Aerosol size-dependent below-cloud scavenging by rain and snow in the ECHAM5-HAM

Wet deposition processes are highly efficient in the removal of aerosols from the atmosphere, and thus strongly influence global aerosol concentrations, and clouds, and their respective radiative forcings. In this study, physically detailed size-dependent below-cloud scavenging parameterizations for rain and snow are implemented in the ECHAM5-HAM global aerosol-climate model. Previously, below-cloud scavenging by rain in the ECHAM5-HAM was simply a function of the aerosol mode, and then scaled by the rainfall rate. The below-cloud scavenging by snow was a function of the snowfall rate alone. The global mean aerosol optical depth, and sea salt burden are sensitive to the below-cloud scavenging coefficients, with reductions near to 15% when the more vigorous size-dependent below-cloud scavenging by rain and snow is implemented. The inclusion of a prognostic rain scheme significantly reduces the fractional importance of below-cloud scavenging since there is higher evaporation in the lower troposphere, increasing the global mean sea salt burden by almost 15%. Thermophoretic effects are shown to produce increases in the global and annual mean number removal of Aitken size particles of near to 10%, but very small increases (near 1%) in the global mean below-cloud mass scavenging of carbonaceous and sulfate aerosols. Changes in the assumptions about the below-cloud scavenging by rain of particles with radius smaller than 10 nm do not cause any significant changes to the global and annual mean aerosol mass or number burdens, despite a change in the below-cloud number removal rate for nucleation mode particles by near to five-fold. Annual and zonal mean nucleation mode number concentrations are enhanced by up to 30% in the lower troposphere with the more vigourous size-dependent below-cloud scavenging. Closer agreement with different observations is found when the more physically detailed below-cloud scavenging parameterization is employed in the ECHAM5-HAM model

Cell Model of In-cloud Scavenging of Highly Soluble Gases

We investigate mass transfer during absorption of highly soluble gases such as HNO_{3}, H_{2}O_{2} by stagnant cloud droplets in the presence of inert admixtures. Thermophysical properties of the gases and liquids are assumed to be constant. Diffusion interactions between droplets, caused by the overlap of depleted of soluble gas regions around the neighboring droplets, are taken into account in the approximation of a cellular model of a gas-droplet suspension whereby a suspension is viewed as a periodic structure consisting of the identical spherical cells with periodic boundary conditions at the cell boundary. Using this model we determined temporal and spatial dependencies of the concentration of the soluble trace gas in a gaseous phase and in a droplet and calculated the dependence of the scavenging coefficient on time. It is shown that scavenging of highly soluble gases by cloud droplets leads to essential decrease of soluble trace gas concentration in the interstitial air. We found that scavenging coefficient for gas absorption by cloud droplets remains constant and sharply decreases only at the final stage of absorption. In the calculations we employed gamma size distribution of cloud droplets. It was shown that despite of the comparable values of Henry's law constants for the hydrogen peroxide (H2O2) and the nitric acid (HNO3), the nitric acid is scavenged more effectively by cloud than the hydrogen peroxide due to a major affect of the dissociation reaction on HNO3 scavenging.Comment: 28 pages, including 11 Figures, 1 Tabl

Sources of uncertainties in modelling black carbon at the global scale

Our understanding of the global black carbon (BC) cycle is essentially qualitative due to uncertainties in our knowledge of its properties. This work investigates two source of uncertainties in modelling black carbon: those due to the use of different schemes for BC ageing and its removal rate in the global Transport-Chemistry model TM5 and those due to the uncertainties in the definition and quantification of the observations, which propagate through to both the emission inventories, and the measurements used for the model evaluation. The schemes for the atmospheric processing of black carbon that have been tested with the model are (i) a simple approach considering BC as bulk aerosol and a simple treatment of the removal with fixed 70% of in-cloud black carbon concentrations scavenged by clouds and removed when rain is present and (ii) a more complete description of microphysical ageing within an aerosol dynamics model, where removal is coupled to the microphysical properties of the aerosol, which results in a global average of 40% in-cloud black carbon that is scavenged in clouds and subsequently removed by rain, thus resulting in a longer atmospheric lifetime. This difference is reflected in comparisons between both sets of modelled results and the measurements. Close to the sources, both anthropogenic and vegetation fire source regions, the model results do not differ significantly, indicating that the emissions are the prevailing mechanism determining the concentrations and the choice of the aerosol scheme does not influence the levels. In more remote areas such as oceanic and polar regions the differences can be orders of magnitude, due to the differences between the two schemes. The more complete description reproduces the seasonal trend of the black carbon observations in those areas, although not always the magnitude of the signal, while the more simplified approach underestimates black carbon concentrations by orders of magnitude. The sensitivity to wet scavenging has been tested by varying in-cloud and below-cloud removal. BC lifetime increases by 10% when large scale and convective scale precipitation removal efficiency are reduced by 30%, while the variation is very small when below-cloud scavenging is zero. Since the emission inventories are representative of elemental carbon-like substance, the model output should be compared to elemental carbon measurements and if known, the ratio of black carbon to elemental carbon mass should be taken into account when the model is compared with black carbon observation

