Scavenging of Soluble Gaseous Pollutants by Rain Droplets in the Atmosphere With Nocturnal Temperature Profile

Author(s):  
Andrew Fominykh ◽  
Tov Elperin ◽  
Boris Krasovitov

We analyze non-isothermal absorption of trace gases by the rain droplets with internal circulation which is caused by interfacial shear stresses. It is assumed that the temperature and concentration of soluble trace gases in the atmosphere varies in a vertical direction. The rate of scavenging of soluble trace gases by falling rain droplets is determined by solving heat and mass transfer equations. In the analysis we accounted for the accumulation of the absorbate in the bulk of the falling rain droplet. The problem is solved in the approximation of a thin concentration and temperature boundary layers in the droplet and in the surrounding air. We assumed that the bulk of a droplet, beyond the diffusion boundary layer, is completely mixed and concentration of the absorbate and temperature are homogeneous and time-dependent in the bulk. By combining the generalized similarity transformation method with Duhamel’s theorem, the system of transient conjugate equations of convective diffusion and energy conservation for absorbate transport in liquid and gaseous phases with time-dependent boundary conditions is reduced to a system of linear convolution Volterra integral equations of the second kind which is solved numerically. Calculations are performed using available experimental data on nocturnal temperature profiles in the atmosphere. It is shown than if concentration of a trace gas in the atmosphere is homogeneous and temperature in the atmosphere increases with altitude, droplet absorbs gas during all the period of its fall. Neglecting temperature inhomogenity in the atmosphere described by nocturnal temperature inversion leads to essential underestimation of the trace gas concentration in a droplet on the ground.

Author(s):  
Tov Elperin ◽  
Boris Krasovitov ◽  
Andrew Fominykh

We analyze non-isothermal absorption of soluble atmospheric trace gases by the falling rain droplets with internal circulation which is caused by interfacial shear stresses. It is assumed that the concentration of soluble trace gases and temperature in the atmosphere varies in a vertical direction. In the analysis we accounted for the accumulation of the absorbate in the bulk of the falling rain droplet. The problem is solved in the approximation of a thin concentration and temperature boundary layers in the droplet and in the surrounding air. We assumed that the bulk of a droplet, beyond the diffusion boundary layer, is completely mixed and concentration of the absorbate and temperature are homogeneous and time-dependent in the bulk. By combining the generalized similarity transformation method with Duhamel’s theorem, the system of transient conjugate equations of convective diffusion and energy conservation for absorbate transport in liquid and gaseous phases with time-dependent boundary conditions is reduced to a system of linear convolution Volterra integral equations of the second kind which is solved numerically. It is shown that the non-uniform vertical distribution of absorbate and temperature in a gaseous phase strongly affects mass transfer during gas absorption by a falling droplet.


2009 ◽  
Vol 66 (8) ◽  
pp. 2349-2358 ◽  
Author(s):  
Tov Elperin ◽  
Andrew Fominykh ◽  
Boris Krasovitov

Abstract This paper analyzes absorption of soluble atmospheric trace gases by falling rain droplets with internal circulation, which is caused by interfacial shear stresses. It is assumed that the concentration of soluble trace gases in the atmosphere varies in a vertical direction. In the analysis the accumulation of the absorbate in the bulk of the falling rain droplet was accounted for. The problem is solved in the approximation of a thin concentration boundary layer in the droplet and in the surrounding air. It was assumed that the bulk of a droplet, beyond the diffusion boundary layer, is completely mixed and that concentration of the absorbate is homogeneous and time dependent in the bulk. By combining the generalized similarity transformation method with Duhamel’s theorem, the system of transient conjugate equations of convective diffusion for absorbate transport in liquid and gaseous phases with time-dependent boundary conditions is reduced to a linear-convolution Volterra integral equation of the second kind, which is solved numerically. It is shown that the nonuniform vertical distribution of absorbate in a gaseous phase strongly affects mass transfer during gas absorption by a falling droplet.


2012 ◽  
Vol 12 (12) ◽  
pp. 32985-33023
Author(s):  
D. R. Allen ◽  
K. W. Hoppel ◽  
G. E. Nedoluha ◽  
D. D. Kuhl ◽  
N. L. Baker ◽  
...  

