To estimate the global co-variability between mineral dust aerosol and cloud glaciation, we combined an aerosol model reanalysis with satellite retrievals of cloud thermodynamic phase. We used the ...CALIPSO-GOCCP product from the A-Train satellite constellation to assess whether clouds are composed of liquid or ice and the MACC reanalysis to estimate the dust mixing ratio in the atmosphere. Night-time retrievals within a temperature range from +3 to −42 ∘C for the period 2007–2010 were included. The results confirm that the cloud thermodynamic phase is highly dependent on temperature and latitude. However, at middle and high latitudes, at equal temperature and within narrow constraints for humidity and static stability, the average frequency of fully glaciated clouds increases by +5 to +10 % for higher mineral dust mixing ratios. The discrimination between humidity and stability regimes reduced the confounding influence of meteorology on the observed relationship between dust and cloud ice. Furthermore, for days with similar mixing ratios of mineral dust, the cloud ice occurrence frequency in the Northern Hemisphere was found to be higher than in the Southern Hemisphere at −30 ∘C but lower at −15 ∘C. This contrast may suggest a difference in the susceptibility of cloud glaciation to the presence of dust. Based on previous studies, the differences at −15 ∘C could be explained by higher feldspar fractions in the Southern Hemisphere, while the higher freezing efficiency of clay minerals in the Northern Hemisphere may explain the differences at −30 ∘C.
The synoptic and local meteorological conditions during the ground-based cloud passage experiment FEBUKO performed at the Schmücke Mountain (Thüringer Wald) during October 2001 and 2002 are reviewed ...and discussed. A general description of the weather types and a classification of air masses are presented. In the second part the meteorological situations are illustrated in detail for the different experimental cloud events. The main objective of this two-part study is to classify the cloud events with respect to the occurring weather conditions and consistency to the philosophy of cloud passage experiments. Therefore, particular emphasis is placed on the incident flow conditions and on the separation of orographic and non-orographic cloud types. In the case of the flow characterisation, weather charts and calculated backward trajectories are used to determine the horizontal wind pattern and the rawinsonde data for the vertical structure of wind vectors. Additionally, in order to describe the local flow conditions the observed wind speed and direction at the experimental site on the summit are applied for the total of 14 cloud episodes. For the examination of the orographic character and properties of clouds, satellite pictures of different spectral channels, vertical thermodynamic data of the rawinsonde as well as the measured liquid water content and the cloud base height are evaluated. The resulting event evaluation provides a basis for subsequent local analysis of the flow over and/or around the mountain range (Part II of the study). Generally, it is found that more suitable conditions were encountered in October 2001 than in October 2002. Especially for the anticyclonic southwest weather-type, stable incoming flow condition as well as orographically induced clouds could be clearly identified.
Aerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects.
Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, ...has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day.
Current climate models, however, are still struggling to reproduce Arctic aerosol conditions.
We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC.
The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005–2017, with a focus on BC.
Four different setups of air pollution emissions are tested.
The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic.
Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC.
Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30 % higher annual BC burden locally.
This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1 W m−2 at the top of the atmosphere over the Arctic region (60–90∘ N), being locally more than 0.2 W m−2 over the eastern Arctic Ocean.
We estimate BC in the Arctic as leading to an annual net gain of 0.5 W m−2 averaged over the Arctic region but to a local gain of up to 0.8 W m−2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction.
Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer.
This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign.
Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC.
The ability to achieve high spatial resolutions is an important feature for numerical models to accurately represent the large spatial variability of urban air pollution. On the one hand, the ...well-established mesoscale chemistry transport models have their obvious shortcomings due to the extensive use of physical parameterizations. On the other hand, obstacle-resolving computational fluid dynamics (CFD) models, although accurate, are still often too computationally intensive to be applied regularly for entire cities. The major reason for the inflated computational costs is the required horizontal resolution to meaningfully apply obstacle discretization, which is mostly based on boundary-fitted grids, e.g., the marker-and-cell method.
In this paper, we present the new City-scale AIR dispersion model with DIffuse Obstacles (CAIRDIO v1.0), in which the diffuse interface method, simplified for non-moving obstacles, is incorporated into the governing equations for incompressible large-eddy simulations. While the diffuse interface method is widely used in two-phase modeling, this method has not been used in urban boundary-layer modeling so far. It allows us to consistently represent buildings over a wide range of spatial resolutions, including grid spacings equal to or larger than typical building sizes. This way, the gray zone between obstacle-resolving microscale simulations and mesoscale simulations can be addressed. Orographic effects can be included by using terrain-following coordinates. The dynamic core is compared against a standard quality-assured wind-tunnel dataset for dispersion-model evaluation. It is shown that the model successfully reproduces dispersion patterns within a complex city morphology across a wide range of spatial resolutions tested. As a result of the diffuse obstacle approach, the accuracy test is also passed at a horizontal grid spacing of 40 m. Although individual flow features within individual street canyons are not resolved at the coarse-grid spacing, the building effect on the dispersion of the air pollution plume is preserved at a larger scale. Therefore, a very promising application of the CAIRDIO model lies in the realization of computationally feasible yet accurate air-quality simulations for entire cities.
