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Top-down observational constraints on emissions flux estimates from satellite observations of chemical composition are subject to biases and errors stemming from transport, chemistry and prior emissions estimates. In this context, we developed an ensemble data assimilation system to optimize the initial conditions for carbon monoxide (CO) and aerosols, while also quantifying the respective emission fluxes with a distinct attribution of anthropogenic and wildfire sources. We present the separate assimilation of CO profile v9 retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument and Aerosol Optical Depth (AOD), collection 6.1, from the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. This assimilation system is built on the Data Assimilation Research Testbed (DART) and includes a meteorological ensemble to assimilate weather observations within the online Community Atmosphere Model with Chemistry (CAM-chem). Inversions indicate an underestimation of CO emissions in CAMS-GLOB-ANT_v5.1 in China for 2015 and an overestimation of CO emissions in the Fire INventory from NCAR (FINN) version 2.2, especially in the tropics. These emissions increments are consistent between the MODIS AOD and the MOPITT CO-based inversions. Additional simulations and comparison with in situ observations from the NASA Atmospheric Tomography Mission (ATom) show that biases in hydroxyl radical (OH) chemistry dominate the CO errors.

Nitrous oxide (N2O) is the third most abundant anthropogenous greenhouse gas (after carbon dioxide and methane), with a long atmospheric lifetime and a continuously increasing concentration due to human activities, making it an important gas to monitor. In this work, we present a new method to retrieve N2O concentration profiles (with up to two degrees of freedom) from each cloud-free satellite observation by the Infrared Atmospheric Sounding Interferometer (IASI), using spectral micro-windows in the N2O ν3 band, the Radiative Transfer for TOVS (RTTOV) tools and the Tikhonov regularization scheme. A time series of ten years (2011–2020) of IASI N2O profiles and integrated partial columns has been produced and validated with collocated ground-based Network for the Detection of Atmospheric Composition Change (NDACC) and Total Carbon Column Observing Network (TCCON) data. The importance of consistency in the ancillary data used for the retrieval for generating consistent time series has been demonstrated. The Nitrous Oxide Profiling from Infrared Radiances (NOPIR) N2O partial columns are of very good quality, with a positive bias of 1.8 to 4% with respect to the ground-based data, which is less than the sum of uncertainties of the compared values. At high latitudes, the comparisons are a bit worse, due to either a known bias in the ground-based data, or to a higher uncertainty in both ground-based and satellite retrievals.

Boreal fires have increased during the last years and are projected to become more intense and frequent as a consequence of climate change. Wildfires produce a wide range of effects on the Arctic climate and ecosystem, and understanding these effects is crucial for predicting the future evolution of the Arctic region. This study focuses on the impact of the long-range transport of biomass-burning aerosol into the atmosphere and the corresponding radiative perturbation in the shortwave frequency range. As a case study, we investigate an intense biomass-burning (BB) event which took place in summer 2017 in Canada and subsequent northeastward transport of gases and particles in the plume leading to exceptionally high values (0.86) of Aerosol Optical Depth (AOD) at 500 nm measured in northwestern Greenland on 21 August 2017. This work characterizes the BB plume measured at the Thule High Arctic Atmospheric Observatory (THAAO; 76.53∘N, 68.74∘W) in August 2017 by assessing the associated shortwave aerosol direct radiative impact over the THAAO and extending this evaluation over the broader region (60∘N–80∘N, 110∘W–0∘E). The radiative transfer simulations with MODTRAN6.0 estimated an aerosol heating rate of up to 0.5 K/day in the upper aerosol layer (8–12 km). The direct aerosol radiative effect (ARE) vertical profile shows a maximum negative value of −45.4 Wm−2 for a 78∘ solar zenith angle above THAAO at 3 km altitude. A cumulative surface ARE of −127.5 TW is estimated to have occurred on 21 August 2017 over a portion (∼3.1×106 km2) of the considered domain (60∘N–80∘N, 110∘W–0∘E). ARE regional mean daily values over the same portion of the domain vary between −65 and −25 Wm−2. Although this is a limited temporal event, this effect can have significant influence on the Arctic radiative budget, especially in the anticipated scenario of increasing wildfires.

From the earliest observations of ozone in the lower atmosphere in the 19th century, both measurement methods and the portion of the globe observed have evolved and changed. These methods have different uncertainties and biases, and the data records differ with respect to coverage (space and time), information content, and representativeness. In this study, various ozone measurement methods and ozone datasets are reviewed and selected for inclusion in the historical record of background ozone levels, based on relationship of the measurement technique to the modern UV absorption standard, absence of interfering pollutants, representativeness of the well-mixed boundary layer and expert judgement of their credibility. There are significant uncertainties with the 19th and early 20th-century measurements related to interference of other gases. Spectroscopic methods applied before 1960 have likely underestimated ozone by as much as 11% at the surface and by about 24% in the free troposphere, due to the use of differing ozone absorption coefficients. There is no unambiguous evidence in the measurement record back to 1896 that typical mid-latitude background surface ozone values were below about 20 nmol mol–1, but there is robust evidence for increases in the temperate and polar regions of the northern hemisphere of 30–70%, with large uncertainty, between the period of historic observations, 1896–1975, and the modern period (1990–2014). Independent historical observations from balloons and aircraft indicate similar changes in the free troposphere. Changes in the southern hemisphere are much less. Regional representativeness of the available observations remains a potential source of large errors, which are difficult to quantify. The great majority of validation and intercomparison studies of free tropospheric ozone measurement methods use ECC ozonesondes as reference. Compared to UV-absorption measurements they show a modest (~1–5% ±5%) high bias in the troposphere, but no evidence of a change with time. Umkehr, lidar, and FTIR methods all show modest low biases relative to ECCs, and so, using ECC sondes as a transfer standard, all appear to agree to within one standard deviation with the modern UV-absorption standard. Other sonde types show an increase of 5–20% in sensitivity to tropospheric ozone from 1970–1995. Biases and standard deviations of satellite retrieval comparisons are often 2–3 times larger than those of other free tropospheric measurements. The lack of information on temporal changes of bias for satellite measurements of tropospheric ozone is an area of concern for long-term trend studies.