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© Author(s) 2018. The CHRONOS space mission concept provides time-resolved abundance for emissions and transport studies of the highly variable and highly uncertain air pollutants carbon monoxide and methane, with sub-hourly revisit rate at fine (-4 km) horizontal spatial resolution across a North American domain. CHRONOS can provide complete synoptic air pollution maps ("snapshots") of the continental domain with less than 10 min of observations. This rapid mapping enables visualization of air pollution transport simultaneously across the entire continent and enables a sentinel-like capability for monitoring evolving, or unanticipated, air pollution sources in multiple locations at the same time with high temporal resolution. CHRONOS uses a compact imaging gas filter correlation radiometer for these observations, with heritage from more than 17 years of scientific data and algorithm advances by the science teams for the Measurements of Pollution in the Troposphere (MOPITT) instrument on NASA's Terra spacecraft in low Earth orbit. To achieve continental-scale sub-hourly sampling, the CHRONOS mission would be conducted from geostationary orbit, with the instrument hosted on a communications or meteorological platform. CHRONOS observations would contribute to an integrated observing system for atmospheric composition using surface, suborbital and satellite data with atmospheric chemistry models, as defined by the Committee on Earth Observing Satellites. Addressing the U.S. National Academy's 2007 decadal survey direction to characterize diurnal changes in tropospheric composition, CHRONOS observations would find direct societal applications for air quality management and forecasting to protect public health.

©2017. American Geophysical Union. All Rights Reserved. Understanding changes in the burden and growth rate of atmospheric methane (CH4) has been the focus of several recent studies but still lacks scientific consensus. Here we investigate the role of decreasing anthropogenic carbon monoxide (CO) emissions since 2002 on hydroxyl radical (OH) sinks and tropospheric CH4 loss. We quantify this impact by contrasting two model simulations for 2002–2013: (1) a Measurement of the Pollution in the Troposphere (MOPITT) CO reanalysis and (2) a Control-Run without CO assimilation. These simulations are performed with the Community Atmosphere Model with Chemistry of the Community Earth System Model fully coupled chemistry climate model with prescribed CH4 surface concentrations. The assimilation of MOPITT observations constrains the global CO burden, which significantly decreased over this period by ~20%. We find that this decrease results to (a) increase in CO chemical production, (b) higher CH4 oxidation by OH, and (c) ~8% shorter CH4 lifetime. We elucidate this coupling by a surrogate mechanism for CO-OH-CH4 that is quantified from the full chemistry simulations.

We present two new products from near-infrared Greenhouse Gases Observing Satellite (GOSAT) observations: Lowermost tropospheric (LMT, from 0 to 2.5km) and upper tropospheric-stratospheric (U, above 2.5km) carbon dioxide partial column mixing ratios. We compare these new products to aircraft profiles and remote surface flask measurements and find that the seasonal and year-to-year variations in the new partial column mixing ratios significantly improve upon the Atmospheric CO2 Observations from Space (ACOS) and GOSAT (ACOS-GOSAT) initial guess and/or a priori, with distinct patterns in the LMT and U seasonal cycles that match validation data. For land monthly averages, we find errors of 1.9, 0.7, and 0.8ppm for retrieved GOSAT LMT, U, and XCO2; for ocean monthly averages, we find errors of 0.7, 0.5, and 0.5ppm for retrieved GOSAT LMT, U, and XCO2. In the southern hemispheric biomass burning season, the new partial columns show similar patterns to MODIS fire maps and MOPITT multispectral CO for both vertical levels, despite a flat ACOS-GOSAT prior, and a CO-CO2 emission factor comparable to published values. The difference of LMT and U, useful for evaluation of model transport error, has also been validated with a monthly average error of 0.8 (1.4)ppm for ocean (land). LMT is more locally influenced than U, meaning that local fluxes can now be better separated from CO2 transported from far away.

We examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers.We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12%Tg for MOPITT Reanalysis and 291 ± 9%Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime of CH4 (Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O3 and overall photochemical activity via HOx recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.

Rising emissions from wildfires over recent decades in the Pacific Northwest are known to counteract the reductions in human-produced aerosol pollution over North America. Since amplified Pacific Northwest wildfires are predicted under accelerating climate change, it is essential to understand both local and transported contributions to air pollution in North America. Here, we find corresponding increases for carbon monoxide emitted from the Pacific Northwest wildfires and observe significant impacts on both local and down-wind air pollution. Between 2002 and 2018, the Pacific Northwest atmospheric carbon monoxide abundance increased in August, while other months showed decreasing carbon monoxide, so modifying the seasonal pattern. These seasonal pattern changes extend over large regions of North America, to the Central USA and Northeast North America regions, indicating that transported wildfire pollution could potentially impact the health of millions of people., (© 2022. The Author(s).)