Abstract. Time-dependent variational data assimilation allows the possibility of extracting wind information from observations of long-lived trace gases. Since trace gas observations are not available at sufficient resolution for deriving feature-track winds, they must be combined with model background information to produce an analysis. If done with time-dependent variational assimilation, wind information may be extracted via the adjoint of the linearized tracer continuity equation. This paper presents idealized experiments that illustrate the mechanics of tracer-wind extraction and demonstrate some of the limitations of this procedure. We first examine tracer-wind extraction using a simple one-dimensional advection equation. The analytic solution for a single trace gas observation is discussed along with numerical solutions for multiple observations. The limitations of tracer-wind extraction are then explored using highly idealized ozone experiments performed with a development version of the Navy Global Environmental Model (NAVGEM) in which stratospheric globally-distributed hourly stratospheric ozone profiles are assimilated in a single 6-h update cycle in January 2009. Starting with perfect background ozone conditions, but imperfect dynamical conditions, ozone errors develop over the 6-h background window. Wind increments are introduced in the analysis in order to reduce the differences between background ozone and ozone observations. For "perfect" observations (unbiased and no random error), this results in root mean square (RMS) vector wind error reductions of up to ∼ 3 m s−1 in the winter hemisphere and tropics. Wind extraction is more difficult in the summer hemisphere due to weak ozone gradients and smaller background wind errors. The limitations of wind extraction are also explored for observations with imposed random errors and for limited sampling patterns. As expected, the amount of wind information extracted degrades as observation errors or data voids increase. In the case of poorly specified observation error covariances, assimilation of ozone data with imposed errors may result in erroneous wind increments, since the assimilation is constrained too tightly to the noisy observations.


2016 ◽  
Vol 16 (18) ◽  
pp. 11711-11732 ◽  
Author(s):  
Chelsea E. Stockwell ◽  
Thilina Jayarathne ◽  
Mark A. Cochrane ◽  
Kevin C. Ryan ◽  
Erianto I. Putra ◽  
...  

Abstract. Peat fires in Southeast Asia have become a major annual source of trace gases and particles to the regional–global atmosphere. The assessment of their influence on atmospheric chemistry, climate, air quality, and health has been uncertain partly due to a lack of field measurements of the smoke characteristics. During the strong 2015 El Niño event we deployed a mobile smoke sampling team in the Indonesian province of Central Kalimantan on the island of Borneo and made the first, or rare, field measurements of trace gases, aerosol optical properties, and aerosol mass emissions for authentic peat fires burning at various depths in different peat types. This paper reports the trace gas and aerosol measurements obtained by Fourier transform infrared spectroscopy, whole air sampling, photoacoustic extinctiometers (405 and 870 nm), and a small subset of the data from analyses of particulate filters. The trace gas measurements provide emission factors (EFs; grams of a compound per kilogram biomass burned) for up to  ∼  90 gases, including CO2, CO, CH4, non-methane hydrocarbons up to C10, 15 oxygenated organic compounds, NH3, HCN, NOx, OCS, HCl, etc. The modified combustion efficiency (MCE) of the smoke sources ranged from 0.693 to 0.835 with an average of 0.772 ± 0.053 (n  =  35), indicating essentially pure smoldering combustion, and the emissions were not initially strongly lofted. The major trace gas emissions by mass (EF as g kg−1) were carbon dioxide (1564 ± 77), carbon monoxide (291 ± 49), methane (9.51 ± 4.74), hydrogen cyanide (5.75 ± 1.60), acetic acid (3.89 ± 1.65), ammonia (2.86 ± 1.00), methanol (2.14 ± 1.22), ethane (1.52 ± 0.66), dihydrogen (1.22 ± 1.01), propylene (1.07 ± 0.53), propane (0.989 ± 0.644), ethylene (0.961 ± 0.528), benzene (0.954 ± 0.394), formaldehyde (0.867 ± 0.479), hydroxyacetone (0.860 ± 0.433), furan (0.772 ± 0.035), acetaldehyde (0.697 ± 0.460), and acetone (0.691 ± 0.356). These field data support significant revision of the EFs for CO2 (−8 %), CH4 (−55 %), NH3 (−86 %), CO (+39 %), and other gases compared with widely used recommendations for tropical peat fires based on a lab study of a single sample published in 2003. BTEX compounds (benzene, toluene, ethylbenzene, xylenes) are important air toxics and aerosol precursors and were emitted in total at 1.5 ± 0.6 g kg−1. Formaldehyde is probably the air toxic gas most likely to cause local exposures that exceed recommended levels. The field results from Kalimantan were in reasonable agreement with recent lab measurements of smoldering Kalimantan peat for “overlap species,” lending importance to the lab finding that burning peat produces large emissions of acetamide, acrolein, methylglyoxal, etc., which were not measurable in the field with the deployed equipment and implying value in continued similar efforts. The aerosol optical data measured include EFs for the scattering and absorption coefficients (EF Bscat and EF Babs, m2 kg−1 fuel burned) and the single scattering albedo (SSA) at 870 and 405 nm, as well as the absorption Ångström exponents (AAE). By coupling the absorption and co-located trace gas and filter data we estimated black carbon (BC) EFs (g kg−1) and the mass absorption coefficient (MAC, m2 g−1) for the bulk organic carbon (OC) due to brown carbon (BrC). Consistent with the minimal flaming, the emissions of BC were negligible (0.0055 ± 0.0016 g kg−1). Aerosol absorption at 405 nm was  ∼  52 times larger than at 870 nm and BrC contributed  ∼  96 % of the absorption at 405 nm. Average AAE was 4.97 ± 0.65 (range, 4.29–6.23). The average SSA at 405 nm (0.974 ± 0.016) was marginally lower than the average SSA at 870 nm (0.998 ± 0.001). These data facilitate modeling climate-relevant aerosol optical properties across much of the UV/visible spectrum and the high AAE and lower SSA at 405 nm demonstrate the dominance of absorption by the organic aerosol. Comparing the Babs at 405 nm to the simultaneously measured OC mass on filters suggests a low MAC ( ∼  0.1) for the bulk OC, as expected for the low BC/OC ratio in the aerosol. The importance of pyrolysis (at lower MCE), as opposed to glowing (at higher MCE), in producing BrC is seen in the increase of AAE with lower MCE (r2 =  0.65).


