the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Identifying Better Indicators of Aerosol Wet Scavenging During Long-Range Transport
Abstract. As the dominant sink of aerosol particles, wet scavenging greatly influences aerosol lifetime and interactions with clouds, precipitation, and radiation. However, wet scavenging remains highly uncertain in models, hindering accurate predictions of aerosol spatiotemporal distributions and downstream interactions. In this study, we present a flexible, computationally inexpensive method to identify meteorological variables relevant to estimating wet scavenging using a combination of aircraft, satellite, and reanalysis data augmented by trajectory modeling to account for air mass history. Treating the enhancement (Δ) ratio of black carbon and carbon monoxide (ΔBC/ΔCO) measured by aircraft as an in situ proxy for wet scavenging, we assess the capabilities of an array of meteorological variables to predict ΔBC/ΔCO using regression statistics derived from curve-fitting and k-fold cross-validation. We find that accumulated precipitation along trajectories (APT) – treated as a wet scavenging indicator across multiple studies – is unable to accurately capture ΔBC/ΔCO trends, suggesting that APT is not a good indicator of wet scavenging effects. In contrast, the frequencies of precipitation or high relative humidity along trajectories better predict ΔBC/ΔCO trends and magnitudes, suggesting that these types of meteorological variables are better than APT for estimating the degree of wet scavenging in an air mass. Precipitation characteristics (e.g., intensity, frequency) from satellite retrievals are better indicators of ΔBC/ΔCO than those calculated from reanalysis, supporting previous studies that demonstrated reanalysis to be less reliable than satellite retrievals in terms of precipitation. Finally, top quantiles (e.g., 90th) of relative humidity are able to consistently capture the behavior of ΔBC/ΔCO and may also be a more suitable indicator of wet scavenging than APT. Future studies can use the best-performing meteorological variables identified in our study to estimate wet scavenging. Furthermore, this method can be repeated for different regions to identify region-specific factors influencing wet scavenging, and our findings may be useful for informing scavenging parametrization schemes in models.
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Notice on discussion status
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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Preprint
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
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Supplement
(625 KB) - BibTeX
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- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2023-726', Anonymous Referee #1, 13 Jul 2023
The comments were posted as a supplement file (PDF).
- AC1: 'Reply on RC1', Miguel Ricardo Hilario, 25 Oct 2023
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RC2: 'Comment on egusphere-2023-726', Anonymous Referee #2, 01 Aug 2023
This study aims to identify meteorological variables affecting precipitation scavenging of atmospheric aerosols using a combination of aircraft, satellite, and reanalysis data augmented by trajectory modeling to account for air mass history. In literature, key variables controlling below-cloud aerosol scavenging have been well documented, although existing parametrizations still have large uncertainties (especially for particles in the submicron size range). This study addresses the former (key variables), but added little knowledge on the latter (how to reduce the uncertainties in parametrizations). The analysis approach is also subject to large uncertainties. I only provided a few comments related to the science of precipitation scavenging for the authors to consider in improving the quality of the manuscript.
Lines 25-28: Most existing parameterizations for precipitation scavenging of atmospheric aerosols have considered precipitation intensity, precipitation amount, and raindrop and aerosol size distributions, etc. It is not clear what (additional) variables this study proposes (after reading the whole abstract) for better parametrizing wet scavenging of atmospheric aerosols. The authors are encouraged to provide an explicit recommendation instead of a general statement. This comment also applies to the Conclusions section (the last paragraph) since no clear message of their recommendations is provided.
Section 2.2: If BC and CO have the same sources but different sinks (one is wet scavenged and the other is not), then using this ratio approach is reasonable in tracking the wet scavenging of BC. However, if they have different sources along the air mass trajectory (which is likely the case), this approach would cause very larger uncertainties.
Lines 78-92: In Chemical transport models, time splitting approach is used for calculating each physical and chemical process (emission, transport/diffusion, chemical transformation, deposition (in-cloud nucleation, below-cloud scavenging, and dry deposition)). Each process needs to be calculated or parametrized as accurate as possible. To improve the parameterization of below-cloud aerosol scavenging, collecting field data through measuring aerosol concentrations before and after precipitation events covering different precipitation types and intensities would be the best approach, in my opinion. The approach used in this study involves both in-cloud and below-cloud scavenging contributions as well as additional entrainment of pollutants along the air mass trajectory, and is not possible to quantify precipitation scavenging. I have difficulties in finding the true scientific value in such an analysis for improving our understanding in below-cloud aerosol scavenging (which seems to the major goal of this study).
Line 11 and line 31: This sentence implies that wet scavenging is the only dominant sink for aerosol particles. I would consider both dry deposition and wet scavenging as dominant sinks. Maybe change to “As one of the dominant sinks”.
Lines 43-44: You should also include “precipitation intensity, amount, frequency, type”. Precipitation type includes liquid and solid (snow) precipitation.