More than 1 Tg smoke aerosol was emitted into the atmosphere by
the exceptional 2019–2020 southeastern Australian wildfires. Triggered by the
extreme fire heat, several deep pyroconvective events ...carried the smoke
directly into the stratosphere. Once there, smoke aerosol remained airborne
considerably longer than in lower atmospheric layers. The thick plumes
traveled eastward, thereby being distributed across the high and mid-latitudes in the
Southern Hemisphere, enhancing the atmospheric opacity. Due to the increased
atmospheric lifetime of the smoke plume, its radiative effect increased
compared to smoke that remains in lower altitudes. Global models describing
aerosol-climate impacts lack adequate descriptions of the emission height of
aerosols from intense wildfires. Here, we demonstrate, by a combination of
aerosol-climate modeling and lidar observations, the importance of the
representation of those high-altitude fire smoke layers for estimating the
atmospheric energy budget. Through observation-based input into the
simulations, the Australian wildfire emissions by pyroconvection are
explicitly prescribed to the lower stratosphere in different scenarios.
Based on our simulations, the 2019–2020 Australian fires caused a
significant top-of-atmosphere (TOA) hemispheric instantaneous direct radiative
forcing signal that reached a magnitude comparable to the radiative forcing
induced by anthropogenic absorbing aerosol. Up to +0.50 W m−2
instantaneous direct radiative forcing was modeled at TOA,
averaged for the Southern Hemisphere (+0.25 W m−2 globally) from January to March 2020 under all-sky conditions. At the surface, on the other
hand, an instantaneous solar radiative forcing of up to −0.81 W m−2
was found for clear-sky conditions, with the respective estimates depending
on the model configuration and subject to the model uncertainties in the
smoke optical properties. Since extreme wildfires are expected to occur more
frequently in the rapidly changing climate, our findings suggest that
high-altitude wildfire plumes must be adequately considered in climate
projections in order to obtain reasonable estimates of atmospheric energy
budget changes.
The magnitude of solar radiative effects (cooling or warming) of black carbon (BC) particles embedded in the Arctic atmosphere and surface snow layer was explored on the basis of case studies. For ...this purpose, combined atmospheric and snow radiative transfer simulations were performed for cloudless and cloudy conditions on the basis of BC mass concentrations measured in pristine early summer and more polluted early spring conditions. The area of interest is the remote sea-ice-covered Arctic Ocean in the vicinity of Spitsbergen, northern Greenland, and northern Alaska typically not affected by local pollution. To account for the radiative interactions between the black-carbon-containing snow surface layer and the atmosphere, an atmospheric and snow radiative transfer model were coupled iteratively.
For pristine summer conditions (no atmospheric BC, minimum solar zenith angles of 55∘) and a representative BC particle mass concentration of 5 ng g−1 in the surface snow layer, a positive daily mean solar radiative forcing of +0.2 W m−2 was calculated for the surface radiative budget. A higher load of atmospheric BC representing early springtime conditions results in a slightly negative mean radiative forcing at the surface of about −0.05 W m−2, even when the low BC mass concentration measured in the pristine early summer conditions was embedded in the surface snow layer. The total net surface radiative forcing combining the effects of BC embedded in the atmosphere and in the snow layer strongly depends on the snow optical properties (snow specific surface area and snow density).
For the conditions over the Arctic Ocean analyzed in the simulations, it was found that the atmospheric heating rate by water vapor or clouds is 1 to 2 orders of magnitude larger than that by atmospheric BC. Similarly, the daily mean total heating rate (6 K d−1) within a snowpack due to absorption by the ice was more than 1 order of magnitude larger than that of atmospheric BC (0.2 K d−1).
Also, it was shown that the cooling by atmospheric BC of the near-surface air and the warming effect by BC embedded in snow are reduced in the presence of clouds.
Atmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four ...different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for present-day aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidar-derived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1.5×109 CCN m−3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height.
