Isoprene is the atmosphere’s most important non-methane organic compound, with key impacts on atmospheric oxidation, ozone, and organic aerosols. In-situ isoprene measurements are sparse, and satellite-based constraints have employed an indirect approach using its oxidation product formaldehyde, which is affected by non-isoprene sources plus uncertainty and spatial smearing in the isoprene-formaldehyde relationship. Direct global isoprene measurements are therefore needed to better understand its sources, sinks, and atmospheric impacts. Here we show that the isoprene spectral signatures are detectable from space using the satellite-borne Cross-track Infrared Sounder (CrIS), develop a full-physics retrieval methodology for quantifying isoprene abundances from these spectral features, and apply the algorithm to CrIS measurements over Amazonia. The results are consistent with model output and in-situ data, and establish the feasibility of direct global space-based isoprene measurements. Finally, we demonstrate the potential for combining space-based measurements of isoprene and formaldehyde to constrain atmospheric oxidation over isoprene source regions.

Isoprene is the dominant nonmethane organic compound emitted to the atmosphere, where it drives ozone and aerosol production, modulates atmospheric oxidation, and interacts with the global nitrogen cycle. Isoprene emissions are highly variable and uncertain, as is the nonlinear chemistry coupling isoprene and its primary sink, the hydroxyl radical. Space‐based isoprene measurements can help close the gap on these uncertainties, and when combined with concurrent formaldehyde data provide a new constraint on atmospheric oxidation regimes. Here, we present a next‐generation machine‐learning isoprene retrieval for the Cross‐track Infrared Sounder (CrIS) that provides improved sensitivity, lower noise, and thus higher space‐time resolution than earlier approaches. The Retrieval of Organics from CrIS Radiances (ROCR) isoprene measurements compare well with previous space‐based retrievals as well as with the first‐ever ground‐based isoprene column measurements, with 20%–50% discrepancies that reflect differing sources of systematic uncertainty. An ensemble of sensitivity tests points to the spectral background and isoprene profile specification as the most relevant uncertainty sources in the ROCR framework. We apply the ROCR isoprene algorithm to the full CrIS record from 2012 to 2020, showing that it can resolve fine‐scale spatial gradients at daily resolution over the world's isoprene hotspots. Results over North America and Amazonia highlight emergent connections between isoprene abundance and daily‐to‐interannual variations in temperature and nitrogen oxides.

The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (O₃) can benefit from a better understanding of its source contributions in different US regions during recent years. In the Hemispheric Transport of Air Pollution experiment phase 1 (HTAP1), various global models were used to determine the O₃ source–receptor (SR) relationships among three continents in the Northern Hemisphere in 2001. In support of the HTAP phase 2 (HTAP2) experiment that studies more recent years and involves higher-resolution global models and regional models' participation, we conduct a number of regional-scale Sulfur Transport and dEposition Model (STEM) air quality base and sensitivity simulations over North America during May–June 2010. STEM's top and lateral chemical boundary conditions were downscaled from three global chemical transport models' (i.e., GEOS-Chem, RAQMS, and ECMWF C-IFS) base and sensitivity simulations in which the East Asian (EAS) anthropogenic emissions were reduced by 20 %. The mean differences between STEM surface O₃ sensitivities to the emission changes and its corresponding boundary condition model's are smaller than those among its boundary condition models, in terms of the regional/period-mean (< 10 %) and the spatial distributions. An additional STEM simulation was performed in which the boundary conditions were downscaled from a RAQMS (Realtime Air Quality Modeling System) simulation without EAS anthropogenic emissions. The scalability of O₃ sensitivities to the size of the emission perturbation is spatially varying, and the full (i.e., based on a 100 % emission reduction) source contribution obtained from linearly scaling the North American mean O₃ sensitivities to a 20 % reduction in the EAS anthropogenic emissions may be underestimated by at least 10 %. The three boundary condition models' mean O₃ sensitivities to the 20 % EAS emission perturbations are ∼ 8 % (May–June 2010)/∼ 11 % (2010 annual) lower than those estimated by eight global models, and the multi-model ensemble estimates are higher than the HTAP1 reported 2001 conditions. GEOS-Chem sensitivities indicate that the EAS anthropogenic NO_x emissions matter more than the other EAS O₃ precursors to the North American O₃, qualitatively consistent with previous adjoint sensitivity calculations. In addition to the analyses on large spatial–temporal scales relative to the HTAP1, we also show results on subcontinental and event scales that are more relevant to the US air quality management. The EAS pollution impacts are weaker during observed O₃exceedances than on all days in most US regions except over some high-terrain western US rural/remote areas. Satellite O₃ (TES, JPL–IASI, and AIRS) and carbon monoxide (TES and AIRS) products, along with surface measurements and model calculations, show that during certain episodes stratospheric O₃ intrusions and the transported EAS pollution influenced O₃ in the western and the eastern US differently. Free-running (i.e., without chemical data assimilation) global models underpredicted the transported background O₃ during these episodes, posing difficulties for STEM to accurately simulate the surface O₃ and its source contribution. Although we effectively improved the modeled O₃ by incorporating satellite O₃ (OMI and MLS) and evaluated the quality of the HTAP2 emission inventory with the Royal Netherlands Meteorological Institute–Ozone Monitoring Instrument (KNMI–OMI) nitrogen dioxide, using observations to evaluate and improve O₃ source attribution still remains to be further explored.

The second Radiative Heating in Underexplored Bands Campaign (RHUBC‐II) was conducted in 2009 by the U.S. Department of Energy Atmospheric Radiation Measurement program to improve water vapor spectroscopy in the far‐infrared spectral region. RHUBC‐II was located in an extremely dry region of Chile to ensure very low opacities in this spectral region. Spectrally resolved measurements by a far‐infrared spectrometer and a submillimeter interferometer from RHUBC‐II are compared with line‐by‐line radiative transfer model calculations. Water vapor amounts and temperatures used in the calculations come from collocated radiosondes, with extensive adjustments to correct for issues due to the campaign's dry conditions and mountainous terrain. A reanalysis is also performed of far‐infrared measurements taken at the Atmospheric Radiation Measurement North Slope of Alaska site before and during the first RHUBC campaign. These analyses determine that differences between the measurements and model calculations using existing spectroscopic parameters are significant in the far‐infrared and submillimeter regions, leading to the derivation of improved water vapor continuum absorption coefficients and air‐broadened widths of 74 water vapor lines. The foreign continuum is increased by more than 50% in part of the far‐infrared and the widths of more than 20 lines are changed by more than 10%. The uncertainty in the foreign continuum coefficients is estimated as greater than 20% in some spectral regions, primarily a consequence of the uncertainty in the specification of water vapor. The improved far‐infrared spectroscopic parameters have a notable impact on calculated spectral radiances and a modest impact on broadband radiative fluxes and heating rates.

During summer 2023 Canada experienced its most intense wildfire season on record. Smoke plumes from these fires advected across the United States (U.S.) Upper Midwest, producing regional scale surface enhancements of PM_2.5 and ozone, as recorded by the U.S. surface monitoring network. These events are notable because they occurred early in the fire season (May 15‐June 30), and they produced the highest regional‐scale surface ozone levels ever recorded across the northern tier of the U.S. during early (May–June) or late (July‐August) summer. Specifically, the Upper Midwest 50th ozone percentile was greater than in any other year since 1995, when the ozone monitoring network had sufficient coverage to assess regional‐scale ozone levels; the 90th percentile was the highest since 2002. Satellite and aircraft measurements demonstrate the availability of ozone precursors and ozone production within the smoke plumes.