Global nature run data with realistic high-resolution carbon weather for the year of the Paris Agreement.

The CO2 Human Emissions project has generated realistic high-resolution 9 km global simulations for atmospheric carbon tracers referred to as nature runs to foster carbon-cycle research applications with current and planned satellite missions, as well as the surge of in situ observations. Realistic atmospheric CO2, CH4 and CO fields can provide a reference for assessing the impact of proposed designs of new satellites and in situ networks and to study atmospheric variability of the tracers modulated by the weather. The simulations spanning 2015 are based on the Copernicus Atmosphere Monitoring Service forecasts at the European Centre for Medium Range Weather Forecasts, with improvements in various model components and input data such as anthropogenic emissions, in preparation of a CO2 Monitoring and Verification Support system. The relative contribution of different emissions and natural fluxes towards observed atmospheric variability is diagnosed by additional tagged tracers in the simulations. The evaluation of such high-resolution model simulations can be used to identify model deficiencies and guide further model improvements.

Global Changes in Secondary Atmospheric Pollutants During the 2020 COVID-19 Pandemic.

We use the global Community Earth System Model to investigate the response of secondary pollutants (ozone O3, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID-19 pandemic. We quantify the respective effects of the reductions in NOx and in volatile organic carbon (VOC) emissions, which, in most cases, affect oxidants in opposite ways. Using model simulations, we show that the level of NOx has been reduced by typically 40% in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020, in good agreement with space and surface observations. We show that, relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx-saturated regions (northern China, northern Europe, and the US) during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx-controlled, the concentration of ozone decreased. SOA concentrations decrease in response to the concurrent reduction in the NOx and VOC emissions. The model also shows that atmospheric meteorological anomalies produced substantial variations in the concentrations of chemical species during the pandemic. In Europe, for example, a large fraction of the ozone increase in February 2020 was associated with meteorological anomalies, while in the North China Plain, enhanced ozone concentrations resulted primarily from reduced emissions of primary pollutants.

Diverse response of surface ozone to COVID-19 lockdown in China.

Ozone (O3) is a key oxidant and pollutant in the lower atmosphere. Significant increases in surface O3 have been reported in many cities during the COVID-19 lockdown. Here we conduct comprehensive observation and modeling analyses of surface O3 across China for periods before and during the lockdown. We find that daytime O3 decreased in the subtropical south, in contrast to increases in most other regions. Meteorological changes and emission reductions both contributed to the O3 changes, with a larger impact from the former especially in central China. The plunge in nitrogen oxide (NOx) emission contributed to O3 increases in populated regions, whereas the reduction in volatile organic compounds (VOC) contributed to O3 decreases across the country. Due to a decreasing level of NOx saturation from north to south, the emission reduction in NOx (46%) and VOC (32%) contributed to net O3 increases in north China; the opposite effects of NOx decrease (49%) and VOC decrease (24%) balanced out in central China, whereas the comparable decreases (45-55%) in these two precursors contributed to net O3 declines in south China. Our study highlights the complex dependence of O3 on its precursors and the importance of meteorology in the short-term O3 variability.

Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ.

Global coupled chemistry-climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea-United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42% in the control run and by 12% with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80% for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O3 datasets and observationally constrained box model simulations of OH and HO2. Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29% for CO, 18% for ozone, 11% for HO2, and 27% for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O3, with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NO x controls, can improve ozone pollution over East Asia.