2017 ◽  
Vol 10 (12) ◽  
pp. 5075-5088 ◽  
Author(s):  
António Dias ◽  
Sebastian Ehrhart ◽  
Alexander Vogel ◽  
Christina Williamson ◽  
João Almeida ◽  
...  

Abstract. The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN (European Council for Nuclear Research) investigates the nucleation and growth of aerosol particles under atmospheric conditions and their activation into cloud droplets. A key feature of the CLOUD experiment is precise control of the experimental parameters. Temperature uniformity and stability in the chamber are important since many of the processes under study are sensitive to temperature and also to contaminants that can be released from the stainless steel walls by upward temperature fluctuations. The air enclosed within the 26 m3 CLOUD chamber is equipped with several arrays (strings) of high precision, fast-response thermometers to measure its temperature. Here we present a study of the air temperature uniformity inside the CLOUD chamber under various experimental conditions. Measurements were performed under calibration conditions and run conditions, which are distinguished by the flow rate of fresh air and trace gases entering the chamber at 20 and up to 210 L min−1, respectively. During steady-state calibration runs between −70 and +20 °C, the air temperature uniformity is better than ±0.06 °C in the radial direction and ±0.1 °C in the vertical direction. Larger non-uniformities are present during experimental runs, depending on the temperature control of the make-up air and trace gases (since some trace gases require elevated temperatures until injection into the chamber). The temperature stability is ±0.04 °C over periods of several hours during either calibration or steady-state run conditions. During rapid adiabatic expansions to activate cloud droplets and ice particles, the chamber walls are up to 10 °C warmer than the enclosed air. This results in temperature differences of ±1.5 °C in the vertical direction and ±1 °C in the horizontal direction, while the air returns to its equilibrium temperature with a time constant of about 200 s.


1966 ◽  
Vol 21 (7) ◽  
pp. 1098-1106 ◽  
Author(s):  
R. Lust ◽  
M. Scholer

The propagation of waves in the solar atmosphere is investigated with respect to the problem of the chromospheric spiculae and of the heating of the solar chromosphere and corona. In particular the influence of external magnetic fields is considered. Waves of finite amplitudes are numerically calculated by solving the time-dependent magnetohydrodynamic equation for two spatial dimensions by assuming axial symmetry. For the case without a magnetic field the comparison between one dimensional and two dimensional treatment shows the strong influence of the radial propagation on the steepening of waves in the vertical direction. In the presence of a magnetic field it is shown that the propagation is strongly guided along the lines of force. The steepening of the waves along the field is much larger as compared to the case where no field is present.


2016 ◽  
Author(s):  
Chelsea E. Stockwell ◽  
Thilina Jayarathne ◽  
Mark A. Cochrane ◽  
Kevin C. Ryan ◽  
Erianto I. Putra ◽  
...  