Infrared “Desert Dust” composite imagery taken by the Spinning Enhanced Visible and InfraRed Imager (SEVIRI), onboard the Meteosat Second Generation (MSG) series of satellites above the equatorial ...East Atlantic, has been widely used for more than a decade to identify and track the presence of dust storms from and over the Sahara Desert, the Middle East, and southern Africa. Dust is characterised by distinctive pink colours in the Desert Dust false-colour imagery; however, the precise colour is influenced by numerous environmental properties, such as the surface thermal emissivity and skin temperature, the atmospheric water vapour content, the quantity and height of dust in the atmosphere, and the infrared optical properties of the dust itself. For this paper, simulations of SEVIRI infrared measurements and imagery have been performed using a modelling system, which combines dust concentrations simulated by the aerosol transport model COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdelling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model) with radiative transfer simulations from the RTTOV (Radiative Transfer for TOVS) model. Investigating the sensitivity of the synthetic infrared imagery to the environmental properties over a 6-month summertime period from 2011 to 2013, it is confirmed that water vapour is a major control on the apparent colour of dust, obscuring its presence when the moisture content is high. Of the three SEVIRI channels used in the imagery (8.7, 10.8, and 12.0 µm), the channel at 10.8 µm has the highest atmospheric transmittance and is therefore the most sensitive to the surface skin temperature. A direct consequence of this sensitivity is that the background desert surface exhibits a strong diurnal cycle in colour, with light blue colours possible during the day and purple hues prevalent at night. In dusty scenes, the clearest pink colours arise from high-altitude dust in dry atmospheres. Elevated dust influences the dust colour primarily by reducing the contrast in atmospheric transmittance above the dust layer between the SEVIRI channels at 10.8 and 12.0 µm, thereby boosting red and pink colours in the imagery. Hence, the higher the dust altitude, the higher the threshold column moisture needed for dust to be obscured in the imagery: for a sample of dust simulated to have an aerosol optical depth (AOD) at 550 nm of 2–3 at an altitude of 3–4 km, the characteristic colour of the dust may only be impaired when the total column water vapour is particularly moist (⪆39 mm). Meanwhile, dust close to the surface (altitude <1 km) is only likely to be apparent when the atmosphere is particularly dry and when the surface is particularly hot, requiring column moisture ⪅13 mm and skin temperatures ⪆314 K, and is highly unlikely to be apparent when the skin temperature is ⪅300 K. Such low-altitude dust will regularly be almost invisible within the imagery, since it will usually be beneath much of the atmospheric water vapour column. It is clear that the interpretation of satellite-derived dust imagery is greatly aided by knowledge of the background environment.
Satellite imagery of atmospheric mineral dust is sensitive to the optical properties of the dust, governed by the mineral refractive indices, particle size, and particle shape. In infrared channels ...the imagery is also sensitive to the dust layer height and to the surface and atmospheric environment. Simulations of mineral dust in infrared Desert Dust imagery from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) have been performed, using the COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdelling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model) dust transport model and the Radiative Transfer for TOVS (RTTOV) program, in order to investigate the sensitivity of the imagery to assumed dust properties. This paper introduces the technique and performs initial validation and comparisons with SEVIRI measurements over North Africa for daytime hours during 6 months covering June and July of 2011–2013. Using T-matrix scattering theory and assuming the dust particles to be spherical or spheroidal, wavelength- and size-dependent dust extinction values are calculated for a number of different dust refractive index databases, along with several values of the particle aspect ratio, denoting the particle shape. The consequences for the infrared extinction values of both the particle shape and the particle orientation are explored: this analysis shows that as the particle asphericity increases, the extinctions increase if the particles are aligned horizontally, and decrease if they are aligned vertically. Randomly oriented spheroidal particles have very similar infrared extinction properties as spherical particles, whereas the horizontally and vertically aligned particles can be considered to be the upper and lower bounds on the extinction values. Inputting these values into COSMO-MUSCAT-RTTOV, it is found that spherical particles do not appear to be sufficient to describe fully the resultant colour of the dust in the infrared imagery. Comparisons of SEVIRI and simulation colours indicate that of the dust types tested, the dust refractive index dataset produced by Volz (1973) shows the most similarity in the colour response to dust in the SEVIRI imagery, although the simulations have a smaller range of colour than do the observations. It is also found that the thermal imagery is most sensitive to intermediately sized particles (radii between 0.9 and 2.6 µm): larger particles are present in too small a concentration in the simulations, as well as with insufficient contrast in extinction between wavelength channels, to have much ability to perturb the resultant colour in the SEVIRI dust imagery.
An overview of the two FEBUKO aerosol–cloud interaction field experiments in the Thüringer Wald (Germany) in October 2001 and 2002 and the corresponding modelling project MODMEP is given. ...Experimentally, a variety of measurement methods were deployed to probe the gas phase, particles and cloud droplets at three sites upwind, downwind and within an orographic cloud with special emphasis on the budgets and interconversions of organic gas and particle phase constituents. Out of a total of 14 sampling periods within 30 cloud events three events (EI, EII and EIII) are selected for detailed analysis. At various occasions an impact of the cloud process on particle chemical composition such as on the organic compounds content, sulphate and nitrate and also on particle size distributions and particle mass is observed. Moreover, direct phase transfer of polar organic compound from the gas phase is found to be very important for the understanding of cloudwater composition.
For the modelling side, a main result of the MODMEP project is the development of a cloud model, which combines a complex multiphase chemistry with detailed microphysics. Both components are described in a fine-resolved particle/drop spectrum. New numerical methods are developed for an efficient solution of the entire complex model. A further development of the CAPRAM mechanism has lead to a more detailed description of tropospheric aqueous phase organic chemistry. In parallel, effective tools for the reduction of highly complex reaction schemes are provided. Techniques are provided and tested which allow the description of complex multiphase chemistry and of detailed microphysics in multidimensional chemistry-transport models.
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