Lines 41-50: I would like to draw your attention of a series of studies on below-cloud aerosol scavenging conducted by a group in Environment Canada to enhance the discuss presented in this paragraph. They not only systematically assessed important parameters affecting below-cloud aerosol scavenging (Wang et al., 2010, ACP, 10, 5685-5705; Wang et al., 2011, ACP 11, 11859-11866; Zhang et al., 2013, ACP 13, 10005-10025), but also developed a new set of semi-empirical parameterizations (Wang et al., 2014a, GMD, 7, 799–819; 2014b, JAMES, 6, 1301-1310).
Line 97: Was the experiment cover one single site or one big area?
Lines 229 and below: RH is identified as a key variable, but it is likely because its directly link with precipitation. In this case, there is no need to include this additional variable in precipitation scavenging parameterization. If the effect of the high RH is through hydroscopic growth of particles, then this needs to be mentioned.
Citation: https://doi.org/10.5194/egusphere-2023-726-RC2 - AC1: 'Reply on RC1', Miguel Ricardo Hilario, 25 Oct 2023
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2023-726', Anonymous Referee #1, 13 Jul 2023
The comments were posted as a supplement file (PDF).
- AC1: 'Reply on RC1', Miguel Ricardo Hilario, 25 Oct 2023
-
RC2: 'Comment on egusphere-2023-726', Anonymous Referee #2, 01 Aug 2023
This study aims to identify meteorological variables affecting precipitation scavenging of atmospheric aerosols using a combination of aircraft, satellite, and reanalysis data augmented by trajectory modeling to account for air mass history. In literature, key variables controlling below-cloud aerosol scavenging have been well documented, although existing parametrizations still have large uncertainties (especially for particles in the submicron size range). This study addresses the former (key variables), but added little knowledge on the latter (how to reduce the uncertainties in parametrizations). The analysis approach is also subject to large uncertainties. I only provided a few comments related to the science of precipitation scavenging for the authors to consider in improving the quality of the manuscript.
Lines 25-28: Most existing parameterizations for precipitation scavenging of atmospheric aerosols have considered precipitation intensity, precipitation amount, and raindrop and aerosol size distributions, etc. It is not clear what (additional) variables this study proposes (after reading the whole abstract) for better parametrizing wet scavenging of atmospheric aerosols. The authors are encouraged to provide an explicit recommendation instead of a general statement. This comment also applies to the Conclusions section (the last paragraph) since no clear message of their recommendations is provided.
Section 2.2: If BC and CO have the same sources but different sinks (one is wet scavenged and the other is not), then using this ratio approach is reasonable in tracking the wet scavenging of BC. However, if they have different sources along the air mass trajectory (which is likely the case), this approach would cause very larger uncertainties.
Lines 78-92: In Chemical transport models, time splitting approach is used for calculating each physical and chemical process (emission, transport/diffusion, chemical transformation, deposition (in-cloud nucleation, below-cloud scavenging, and dry deposition)). Each process needs to be calculated or parametrized as accurate as possible. To improve the parameterization of below-cloud aerosol scavenging, collecting field data through measuring aerosol concentrations before and after precipitation events covering different precipitation types and intensities would be the best approach, in my opinion. The approach used in this study involves both in-cloud and below-cloud scavenging contributions as well as additional entrainment of pollutants along the air mass trajectory, and is not possible to quantify precipitation scavenging. I have difficulties in finding the true scientific value in such an analysis for improving our understanding in below-cloud aerosol scavenging (which seems to the major goal of this study).
Line 11 and line 31: This sentence implies that wet scavenging is the only dominant sink for aerosol particles. I would consider both dry deposition and wet scavenging as dominant sinks. Maybe change to “As one of the dominant sinks”.
Lines 43-44: You should also include “precipitation intensity, amount, frequency, type”. Precipitation type includes liquid and solid (snow) precipitation.
Lines 41-50: I would like to draw your attention of a series of studies on below-cloud aerosol scavenging conducted by a group in Environment Canada to enhance the discuss presented in this paragraph. They not only systematically assessed important parameters affecting below-cloud aerosol scavenging (Wang et al., 2010, ACP, 10, 5685-5705; Wang et al., 2011, ACP 11, 11859-11866; Zhang et al., 2013, ACP 13, 10005-10025), but also developed a new set of semi-empirical parameterizations (Wang et al., 2014a, GMD, 7, 799–819; 2014b, JAMES, 6, 1301-1310).
Line 97: Was the experiment cover one single site or one big area?
Lines 229 and below: RH is identified as a key variable, but it is likely because its directly link with precipitation. In this case, there is no need to include this additional variable in precipitation scavenging parameterization. If the effect of the high RH is through hydroscopic growth of particles, then this needs to be mentioned.
Citation: https://doi.org/10.5194/egusphere-2023-726-RC2 - AC1: 'Reply on RC1', Miguel Ricardo Hilario, 25 Oct 2023
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Miguel Ricardo A. Hilario
Avelino F. Arellano
Ali Behrangi
Ewan C. Crosbie
Joshua P. DiGangi
Glenn S. Diskin
Michael A. Shook
Luke D. Ziemba
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(1373 KB) - Metadata XML
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Supplement
(625 KB) - BibTeX
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- Final revised paper