Abstract. Peat fires in Southeast Asia have become a major annual source of trace gases and particles to the regional-global atmosphere. The assessment of their influence on atmospheric chemistry, climate, air quality, and health has been uncertain partly due to a lack of field measurements of the smoke characteristics. During the strong 2015 El Niño event we deployed a mobile smoke sampling team in the Indonesian province of Central Kalimantan on the island of Borneo and made the first, or rare, field measurements of trace gases, aerosol optical properties, and aerosol mass emissions for authentic peat fires burning at various depths in different peat types. This paper reports the trace gas and aerosol measurements obtained by Fourier transform infrared spectroscopy, whole air sampling, photoacoustic extinctiometers (405 and 870 nm), and a small subset of the data from analyses of particulate filters. The trace gas measurements provide emission factors (EFs, g compound per kg biomass burned) for CO2, CO, CH4, non-methane hydrocarbons up to C10, 15 oxygenated organic compounds, NH3, HCN, NOx, OCS, HCl, etc.; up to ~90 gases in all. The modified combustion efficiency (MCE) of the smoke sources ranged from 0.693 to 0.835 with an average of 0.772 ± 0.053 (n = 35) indicating essentially pure smoldering combustion and the emissions were not initially strongly lofted. The major trace gas emissions by mass (EF as g/kg) were: carbon dioxide (1564 ± 77), carbon monoxide (291 ± 49), methane (9.51 ± 4.74), hydrogen cyanide (5.75 ± 1.60), acetic acid (3.89 ± 1.65), ammonia (2.86 ± 1.00), methanol (2.14 ± 1.22), ethane (1.52 ± 0.66), dihydrogen (1.22 ± 1.01), propylene (1.07 ± 0.53), propane (0.989 ± 0.644), ethylene (0.961 ± 0.528), benzene (0.954 ± 0.394), formaldehyde (0.867 ± 0.479), hydroxyacetone (0.860 ± 0.433), furan (0.772 ± 0.035), acetaldehyde (0.697 ± 0.460), and acetone (0.691 ± 0.356). These field data support significant revision of the EFs for CO2 (−8 %), CH4 (−55 %), NH3 (−86 %), CO (+39 %) and other gases compared with widely-used recommendations for tropical peat fires based on a lab study of a single sample published in 2003. BTEX compounds (benzene, toluene, ethylbenzene, xylenes) are important air toxics and aerosol precursors and were emitted in total at 1.5 ± 0.6 g/kg. Formaldehyde is probably the air toxic gas most likely to cause local exposures that exceed recommended levels. The field results from Kalimantan were in reasonable agreement with recent (2012) lab measurements of smoldering Kalimantan peat for “overlap species,” lending importance to the lab finding that burning peat produces large emissions of acetamide, acrolein, methylglyoxal, etc., which were not measureable in the field with the deployed equipment and implying value in continued similar efforts. The aerosol optical data measured include EFs for the scattering and absorption coefficients (EF Bscat and EF Babs, m2/kg fuel burned) and the single scattering albedo (SSA) at 870 and 405 nm, as well as the absorption Ångstrӧm exponents (AAE). By coupling the absorption and co-located trace gas and filter data we estimated black carbon (BC) EFs (g/kg) and the mass absorption coefficient (MAC, m2/g) for the bulk organic carbon (OC) due to brown carbon (BrC). Consistent with the minimal flaming, the emissions of BC were negligible (0.0055 ± 0.0016 g/kg). Aerosol absorption at 405 nm was ~52 times larger than at 870 nm and BrC contributed ~96 % of the absorption at 405 nm. Average AAE was 4.97 ± 0.65 (range, 4.29–6.23). The average SSA at 405 nm (0.974 ± 0.016) was marginally lower than the average SSA at 870 nm (0.998 ± 0.001). These data facilitate modeling climate-relevant aerosol optical properties across much of the UV/visible spectrum and the high AAE and lower SSA at 405 nm demonstrate the dominance of absorption by the organic aerosol. Comparing the Babs at 405 nm to the simultaneously measured OC mass on filters suggests a low MAC (~0.1) for the bulk OC, as expected for the low BC / OC ratio in the aerosol. The importance of pyrolysis (at lower MCE), as opposed to glowing (at higher MCE), in producing BrC is seen in the increase of AAE with lower MCE (r2 = 0.65).


