli, Claudia; et al. (2010)
Atmospheric Chemistry and Physics
We present vapor pressure data of the C2 to C5 dicarboxylic acids deduced from measured evaporation rates of single levitated particles as both, aqueous droplets and solid crystals. The data of aqueous solution particles over a wide concentration range allow us to directly calculate activities of the dicarboxylic acids and comparison of these activities with parameterizations reported in the literature. The data of the pure liquid state acids, i.e. the dicarboxylic acids in their supercooled melt state, exhibit no even-odd alternation in vapor pressure, while the acids in the solid form do. This observation is consistent with the known solubilities of the acids and our measured vapor pressures of the supercooled melt. Thus, the gas/particle partitioning of the different dicarboxylic acids in the atmosphere depends strongly on the physical state of the aerosol phase, the difference being largest for the even acids. Our results show also that, in general, measurements of vapor pressures of solid dicarboxylic acids may be compromised by the presence of polymorphic forms, crystalline structures with a high defect number, and/or solvent inclusions in the solid material, yielding a higher vapor pressure than the one of the thermodynamically stable crystalline form at the same temperature.
Introduction of prognostic rain in ECHAM5: design and single column model simulations
Posselt, Rebekka; Lohmann, Ulrike (2008)
Atmospheric Chemistry and Physics
Prognostic equations for the rain mass mixing ratio and the rain drop number concentration are introduced into the large-scale cloud microphysics parameterization of the ECHAM5 general circulation model (ECHAM5-PROG). To this end, a rain flux from one level to the next with the appropriate fall speed is introduced. This maintains rain water in the atmosphere to be available for the next time step. Rain formation in ECHAM5-PROG is, therefore, less dependent on the autoconversion rate than the standard ECHAM5 but shifts the emphasis towards the accretion rates in accordance with observations. ECHAM5-PROG is tested and evaluated with Single Column Model (SCM) simulations for two cases: the marine stratocumulus study EPIC (October 2001) and the continental mid-latitude ARM Cloud IOP (shallow frontal cloud case – March 2000). In case of heavy precipitation events, the prognostic equations for rain hardly affect the amount and timing of precipitation at the surface in different SCM simulations because heavy rain depends mainly on the large-scale forcing. In case of thin, drizzling clouds (i.e., stratocumulus), surface precipitation is sensitive to the number of sub-time steps used in the prognostic rain scheme. Cloud microphysical quantities, such as cloud liquid and rain water within the atmosphere, are sensitive to the number of sub-time steps in both considered cases. This results from the decreasing autoconversion rate and increasing accretion rate.
The representation of solar cycle signals in stratospheric ozone - Part 2: Analysis of global models
Maycock, Amanda C.; Matthes, Katja; Tegtmeier, Susann; et al. (2018)
Atmospheric Chemistry and Physics
The impact of changes in incoming solar irradiance on stratospheric ozone abundances should be included in climate simulations to aid in capturing the atmospheric response to solar cycle variability. This study presents the first systematic comparison of the representation of the 11-year solar cycle ozone response (SOR) in chemistry–climate models (CCMs) and in pre-calculated ozone databases specified in climate models that do not include chemistry, with a special focus on comparing the recommended protocols for the Coupled Model Intercomparison Project Phase 5 and Phase 6 (CMIP5 and CMIP6). We analyse the SOR in eight CCMs from the Chemistry–Climate Model Initiative (CCMI-1) and compare these with results from three ozone databases for climate models: the Bodeker Scientific ozone database, the SPARC/Atmospheric Chemistry and Climate (AC&C) ozone database for CMIP5 and the SPARC/CCMI ozone database for CMIP6. The peak