Large Variation of Mercury Isotope Composition During a Single Precipitation Event at Lhasa City, Tibetan Plateau, China

AbstractThis study examined for the first time the Hg isotope composition in rain samples from a single precipitation event at Lhasa City (China) on the Tibetan Plateau, the “world's third pole”. Large variations of both mass-dependent fractionation (MDF, δ202Hg from -0.80‰ to -0.42‰) and mass-independent fractionation (MIF, Δ199Hg from 0.38‰ to 0.76‰) were observed, with the latter increasing with time. Our results demonstrated that the large variation of Hg isotope ratios likely resulted from mixing of locally emitted Hg and long-term transported Hg, which were characterized by different Hg isotope signatures and mainly leached by below-cloud scavenging and in-cloud scavenging processes, respectively. Our findings demonstrated that Hg isotopes are a powerful tool for investigating the dynamics of precipitation events and emphasized the importance of systematic monitoring studies of the chemical and isotope variability of Hg and other elements during rainfall events

Scavenging of aerosol particles by rain in a cloud resolving model

International audienceWe describe a below-cloud scavenging module of aerosol particles by raindrops for use in a three-dimensional mesoscale cloud resolving model. The rate of particle removal is computed by integrating the scavenging efficiency over the aerosol particle and the drop size distributions. Here the numerical integration is performed accurately with a Gauss quadrature algorithm. The efficiency of the scavenging module is partially confirmed with experimental data. More interestingly, it is illustrated by two numerical experiments: the simulation of a forced convective circulation in a tropical cloudy boundary layer and a two-dimensional simulation of an African squall line. The results show a very selective wet removal of the aerosol particles which clearly depends on the mode radius, the width and the vertical profile of concentration. Furthermore, the squall line case shows the importance of resolving internal circulations to redistribute layers of aerosol particles in order to improve estimates of particle removal by below-cloud scavenging

Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90%) scavenged by cloud nucleation processes for all aerosol species, except for dust (50%). The aerosol number scavenged is primarily (>90%) attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20–30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds), mid-troposphere <sup>210</sup>Pb vertical profiles, and the geographic distribution of aerosol optical depth is found for the new diagnostic scavenging scheme compared to the prescribed scavenging fraction scheme of the standard ECHAM5-HAM. The diagnostic and prognostic schemes represent the variability of scavenged fractions particularly for submicron size aerosols, and for mixed and ice phase clouds, and are recommended in preference to the prescribed scavenging fractions method

Estimated variability of below-cloud aerosol removal by rainfall for observed aerosol size distributions

International audienceBelow-cloud scavenging (BCS) coefficients of aerosols by rainfall are estimated for reported aerosol size distributions measured during field experiments in various environments. The method employed is based on explicit calculations of the efficiency of collision between a raindrop and aerosol particles. Results show that BCS coefficient increases with rainfall rate and has a significant dependence on aerosol size distribution parameters. Thus, BCS is important for very small particles (with diameters less than 0.01 µm) and for coarse particles (with diameters larger than 2 µm). For rainfall rate R ~ 1 mm hr -1, the 0.5-folding time of these particles is of the order of one hour. It is shown that BCS is negligible for aerosol particles in the range [0.1-1] µm if compared with in-cloud scavenging rates for low and moderate rainfall rates (R ~ 0.1-10 mm hr -1). The results indicate that a boundary layer aerosol size distribution with coarse mode is drastically affected very shortly after rain starts (in a fraction of one hour) and consequently, the below-cloud aerosol size distribution becomes dominated by particles in the accumulation mode