2021 ◽  
Author(s):  
Pieternel F. Levelt ◽  
Deborah C. Stein Zweers ◽  
Ilse Aben ◽  
Maite Bauwens ◽  
Tobias Borsdorff ◽  
...  

Abstract. The aim of this paper is two-fold: to provide guidance on how to best interpret TROPOMI trace gas retrievals and to highlight how TROPOMI trace gas data can be used to understand event-based impacts on air quality from regional to city-scales around the globe. For this study, we present the observed changes in the atmospheric column amounts of five trace gases (NO2, SO2, CO, HCHO and CHOCHO) detected by the Sentinel-5P TROPOMI instrument, driven by reductions of anthropogenic emissions due to COVID-19 lockdown measures in 2020. We report clear COVID-19-related decreases in NO2 concentrations on all continents. For megacities, reductions in column amounts of tropospheric NO2 range between 14 % and 63 %. For China and India supported by NO2 observations, where the primary source of anthropogenic SO2 is coal-fired power generation, we were able to detect sector-specific emission changes using the SO2 data. For HCHO and CHOCHO, we consistently observe anthropogenic changes in two-week averaged column amounts over China and India during the early phases of the lockdown periods. That these variations over such a short time scale are detectable from space, is due to the high resolution and improved sensitivity of the TROPOMI instrument. For CO, we observe a small reduction over China which is in concert with the other trace gas reductions observed during lockdown, however large, interannual differences prevent firm conclusions from being drawn. The joint analysis of COVID-19 lockdown-driven reductions in satellite observed trace gas column amounts, using the latest operational and scientific retrieval techniques for five species concomitantly is unprecedented. However, the meteorologically and seasonally driven variability of the five trace gases does not allow for drawing fully quantitative conclusions on the reduction of anthropogenic emissions based on TROPOMI observations alone. We anticipate that in future, the combined use of inverse modelling techniques with the high spatial resolution data from S5P/TROPOMI for all observed trace gases presented here, will yield a significantly improved sector-specific, space-based analysis of the impact of COVID-19 lockdown measures as compared to other existing satellite observations. Such analyses will further enhance the scientific impact and societal relevance of the TROPOMI mission.


2021 ◽  
Author(s):  
Zoe Davis ◽  
Debora Griffin ◽  
Yue Jia ◽  
Susann Tegtmeier ◽  
Mallory Loria ◽  
...  

<p>A recent method uses satellite measurements to estimate lifetimes and emissions of trace-gases from point sources (Fioletov et al., 2015). Emissions are retrieved by fitting measured vertical column densities (VCDs) of trace-gases to a three-dimensional function of the wind speed and spatial coordinates. In this study, a plume model generated “synthetic” satellite observations of prescribed emissions to examine the accuracy of the retrieved emissions. The Lagrangian transport and dispersion model FLEXPART (v10.0) modelled the plume from a point source over a multi-day simulation period at a resolution much higher than current satellite observations. The study aims to determine how various assumptions in the retrieval method and local meteorological conditions affect the accuracy and precision of emissions. These assumptions include that the use of a vertical mean of the wind profile is representative of the transport of the plume’s vertical column. In the retrieval method, the VCDs’ pixel locations are rotated around the source based on wind direction so that all plumes have a common wind direction. Retrievals using a vertical mean wind for rotation will be compared to retrievals using VCDs determined by rotating each altitude of the vertical profile of trace-gas using the respective wind-direction. The impact of local meteorological factors on the two approaches will be presented, including atmospheric mixing, vertical wind shear, and boundary layer height. The study aims to suggest which altitude(s) of the vertical profile of winds results in the most accurate retrievals given the local meteorological conditions. The study will also examine the impact on retrieval accuracy due to satellite resolution, trace-gas lifetime, plume source altitude, number of overpasses, and random and systematic errors. Sensitivity studies repeated using a second, “line-density”, retrieval method will also be presented (Adams et al., 2019; Goldberg et al., 2019).</p>


2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  

<p>Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO<sub>2</sub>, CH<sub>4</sub>, CO, and O<sub>3</sub> conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM<sub>2.5 </sub>chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO<sub>2</sub>, CH<sub>4</sub> and O<sub>3</sub> mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O<sub>3</sub> levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM<sub>2.5 </sub>composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.</p><p> </p><p><strong>REFERENCES</strong></p><p>[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172–1187 (2019).</p><p>[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.</p>


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