Top-down estimates using satellite data provide important information on the sources of air pollutants. We develop a sector-based 4D-Var framework based on the GEOS-Chem adjoint model to address the impacts of co-emissions and chemical interactions on top-down emission estimates. We apply OMI NO 2 , OMI SO 2 , and MOPITT CO observations to estimate NO x , SO 2 , and CO emissions in East Asia during 2005-2012. Posterior evaluations with surface measurements show reduced normalized mean bias (NMB) by 7% (NO 2 )-15% (SO 2 ) and normalized mean square error (NMSE) by 8% (SO 2 )-9% (NO 2 ) compared to a species-based inversion. This new inversion captures the peak years of Chinese SO 2 (2007) and NO x (2011) emissions and attributes their drivers to industry and energy activities. The CO peak in 2007 in China is driven by residential and industry emissions. In India, the inversion attributes NO x and SO 2 trends mostly to energy and CO trend to residential emissions., (© 2022. The Authors.)

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 O 3 datasets and observationally constrained box model simulations of OH and HO 2 . Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29% for CO, 18% for ozone, 11% for HO 2 , 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 O 3 , 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., Competing Interests: Competing interests. The authors declare that they have no conflict of interest.

Several viable but conflicting explanations have been proposed to explain the recent ~8 p.p.b. per year increase in atmospheric methane after 2006, equivalent to net emissions increase of ~25 Tg CH 4 per year. A concurrent increase in atmospheric ethane implicates a fossil source; a concurrent decrease in the heavy isotope content of methane points toward a biogenic source, while other studies propose a decrease in the chemical sink (OH). Here we show that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH 4 per year from the 2001-2007 to the 2008-2014 time periods using satellite measurements of CO and CH 4 , nearly twice the decrease expected from prior estimates. After updating both the total and isotopic budgets for atmospheric methane with these revised biomass burning emissions (and assuming no change to the chemical sink), we find that fossil fuels contribute between 12-19 Tg CH 4 per year to the recent atmospheric methane increase, thus reconciling the isotopic- and ethane-based results.

The 2015 fire season and related smoke pollution in Indonesia was more severe than the major 2006 episode, making it the most severe season observed by the NASA Earth Observing System satellites that go back to the early 2000s, namely active fire detections from the Terra and Aqua Moderate Resolution Imaging Spectroradiometers (MODIS), MODIS aerosol optical depth, Terra Measurement of Pollution in the Troposphere (MOPITT) carbon monoxide (CO), Aqua Atmospheric Infrared Sounder (AIRS) CO, Aura Ozone Monitoring Instrument (OMI) aerosol index, and Aura Microwave Limb Sounder (MLS) CO. The MLS CO in the upper troposphere showed a plume of pollution stretching from East Africa to the western Pacific Ocean that persisted for 2 mo. Longer-term records of airport visibility in Sumatra and Kalimantan show that 2015 ranked after 1997 and alongside 1991 and 1994 as among the worst episodes on record. Analysis of yearly dry season rainfall from the Tropical Rainfall Measurement Mission (TRMM) and rain gauges shows that, due to the continued use of fire to clear and prepare land on degraded peat, the Indonesian fire environment continues to have nonlinear sensitivity to dry conditions during prolonged periods with less than 4 mm/d of precipitation, and this sensitivity appears to have increased over Kalimantan. Without significant reforms in land use and the adoption of early warning triggers tied to precipitation forecasts, these intense fire episodes will reoccur during future droughts, usually associated with El Niño events., Competing Interests: The authors declare no conflict of interest.

Spectra measured by off-axis detectors in a high-resolution Fourier-transform spectrometer are characterized by frequency scaling, asymmetry and broadening of their line shape, and self-apodization in the corresponding interferogram. For a narrow-band input spectrum and a specified detector geometry, a formalism is presented that accounts for these effects with separate terms. Some of the terms are used to correct the larger off-axis effects as part of the calibration. The remaining terms are used to model the residual effects with the on-axis instrument line shape. We extend this approach to the broadband case using filter banks. The technique is applied to simulated spectra for the Tropospheric Emissions Spectrometer. This approach is shown to maintain a radiometric accuracy to less than 0.1%.