the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Parameterization of particle formation rates in distinct atmospheric environments
Abstract. Atmospheric particle formation rate (J) is one of the key characteristics in new particle formation (NPF) processes worldwide. It is related to the development of ultrafine particle growth to cloud condensation nuclei (CCN) and, hence, to Earth radiative forcing in global models, which helps us to better understand the impact of NPF on cloud properties and climate change. In this work, we parameterized four semi-empirical J models for 5 nm atmospheric particles using field measurements obtained from distinct environments that varied from clean to heavily polluted regions and from tropical to polar regions. The models rely primarily on sulfuric acid as a condensing vapor, condensation sink to account for the vapor loss, and relative humidity for meteorological contribution to J. The parameterization results showed that our models were able to produce plausible predictions for boreal forest environments, heavily polluted environments, and biogenic environments with high relative humidity. We further tested the models in the global simulation module Tracer Model 5 (TM5, massive parallel version) to simulate particle number size distribution across 14 global atmospheric measurement sites. The simulated results showed satisfactory predictions on particle number concentrations for all the tested environments, with significant improvement in the nucleation mode, and better prediction accuracy for Aitken and accumulation modes compared to the binary sulfuric acid-organic vapor model in Riccobono (2014). Our study has successfully provided powerful tools to predict J5 on a global scale across various environment types using the most essential and more accessible variables involved in the NPF processes. Essentially, this work reinforces the necessity for global research into the investigation of environment-oriented meteorology-involved NPF processes.
Competing interests: At least one of the (co-)authors is a member of the editorial board of Aerosol Research.
Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this preprint. The responsibility to include appropriate place names lies with the authors.- Preprint
(2191 KB) - Metadata XML
-
Supplement
(897 KB) - BibTeX
- EndNote
Status: open (until 20 Mar 2025)
-
RC1: 'Comment on ar-2025-3', Anonymous Referee #1, 06 Mar 2025
reply
Based on a comprehensive dataset of field observation, Li et al. developed a series of J-models to better predict aerosol formation rates globally. In the models, sulfuric acid (SA) was considered the dominant gaseous nucleation precursor, and RH was used to represent the meteorological impacts of NPF. Overall, the models' performance was satisfactory and showed significant improvements over the SA-Organic binary nucleation model. It is well-accepted that aerosols play an important but extremely uncertain role in regulating the solar-terrestrial radiation budget. It is still very challenging for climate models to accurately predict PNSD and aerosol number concentration on a global scale due to the complexity and diversity of nucleation mechanisms worldwide. Therefore, this is a very important work although the parameterization method were compromised by data availability and the possibility of over-fitting. It is difficult to use one set of parameters to estimate NPF rates worldwide. The limitations of these models should be fully addressed. Therefore, I would recommend this manuscript for publication after the following comments are sufficiently addressed.
Specific comments:
1) L217-218: I think the correction for hygroscopic growth was necessary for the intercomparisons. The CS and CoagS terms may vary substantially depending on the RH and the aerosol chemical compositions.
2)L248: It is understandable not to include HOMs and NH3 in the parameterization due to the lack of data. However, it is more important to know how the exclusion of these compounds would impact the performance of these models. How sensitive are these models to the H2SO4 data, especially when H2SO4 proxies are used, which may lead to substantial uncertainty in H2SO4 input data?
3) L356: Strictly speaking, NPFs were often associated with Low RH conditions, which does not necessarily mean that low RH favors NPFs. These two phenomena may concur due to the same underlying cause. For instance, stronger solar irradiation can lead to higher ambient temperature and, thus, lower RH. However, the real factor in intensifying NPF could be the increased atmospheric photooxidation capacity that led to more production of NPF gas precursors.
4) L357: It is a bit strange that the higher SA and lower CS in Värriö would lead to a lower frequency of NPF.
5) L373: There is still no direct evidence that meteorology will significantly impact NPF in Beijing. The CS term was indeed playing a critical role in regulating NPF in Beijing.
6) L374-375: How did background aerosols sustain NPF? Did not the loss to preexisting aerosols compete with the formation of sub-5 nm particles? The high levels of background SO2, VOCs, and their oxidation products may be responsible for the intense NPFs in Beijing.
7) L411: These results strongly suggested that precursors other than H2SO4 should be considered for these models to work appropriately in marine environments.
8) L426: The Manacapuru case may be very special. The RH was very high year-round, and thus, J5 became insensitive to variations in RH and the corresponding aerosol hygroscopic growth, which may be treated as a constant. This may explain the better slope (1.02) found in model 1 simulation (Fig. 3h1).
9) These J-models were developed to predict NPF rates globally, but they did not consider nucleation mechanisms involving iodine oxoacids (IO). Since ~70% of the Earth's surface is seawater, how would this affect the application of these J-models by omitting IO-related NPF mechanisms?
Citation: https://doi.org/10.5194/ar-2025-3-RC1
Supplement
Viewed
HTML | XML | Total | Supplement | BibTeX | EndNote | |
---|---|---|---|---|---|---|
149 | 24 | 6 | 179 | 14 | 7 | 4 |
- HTML: 149
- PDF: 24
- XML: 6
- Total: 179
- Supplement: 14
- BibTeX: 7
- EndNote: 4
Viewed (geographical distribution)
Country | # | Views | % |
---|
Total: | 0 |
HTML: | 0 |
PDF: | 0 |
XML: | 0 |
- 1