The COVID-19 global pandemic and associated government lockdowns dramatically altered human activity, providing a window into how changes in individual behavior, enacted en masse, impact atmospheric composition. The resulting reductions in anthropogenic activity represent an unprecedented event that yields a glimpse into a future where emissions to the atmosphere are reduced. Furthermore, the abrupt reduction in emissions during the lockdown periods led to clearly observable changes in atmospheric composition, which provide direct insight into feedbacks between the Earth system and human activity. While air pollutants and greenhouse gases share many common anthropogenic sources, there is a sharp difference in the response of their atmospheric concentrations to COVID-19 emissions changes, due in large part to their different lifetimes. Here, we discuss several key takeaways from modeling and observational studies. First, despite dramatic declines in mobility and associated vehicular emissions, the atmospheric growth rates of greenhouse gases were not slowed, in part due to decreased ocean uptake of CO₂ and a likely increase in CH₄ lifetime from reduced NO_x emissions. Second, the response of O₃ to decreased NO_x emissions showed significant spatial and temporal variability, due to differing chemical regimes around the world. Finally, the overall response of atmospheric composition to emissions changes is heavily modulated by factors including carbon-cycle feedbacks to CH₄ and CO₂, background pollutant levels, the timing and location of emissions changes, and climate feedbacks on air quality, such as wildfires and the ozone climate penalty. Significance The COVID-19 pandemic and associated lockdowns caused significant changes to human activity that temporarily altered our imprint on the atmosphere, providing a brief glimpse of potential future changes in atmospheric composition. This event demonstrated key feedbacks within and between air quality and the carbon cycle: Improvements in air quality increased the lifetime of methane (an important greenhouse gas), while unusually hot weather and intense wildfires in Los Angeles drove poor air quality. This shows that efforts to reduce greenhouse gas emissions and improve air quality cannot be considered separately.

Column-averaged dry air mole fraction of atmospheric CO₂ (XCO₂), obtained by multiple satellite observations since 2003 such as ENVISAT/SCIAMACHY, GOSAT, and OCO-2 satellite, is valuable for understanding the spatio-temporal variations of atmospheric CO₂ concentrations which are related to carbon uptake and emissions. In order to construct long-term spatio-temporal continuous XCO₂ from multiple satellites with different temporal and spatial periods of observations, we developed a precision-weighted spatio-temporal kriging method for integrating and mapping multi-satellite observed XCO₂. The approach integrated XCO₂ from different sensors considering differences in vertical sensitivity, overpass time, the field of view, repeat cycle and measurement precision. We produced globally mapped XCO₂ (GM-XCO₂) with spatial/temporal resolution of 1 × 1 degree every eight days from 2003 to 2016 with corresponding data precision and interpolation uncertainty in each grid. The predicted GM-XCO₂ precision improved in most grids compared with conventional spatio-temporal kriging results, especially during the satellites overlapping period (0.3–0.5 ppm). The method showed good reliability with R² of 0.97 from cross-validation. GM-XCO₂ showed good accuracy with a standard deviation of bias from total carbon column observing network (TCCON) measurements of 1.05 ppm. This method has potential applications for integrating and mapping XCO₂ or other similar datasets observed from multiple satellite sensors. The resulting GM-XCO₂ product may be also used in different carbon cycle research applications with different precision requirements.