amplitude of the annual mean SOR in the tropical upper stratosphere (1–5hPa) decreases by more than a factor of 2, from around 5 to 2%, between the CMIP5 and CMIP6 ozone databases. This substantial decrease can be traced to the CMIP5 ozone database being constructed from a regression model fit to satellite and ozonesonde measurements, while the CMIP6 database is constructed from CCM simulations. The SOR in the CMIP6 ozone database therefore implicitly resembles the SOR in the CCMI-1 models. The structure in latitude of the SOR in the CMIP6 ozone database and CCMI-1 models is considerably smoother than in the CMIP5 database, which shows unrealistic sharp gradients in the SOR across the middle latitudes owing to the paucity of long-term ozone measurements in polar regions. The SORs in the CMIP6 ozone database and the CCMI-1 models show a seasonal dependence with enhanced meridional gradients at mid- to high latitudes in the winter hemisphere. The CMIP5 ozone database does not account for seasonal variations in the SOR, which is unrealistic. Sensitivity experiments with a global atmospheric model without chemistry (ECHAM6.3) are performed to assess the atmospheric impacts of changes in the representation of the SOR and solar spectral irradiance (SSI) forcing between CMIP5 and CMIP6. The larger amplitude of the SOR in the CMIP5 ozone database compared to CMIP6 causes a likely overestimation of the modelled tropical stratospheric temperature response between 11-year solar cycle minimum and maximum by up to 0.55K, or around 80% of the total amplitude. This effect is substantially larger than the change in temperature response due to differences in SSI forcing between CMIP5 and CMIP6. The results emphasize the importance of adequately representing the SOR in global models to capture the impact of the 11-year solar cycle on the atmosphere. Since a number of limitations in the representation of the SOR in the CMIP5 ozone database have been identified, we recommend that CMIP6 models without chemistry use the CMIP6 ozone database and the CMIP6 SSI dataset to better capture the climate impacts of solar variability. The SOR coefficients from the CMIP6 ozone database are published with this paper.
The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds
Wiacek, Aldona; Peter, Thomas; Lohmann, Ulrike (2010)
Atmospheric Chemistry and Physics
This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons, without explicitly modelling dust emission and deposition processes. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high ice clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Downstream of the investigated dust sources, practically none of the simulated air parcels reached conditions of homogeneous ice nucleation (T≲−40 °C) along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through atmospheric regions supersaturated with respect to ice but subsaturated with respect to water, where so-called "warm ice clouds" (T≳−40 °C) theoretically may form prior to supercooled water or mixed-phase clouds. The importance of "warm ice clouds" and the general influence of dust in the mixed-phase cloud region are highly uncertain due to both a considerable scatter in recent laboratory data from ice nucleation experiments, which we briefly review in this work, and due to uncertainties in sub-grid scale vertical transport processes unresolved by the present trajectory analysis. For "classical" cirrus-forming temperatures (T≲−40 °C), our results show that only mineral dust ice nuclei that underwent mixed-phase cloud-processing, most likely acquiring coatings of organic or inorganic material, are likely to be relevant. While the potential paucity of deposition ice nuclei shown in this work dimishes the possibility of deposition nucleation, the absence of liquid water droplets at T≲−40 °C makes the less explored contact freezing mechanism (involving droplet collisions with bare ice nuclei) highly inefficient. These factors together indicate the necessity of further systematic studies of immersion mode ice nucleation on mineral dust suspended in atmospherically relevant coatings.
