the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Modeling simulation of aerosol light absorption over the Beijing-Tianjin-Hebei region: the impact of mixing state and aging processes
Abstract. The mixing state and aging characteristics of black carbon (BC) aerosols are the key factors in calculating their optical properties and quantifying their impacts on radiation balance and global climate change. Considerable uncertainty still exists in the absorption properties of BC-containing aerosols and the absorption enhancement (Eabs) due to the lensing effect. It is crucial to reasonably represent the mixing of BC with other aerosol components to reduce the uncertainty. In this study, the absorption properties of PM2.5 were investigated based on the nested air quality prediction model system (NAQPMS) with different assumptions of the aerosol mixing state. The absorption coefficient (babs) is highest under uniform internal mixing, lower under core-shell mixing, and lowest under the assumption of external mixing. The result under core-shell mixing is closest to the observation. The aging process and coating thickness were well produced by the advanced particle microphysical module (APM) in NAQPMS. Then the fraction of embedded BC and secondary components coating aerosols was used to constrain the mixing state. The Eabs at 880 nm over the Beijing-Tianjin-Hebei region was 2.0~2.5 under core-shell mixing. When the fraction of coated BC and the coating layer are resolved, the Eabs_880 caused by the lensing effect can decrease by 30~43 % to 1.2~1.7, which is close to the range reported in previous studies. This study highlights the importance of representing the microphysical processes governing the mixing state and aging of BC and provides a reference for quantifying its radiative effect.
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RC1: 'Comment on egusphere-2024-1432', Anonymous Referee #1, 09 Sep 2024
This manuscript investigated the influences of mixing state on BC light absorption properties, mainly based on simulations. Different scenarios were designed, and the modeling results were constrained using field observational data. Although the topic of this manuscript is within the scope of ACP, I have substantial concerns on the methodologies as well as some results. It needs to be re-reviewed after major revisions. First, the estimation of POC and SOC using the EC-tracer method. In the current manuscript, the minimum OC to EC ratio (1.16) was used to represent primary emissions (Page 4, equation 1). This approach needs to be refined, e.g., by using the lowest 10 % percentile of ambient OC/EC ratios (please refer to https://doi.org/10.1029/2008JD010902; Atmos. Chem. Phys., 15, 2969–2983, 2015; etc.). In addition, the POC and SOC results should be carefully evaluated, e.g., by examining the dependence of SOC on RH, and the relationship between POC and carbon monoxide. Second, the robustness of the measured babs, i.e., the observational constraint. For AE33, the correction factor for multiple scattering effect should be carefully determined (rather than simply using a reported value). In addition, please confirm that similar to results from in-situ techniques (e.g., photoacoustic spectrometer), the AE33-based light absorption coefficients are “sensitive” to BC mixing state, e.g., by examining the relationship between babs and EC mass concentration. Third, based on Figure 6 and Table 2, the performance of the “CSs” scenario (i.e., core-shell mixing) appeared best for reproducing the measured light absorption coefficients. Then I could not understand why the author argued that “Partial internal mixing and partial coating are the closest to reality”. For the same reason, the logic of Sections 3.3 and 3.4 was confusing.
Citation: https://doi.org/10.5194/egusphere-2024-1432-RC1 -
RC2: 'Comment on egusphere-2024-1432', Anonymous Referee #3, 13 Dec 2024
This study uses the APM model combined with observations to discuss the impact of representative schemes of aerosols on optics. The whole study is meaningful and helpful for the experiment and model development. However, excessive use of concepts to represent aerosol mixing states lacks detailed and intuitive introductions, which reduces readability. A minor revision should be added before accepting.
1. Many excellent concept maps can be referenced to enhance readers' understanding of mixing states, such as Fig. 4 in 10.1038/s41467-018-05635-1, Fig. 1 in 10.1175/bams-d-16-0028.1
2. Line 40: add references for condensation and coagulation processes: 10.1016/j.isci.2023.108125
3. Lines 190-192: Fin and Fc are not clear? Number fraction? Mass fraction?
4. What are the differences between CS-Fin and CS-FinFc? You divided accumulation mode aerosols into 4 types (embedded, partly coated, bare-like BC and BC-free) or 3 types (embedded, bare-like BC and BC-free)? Detailed introductions should be added for mixing states in Table 1.
5. How to define Partial internal mixing and partial coating?
6. Line 313: How do you calculate Eabs? Add detailed calculation/inversion process.
Citation: https://doi.org/10.5194/egusphere-2024-1432-RC2
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