Simulated photochemical response to observational constraints on aerosol vertical distribution over North China

<p>The significance of aerosol–photolysis interaction (API) in atmospheric photochemistry has been emphasized by studies utilizing box models and chemical transport models. However, few studies have considered the actual aerosol vertical distribution when evaluating API effects due to the lack...

Full description

Saved in:
Bibliographic Details
Main Authors: X. Chen, K. Li, T. Yang, X. Jin, L. Chen, Y. Yang, S. Zhao, B. Hu, B. Zhu, Z. Wang, H. Liao
Format: Article
Language:English
Published: Copernicus Publications 2025-08-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/25/9151/2025/acp-25-9151-2025.pdf
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1849229114339229696
author X. Chen
X. Chen
K. Li
K. Li
T. Yang
X. Jin
X. Jin
L. Chen
L. Chen
Y. Yang
Y. Yang
S. Zhao
B. Hu
B. Zhu
Z. Wang
H. Liao
H. Liao
author_facet X. Chen
X. Chen
K. Li
K. Li
T. Yang
X. Jin
X. Jin
L. Chen
L. Chen
Y. Yang
Y. Yang
S. Zhao
B. Hu
B. Zhu
Z. Wang
H. Liao
H. Liao
author_sort X. Chen
collection DOAJ
description <p>The significance of aerosol–photolysis interaction (API) in atmospheric photochemistry has been emphasized by studies utilizing box models and chemical transport models. However, few studies have considered the actual aerosol vertical distribution when evaluating API effects due to the lack of observations and the uncertainties in model simulation. Herein, we integrated lidar and radiosonde observations with the chemical transport model (GEOS-Chem) to quantify the response of photochemistry to observational constraints on aerosol vertical distribution across different seasons in North China. The underestimation of aerosol optical depth (AOD) in lower layers and the overestimation in upper layers in GEOS-Chem model were revised. In response, photolysis rates changed following AOD, showing 33.4 %–73.8 % increases at the surface. Surface ozone increased by an average of 0.9 and 0.5 ppb in winter and summer, and the default API impact on ozone reduced by 36 %–56 %. The weaker response in summer can be related to the compensatory effects of stronger turbulence mixing in the boundary layer. The long-lasting underestimation of ozone levels in winter was also greatly improved. Due to the enhanced photochemistry, PM<span class="inline-formula"><sub>2.5</sub></span> increased by 0.8 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> in winter and 0.2 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> in summer and increased strongly during pollution events, with a maximum daily change of 16.5 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> at Beijing station in winter. The weakened API effect in turn enhanced nitric acid formation by increasing atmospheric oxidizing capacity (13.5 % increase for OH radical) in high NO<span class="inline-formula"><sub><i>x</i></sub></span> emission areas, and this helps explain the strong response of PM<span class="inline-formula"><sub>2.5</sub></span> in winter.</p>
format Article
id doaj-art-9bdbc2a6ff684971848e622c49004b81
institution Kabale University
issn 1680-7316
1680-7324
language English
publishDate 2025-08-01
publisher Copernicus Publications
record_format Article
series Atmospheric Chemistry and Physics
spelling doaj-art-9bdbc2a6ff684971848e622c49004b812025-08-22T05:47:16ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242025-08-01259151916810.5194/acp-25-9151-2025Simulated photochemical response to observational constraints on aerosol vertical distribution over North ChinaX. Chen0X. Chen1K. Li2K. Li3T. Yang4X. Jin5X. Jin6L. Chen7L. Chen8Y. Yang9Y. Yang10S. Zhao11B. Hu12B. Zhu13Z. Wang14H. Liao15H. Liao16State Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaState Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaState Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaState Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaState Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaState Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaCollege of Chemistry and Chemical Engineering, Dezhou University, Dezhou 253023, ChinaState Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaCollaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Key Laboratory for Aerosol-Cloud-Precipitation of China Meteorological Administration, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaState Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC), Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaState Key Laboratory of Climate System Prediction and Risk Management, Joint International Research Laboratory of Climate and Environment Change, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Collaborative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science and Technology, Nanjing 210044, ChinaSchool of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China<p>The significance of aerosol–photolysis interaction (API) in atmospheric photochemistry has been emphasized by studies utilizing box models and chemical transport models. However, few studies have considered the actual aerosol vertical distribution when evaluating API effects due to the lack of observations and the uncertainties in model simulation. Herein, we integrated lidar and radiosonde observations with the chemical transport model (GEOS-Chem) to quantify the response of photochemistry to observational constraints on aerosol vertical distribution across different seasons in North China. The underestimation of aerosol optical depth (AOD) in lower layers and the overestimation in upper layers in GEOS-Chem model were revised. In response, photolysis rates changed following AOD, showing 33.4 %–73.8 % increases at the surface. Surface ozone increased by an average of 0.9 and 0.5 ppb in winter and summer, and the default API impact on ozone reduced by 36 %–56 %. The weaker response in summer can be related to the compensatory effects of stronger turbulence mixing in the boundary layer. The long-lasting underestimation of ozone levels in winter was also greatly improved. Due to the enhanced photochemistry, PM<span class="inline-formula"><sub>2.5</sub></span> increased by 0.8 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> in winter and 0.2 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> in summer and increased strongly during pollution events, with a maximum daily change of 16.5 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span> at Beijing station in winter. The weakened API effect in turn enhanced nitric acid formation by increasing atmospheric oxidizing capacity (13.5 % increase for OH radical) in high NO<span class="inline-formula"><sub><i>x</i></sub></span> emission areas, and this helps explain the strong response of PM<span class="inline-formula"><sub>2.5</sub></span> in winter.</p>https://acp.copernicus.org/articles/25/9151/2025/acp-25-9151-2025.pdf
spellingShingle X. Chen
X. Chen
K. Li
K. Li
T. Yang
X. Jin
X. Jin
L. Chen
L. Chen
Y. Yang
Y. Yang
S. Zhao
B. Hu
B. Zhu
Z. Wang
H. Liao
H. Liao
Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
Atmospheric Chemistry and Physics
title Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
title_full Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
title_fullStr Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
title_full_unstemmed Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
title_short Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
title_sort simulated photochemical response to observational constraints on aerosol vertical distribution over north china
url https://acp.copernicus.org/articles/25/9151/2025/acp-25-9151-2025.pdf
work_keys_str_mv AT xchen simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT xchen simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT kli simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT kli simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT tyang simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT xjin simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT xjin simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT lchen simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT lchen simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT yyang simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT yyang simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT szhao simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT bhu simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT bzhu simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT zwang simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT hliao simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina
AT hliao simulatedphotochemicalresponsetoobservationalconstraintsonaerosolverticaldistributionovernorthchina