Trends and variability of midlatitude stratospheric water vapour deduced from the re-evaluated Boulder balloon series and HALOE
Scherer, M.; Vömel, Holger; Fueglistaler, Stephan; et al. (2008)
Atmospheric Chemistry and Physics
This paper presents an updated trend analysis of water vapour in the lower midlatitude stratosphere from the Boulder balloon-borne NOAA frostpoint hygrometer measurements and from the Halogen Occulation Experiment (HALOE). Two corrections for instrumental bias are applied to homogenise the frostpoint data series, and a quality assessment of all soundings after 1991 is presented. Linear trend estimates based on the corrected data for the period 1980–2000 are up to 40% lower than previously reported. Vertically resolved trends and variability are calculated with a multi regression analysis including the quasi-biennal oscillation and equivalent latitude as explanatory variables. In the range of 380 to 640 K potential temperature (≈14 to 25 km), the frostpoint data from 1981 to 2006 show positive linear trends between 0.3±0.3 and 0.7±0.1%/yr. The same dataset shows trends between −0.2±0.3 and 1.0±0.3%/yr for the period 1992 to 2005. HALOE data over the same time period suggest negative trends ranging from −1.1±0.2 to −0.1±0.1%/yr. In the lower stratosphere, a rapid drop of water vapour is observed in 2000/2001 with little change since. At higher altitudes, the transition is more gradual, with slowly decreasing concentrations between 2001 and 2007. This pattern is consistent with a change induced by a drop of water concentrations at entry into the stratosphere. Previously noted differences in trends and variability between frostpoint and HALOE remain for the homogenised data. Due to uncertainties in reanalysis temperatures and stratospheric transport combined with uncertainties in observations, no quantitative inference about changes of water entering the stratosphere in the tropics could be made with the mid latitude measurements analysed here.
Solar "brightening" impact on summer surface ozone between 1990 and 2010 in Europe - A model sensitivity study of the influence of the aerosol-radiation interactions
Oikonomakis, Emmanouil; Aksoyoglu, Sebnem; Wild, Martin; et al. (2018)
Atmospheric Chemistry and Physics
Surface solar radiation (SSR) observations have indicated an increasing trend in Europe since the mid-1980s, referred to as solar "brightening". In this study, we used the regional air quality model, CAMx (Comprehensive Air Quality Model with Extensions) to simulate and quantify, with various sensitivity runs (where the year 2010 served as the base case), the effects of increased radiation between 1990 and 2010 on photolysis rates (with the PHOT1, PHOT2 and PHOT3 scenarios, which represented the radiation in 1990) and biogenic volatile organic compound (BVOC) emissions (with the BIO scenario, which represented the biogenic emissions in 1990), and their consequent impacts on summer surface ozone concentrations over Europe between 1990 and 2010. The PHOT1 and PHOT2 scenarios examined the effect of doubling and tripling the anthropogenic PM2.5 concentrations, respectively, while the PHOT3 investigated the impact of an increase in just the sulfate concentrations by a factor of 3.4 (as in 1990), applied only to the calculation of photolysis rates. In the BIO scenario, we reduced the 2010 SSR by 3% (keeping plant cover and temperature the same), recalculated the biogenic emissions and repeated the base case simulations with the new biogenic emissions. The impact on photolysis rates for all three scenarios was an increase (in 2010 compared to 1990) of 3–6% which resulted in daytime (10:00–18:00 Local Mean Time – LMT) mean surface ozone differences of 0.2–0.7ppb (0.5–1.5%), with the largest hourly difference rising as high as 4–8ppb (10–16%). The effect of changes in BVOC emissions on daytime mean surface ozone was much smaller (up to 0.08ppb, ∼ 0.2%), as isoprene and terpene (monoterpene and sesquiterpene) emissions increased only by 2.5–3 and 0.7%, respectively. Overall, the impact of the SSR changes on surface ozone was greater via the effects on photolysis rates compared to the effects on BVOC emissions, and the sensitivity test of their combined impact (the combination of PHOT3 and BIO is denoted as the COMBO scenario) showed nearly additive effects. In addition, all the sensitivity runs were repeated on a second base case with increased NOx emissions to account for any potential underestimation of modeled ozone production; the results did not change significantly in magnitude, but the spatial coverage of the effects was profoundly extended. Finally, the role of the aerosol–radiation interaction (ARI) changes in the European summer surface ozone trends was suggested to be more important when comparing to the order of magnitude of the ozone trends instead of the total ozone concentrations, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