Methane (CH₄) is the second most important anthropogenic greenhouse gas with a significant impact on radiative forcing, tropospheric air quality, and stratospheric water vapor. Remote sensing observations enable the detection and quantification of local methane emissions across large geographical areas, which is a critical step for understanding local flux distributions and subsequently prioritizing mitigation strategies. Obtaining methane column concentration measurements with low noise and minimal surface interference has direct consequences for accurately determining the location and emission rates of methane sources. The quality of retrieved column enhancements depends on the choices of the instrument and retrieval parameters. Here, we studied the changes in precision error and bias as a result of different spectral resolutions, instrument optical performance, and detector exposure times by using a realistic instrument noise model. In addition, we formally analyzed the impact of spectrally complex surface albedo features on retrievals using the iterative maximum a posteriori differential optical absorption spectroscopy (IMAP-DOAS) algorithm. We built an end-to-end modeling framework that can simulate observed radiances from reflected solar irradiance through a simulated CH₄ plume over several natural and artificial surfaces. Our analysis shows that complex surface features can alias into retrieved methane abundances, explaining the existence of retrieval biases in current airborne methane observations. The impact can be mitigated with higher spectral resolution and a larger polynomial degree to approximate surface albedo variations. Using a spectral resolution of 1.5 nm, an exposure time of 20 ms, and a polynomial degree of 25, a retrieval precision error below 0.007 mole m⁻² or 1.0 % of total atmospheric CH₄ column can be achieved for high albedo cases, while minimizing the bias due to surface interference such that the noise is uncorrelated among various surfaces. At coarser spectral resolutions, it becomes increasingly harder to separate complex surface albedo features from atmospheric absorption features. Our modeling framework provides the basis for assessing tradeoffs for future remote sensing instruments and algorithmic designs. For instance, we find that improving the spectral resolution beyond 0.2 nm would actually decrease the retrieval precision, as detector readout noise will play an increasing role. Our work contributes towards building an enhanced monitoring system that can measure CH₄ concentration fields to determine methane sources accurately and efficiently at scale.

When retrieving Aerosol Optical Depth (AOD) from passive satellite sensors, the vertical distribution of aerosols usually needs to be assumed, potentially causing uncertainties in the retrievals. In this study, we use the Moderate Resolution Spectroradiometer (MODIS) and Visible Infrared Imaging Radiometer Suite (VIIRS) sensors as examples to investigate the impact of aerosol vertical distribution on AOD retrievals. A series of sensitivity experiments was conducted using radiative transfer models with different aerosol profiles and surface conditions. Assuming a 0.2 AOD, we found that the AOD retrieval error is the most sensitive to the vertical distribution of absorbing aerosols; a −1 km error in aerosol scale height can lead to a ~30% AOD retrieval error. Moreover, for this aerosol type, ignoring the existence of the boundary layer can further result in a ~10% AOD retrieval error. The differences in the vertical distribution of scattering and absorbing aerosols within the same column may also cause −15% (scattering aerosols above absorbing aerosols) to 15% (scattering aerosols below absorbing aerosols) errors. Surface reflectance also plays an important role in affecting the AOD retrieval error, with higher errors over brighter surfaces in general. The physical mechanism associated with the AOD retrieval errors is also discussed. Finally, by replacing the default exponential profile with the observed aerosol vertical profile by a micro-pulse lidar at the Beijing-PKU site in the VIIRS retrieval algorithm, the retrieved AOD shows a much better agreement with surface observations, with the correlation coefficient increased from 0.63 to 0.83 and bias decreased from 0.15 to 0.03. Our study highlights the importance of aerosol vertical profile assumption in satellite AOD retrievals, and indicates that considering more realistic profiles can help reduce the uncertainties.

Legislation in the State of California mandates reductions in emissions of short‐lived climate pollutants of 40% from 2013 levels by 2030 for CH₄. Identification of the sector(s) responsible for these emissions and their temporal and spatial variability is a key step in achieving these goals. Here, we determine the emissions of CH₄ in Los Angeles from 2011–2017 using a mountaintop remote sensing mapping spectrometer. We show that the pattern of CH₄ emissions contains both seasonal and nonseasonal contributions. We find that the seasonal component peaks in the winter and is correlated (R² = 0.58) with utility natural gas consumption from the residential and commercial sectors and not from the industrial and gas‐fired power plant sectors. The nonseasonal component is (22.9 ± 1.4) Gg CH₄/month. If the seasonal correlation is causal, about (1.4 ± 0.1)% of the commercial and residential natural gas consumption in Los Angeles is released into the atmosphere.