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Improved understanding of PM2.5 in Korea and China �through integrated modeling and analysis of satellite, aircraft, and surface observations

�Daniel Jacob

Samsung PM2.5 Strategic Research Program

Year 3 Report

Shixian Zhai

Jared Brewer

Laura Yang

Brewer, J.F., D.J. Jacob, S.H. Jathar, Y. He, A. Akherati, S. Zhai, D.S. Jo, A. Hodzic, B.A. Nault, P. Campuzano-Jost, J.L. Jimenez, R.J. Park, Y.J. Oak, and H. Liao, A scheme for representing aromatic secondary organic aerosols in chemical transport models: application to source attribution of organic aerosols over South Korea during the KORUS-AQ campaign, J. Geophys. Res., e2022JD037257, 2023.

Colombi, N. K., Jacob, D. J., Yang, L. H., Zhai, S., Shah, V., Grange, S. K., Yantosca, R. M., Kim, S., and Liao, H.: Why is ozone in South Korea and the Seoul Metropolitan Area so high and increasing?, Atmos. Chem. Phys., 23, 4031–4044, 2023.

Yang, L.H., D.J. Jacob, N.K. Colombi, S. Zhai, K.H. Bates, V. Shah, E. Beaudry, R.M. Yantosca, H. Lin, J.F. Brewer, H. Chong, K.R. Travis, J.H. Crawford, L. Lamsal, J.-H. Koo, and J. Kim, Tropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: Implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from space, Atmos. Chem. Phys., 23, 2465–2481, 2023.

Zhai, S., Jacob, D. J., Pendergrass, D. C., Colombi, N. K., Shah, V., Yang, L. H., Zhang, Q., Wang, S., Kim, H., Sun, Y., Choi, J.-S., Park, J.-S., Luo, G., Yu, F., Woo, J.-H., Kim, Y., Dibb, J. E., Lee, T., Han, J.-S., Anderson, B. E., Li, K., and Liao, H.: Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate, Atmos. Chem. Phys., 23, 4271–4281, 2023.

Nadia Colombi

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Simulation of organic aerosol observations during KORUS-AQ (May-June 2016)

GEOS-Chem model

  • New SOM-VBS scheme for aromatic and S/IVOC SOA can reproduce observations much better than standard GEOS-Chem schemes
  • Oxidized POA, aromatic SOA, S/IVOC SOA are the main components
  • New scheme is now slated to go into the standard GEOS-Chem

Brewer et al. [2023]

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Contributions to surface organic aerosol over Korea

from GEOS-Chem simulations with SOM-VBS scheme (May-Jun 2016)

baseline simulation

no anthro. emissions in Korea

no anthro. emissions anywhere

OA over Korea is ≈ 1/3 biogenic, 1/3 domestic anthropogenic, 1/3 foreign anthropogenic

Brewer et al. [2023]

Mean OA over Korea

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Why is ozone over Korea so high and increasing?

2016

  • Increase is largest in May
  • GEOS-Chem with 22% decrease in NOx emissions (based on NO2 data) can capture the ozone levels and trend

Colombi et al. [2023]

mean value for Korea

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Further analysis of ozone sources over East Asia in May

Circles: observed 90th percentile MDA8

Background: GEOS-Chem

  • East Asia background ozone (originating from outside) is extremely high, prevents attainment of air quality standard
  • Even if Korea or China emissions were zeroed ozone would still approach 80 ppb

Colombi et al. [2023]

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Observing the diurnal cycle of NO2 from GEMS satellite instrument

Hourly geostationary observations inform NOx emissions, chemistry, transport

slant column density (SCD)

vertical column density (VCD)

Air mass factor

geometric correction

scattering weight (sensitivity)

vertical shape factor

NO2 VCD, 1016 molecules cm-2

Local time, hours

JJA 2021

Park et al., submitted

all depend on time of day

zT

TROPOMI

Hanlim Lee (PKNU)

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Diurnal variation of AMF driven by mixed layer growth

Ensemble of KORUS-AQ aircraft profiles over Seoul (May-June 2016)

Local time, hours

AMFG

AMF

8-9

3.09

0.38

1.19

12-13

2.42

0.46

1.11

15-16

2.77

0.46

1.27

20% diurnal variation from scattering correction factor

Yang et al. [2023]

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Variability of AMF for KORUS-AQ vertical profiles

As calculated from observed and simulated (GEOS-Chem) vertical shape factors

  • 50% variability in AMF mainly driven by land vs. ocean, time of day for land
  • Largest model error is in timing of morning mixed layer growth: difficult to get right!

Yang et al. [2023]

Error in timing of mixed layer growth

AMF error

Error in retrieved diurnal cycle

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Coarse PM trends from air quality networks, 2015-2020

  • Decreasing emissions from construction sites and road dust

Zhai et al., 2023

Coarse PM = PM10 – PM2.5

Road dust

Construction

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Coarse anthropogenic dust suppresses PM2.5 nitrate formation

NOx

HNO3

coarse NO3-

NOx emission

dust emission

PM2.5 NO3-

oxidation

uptake

  • Emitted dust particles are alkaline, take up HNO3 efficiently
  • The resulting coarse NO3- is eventually deposited

NH3 emission

Zhai et al., 2023

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Decreasing coarse PM can partly explain flat PM2.5 nitrate in winter

despite 2015-2021 NOx emission decreases of ~30% in China and Korea

Additional factors are flat ammonia emissions and increased ozone

Zhai et al. , 2023

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Work in progress

  • Ellie Beaudry: ethanol and methanol in China and South Korea as indicators of large emissions of volatile chemical products (VCPs)

  • Nadia Colombi: origin of the elevated ozone background over East Asia

  • Ruijun Dang: Satellite NH3/NO2 ratios as indicator of chemical regime for PM2.5 nitrate formation

  • Yujin Oak: blended GEMS+TROPOMI NO2 satellite product for analyzing diurnal cycles and inferring NOx emissions

  • Drew Pendergrass: intepretation of recent PM2.5 trends in Korea

  • Drew Pendergrass: updated PM2.5 mapping over East Asia from new 2x2 km2 GOCI AOD data

  • Laura Yang: Drivers of elevated methylhydroperoxide in urban air over Korea

Ellie Beaudry

Ruijun Dang

Yujin Oak

Drew Pendergrass