The importance of mixed-phase and ice clouds for climate sensitivity in the global aerosol-climate model ECHAM6-HAM2
Lohmann, Ulrike; Neubauer, David (2018)
Atmospheric Chemistry and Physics
How clouds change in a warmer climate remains one of the largest uncertainties for the equilibrium climate sensitivity (ECS). While a large spread in the cloud feedback arises from low-level clouds, it was recently shown that mixed-phase clouds are also important for ECS. If mixed-phase clouds in the current climate contain too few supercooled cloud droplets, too much ice will change to liquid water in a warmer climate. As shown by Tan et al. (2016), this overestimates the negative cloud-phase feedback and underestimates ECS in the CAM global climate model (GCM). Here we use the newest version of the ECHAM6-HAM2 GCM to investigate the importance of mixed-phase and ice clouds for ECS. Although we also considerably underestimate the fraction of supercooled liquid water globally in the reference version of the ECHAM6-HAM2 GCM, we do not obtain increases in ECS in simulations with more supercooled liquid water in the present-day climate, different from the findings by Tan et al. (2016). We hypothesize that it is not the global supercooled liquid water fraction that matters, but only how well low- and mid-level mixed-phase clouds with cloud-top temperatures in the mixed-phase temperature range between 0 and −35°C that are not shielded by higher-lying ice clouds are simulated. These occur most frequently in midlatitudes, in particular over the Southern Ocean where they determine the amount of absorbed shortwave radiation. In ECHAM6-HAM2 the amount of absorbed shortwave radiation over the Southern Ocean is only significantly overestimated if all clouds below 0°C consist exclusively of ice. Only in this simulation is ECS significantly smaller than in all other simulations and the cloud optical depth feedback is the dominant cloud feedback. In all other simulations, the cloud optical depth feedback is weak and changes in cloud feedbacks associated with cloud amount and cloud-top pressure dominate the overall cloud feedback. However, apart from the simulation with only ice below 0°C, differences in the overall cloud feedback are not translated into differences in ECS in our model. This insensitivity to the cloud feedback in our model is explained with compensating effects in the clear sky.
Modelling of cirrus clouds – Part 2: Competition of different nucleation mechanisms
Spichtinger, Peter; Gierens, K.M. (2009)
Atmospheric Chemistry and Physics
Measurements of UV irradiance within the area of one satellite pixel
Weihs, Philipp; Blumthaler, Mario; Rieder, Harald E.; et al. (2008)
Atmospheric Chemistry and Physics
A measurement campaign was performed in the region of Vienna and its surroundings from May to July 2007. Within the scope of this campaign erythemal UV was measured at six ground stations within a radius of 30 km. First, the homogeneity of the UV levels within the area of one satellite pixel was studied. Second, the ground UV was compared to ground UV retrieved by the ozone monitoring instrument (OMI) onboard the NASA EOS Aura Spacecraft. During clear-sky conditions the mean bias between erythemal UV measured by the different stations was within the measurement uncertainty of ±5%. Short term fluctuations of UV between the stations were below 3% within a radius of 20 km. For partly cloudy conditions and overcast conditions the discrepancy of instantaneous values between the stations is up to 200% or even higher. If averages of the UV index over longer time periods are compared the difference between the stations decreases strongly. The agreement is better than 20% within a distance of 10 km between the stations for 3 h averages. The comparison with OMI UV showed for clear-sky conditions higher satellite retrieved UV values by, on the average, approximately 15%. The ratio of OMI to ground measured UV lies between 0.9 and 1.5. and strongly depends on the aerosol optical depth. For partly cloudy and overcast conditions the OMI derived surface UV estimates show larger deviation from the ground-based reference data, and even bigger systematic positive bias. Here the ratio OMI to ground data lies between 0.5 and 4.5. The average difference between OMI and ground measurements is +24 to +37% for partly cloudy conditions and more than +50% for overcast conditions.

Publications 1 - 10 of 54

Journal: Atmospheric Chemistry and Physics

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