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Monitoring the atmospheric concentrations of greenhouse gases (GHGs) is crucial in order to improve our understanding of their climate impact. However, there are no long-term profile data sets of important GHGs that can be used to gain a better insight into the processes controlling their variations in the atmosphere. Here, we merge chemical transport model (CTM) output and profile measurements from two solar occultation instruments, the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment - Fourier Transform Spectrometer (ACE-FTS), to construct long-term (1991-2021), gap-free stratospheric profile data sets (hereafter, TCOM) for two important GHGs. The Extreme Gradient Boosting (XGBoost) regression model is used to estimate the corrections needed to apply to the CTM profiles. For methane (TCOM-CH4), we use both HALOE and ACE satellite profile measurements (1992-2018) to train the XGBoost model while profiles from three later years (2019-2021) are used as an independent evaluation data set. As there are no nitrous oxide (N2O) profile mea10 surements for earlier years, XGBoost-derived correction terms to construct TCOM-N2O profiles are derived using only ACEFTS profiles for the 2004-2018 time period, with profiles from 2019-2021 again being used for the independent evaluation. Overall, both TCOM-CH4 and TCOM-N2O profiles show excellent agreement with the available satellite measurement-based data sets. We find that compared to evaluation profiles, biases in TCOM-CH4 and TCOM-N2O are generally less than 10% and 50%, respectively, throughout the stratosphere. Daily zonal mean profile data sets on altitude (15-60 km) and pressure (300-0.1 hPa) levels are publicly available via https://doi.org/10.5281/zenodo.7293740 for TCOM-CH4 (Dhomse, 2022a) and https://doi.org/10.5281/zenodo.7386001 for TCOM-N2O (Dhomse, 2022b). [ABSTRACT FROM AUTHOR]

We report the recovery and re-calibration of an extensive dataset of vertical profile measurements of the 1963/64 stratospheric aerosol layer measured from a two-site searchlight measurement facility at White Sands missile base and Sacramento Peak observatory, in New Mexico, US. The recovered dataset comprises 105 profiles of 550nm aerosol extinction (βp(z)) and is part of a longer program of measurements with the US Air Force Cambridge Research Laboratories (AFCRL) searchlight facility that began in February 1963. The recovered series of βp(z) profiles span the 13-month period December 1963 to December 1964 and provide a unique record of the altitude and vertical extent of the Northern Hemisphere dispersed portion of the aerosol cloud from the March 1963 Agung volcanic eruption. The data recovery methodology involved first re-digitizing the 105 original βp(z) profiles (βp(z)) from individual Figures within an AFCRL research report (Elterman, 1966a). The re-calibration involves inverting the original equation used to compute βp(z) in Elterman (1966a; 1966b) to retrieve a normalized detector response (Er(z) Er(35)) profile for each of the 105 re-digitized βp 0(z) profiles. An iterative procedure was then used to compute the re-calibration βp(z) profiles (βp Ra(z)), with the molecular extinction profile calculated with the corresponding daily molecular extinction profile calculated from local soundings, rather than the US Standard Atmosphere 1962 in the original dataset. Two-way molecular and aerosol transmittance corrections are applied using the MODTRAN (MODerate resolution atmospheric TRANsmission) code in transmission mode, applying a best-estimate aerosol phase function calculated from measurements, applied for the entire 2.76 to 35.2 km column. For the tropospheric aerosol transmittance, the AERONET aerosol phase function from White Sands High Energy Laser Systems Test Facility (HELSTF) was applied (2.76 to 10.7 km), a separate stratospheric phase function applied between 11.2 and 35.2 km, calculated from a set of particle size distributions measured by the U-2 high-altitude aircraft over a US region in the vicinity of White Sands in early 1964. Errors were estimated taking as a reference the errors determined in the computation of βp 0(z). Using available tabulated data from the original procedure the errors in the re-digitalization of βp 0(z) and in the retrieval of the Er(z) Er(35) procedures were calculated and later added to the original estimates. Both the βp R(z) and the stratospheric aerosol optical depth magnitudes showed higher magnitudes than βp 0(z) and the original stratospheric aerosol optical depth, however their magnitudes show a reasonable agreement with other contemporary observations. Both the original and recalibration datasets are being submitted to PANGAEA data repository for its storage and public access. [ABSTRACT FROM AUTHOR]

High quality stratospheric ozone profile datasets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments obtain stratospheric ozone profile measurements over typical mission durations of 5-15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create longer term observation-based ozone profile datasets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different datasets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a Random-Forest (RF) ensemble learning method to create a merged 42-year (1979-2020) stratospheric ozone profile dataset (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gas, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) dataset over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991-1998) and Aura (2005-2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based datasets which use pressure as the vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the datasets which are height-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties in the observational datasets. The ML-TOMCAT dataset is thus ideally suited for the evaluation of model ozone profiles from the tropopause to 0.1 hPa. ML-TOMCAT data is freely available via https://zenodo.org/record/4997959#.YNzleUlKiUk (Dhomse et al., 2021). [ABSTRACT FROM AUTHOR]

An updated and improved version of a global, vertically resolved, monthly mean zonal mean ozone database has been calculated - hereafter referred to as the BSVertOzone database. Like its predecessor, it combines measurements from several satellite-based instruments and ozone profile measurements from the global ozonesonde network. Monthly mean zonal mean ozone concentrations in mixing ratio and number density are provided in 5° latitude bins, spanning 70 altitude levels (1 to 70km), or 70 pressure levels that are approximately 1km apart (878.4hPa to 0.046hPa). Different data sets or "Tiers" are provided: "Tier 0" is based only on the available measurements and therefore does not completely cover the whole globe or the full vertical range uniformly; the "Tier 0.5" monthly mean zonal means are calculated as a filled version of the Tier 0 database where missing monthly mean zonal mean values are estimated from correlations against a total column ozone database. The Tier 0.5 data set includes the full range of measurement variability and is created as an intermediate step for the calculation of the "Tier 1" data where a least squares regression model is used to attribute variability to various known forcing factors for ozone. Regression model fit coefficients are expanded in Fourier series and Legendre polynomials (to account for seasonality and latitudinal structure, respectively). Four different combinations of contributions from selected regression model basis functions result in four different "Tier 1" data sets that can be used for comparisons with chemistry-climate model simulations that do not exhibit the same unforced variability as reality (unless they are nudged towards reanalyses). Compared to previous versions of the database, this update includes additional satellite data sources and ozonesonde measurements to extend the database period to 2016. Additional improvements over the previous version of the database include: (i) Adjustments of measurements to account for biases and drifts between different data sources (using a chemistry-transport model simulation as a transfer standard), (ii) a more objective way to determine the optimum number of Fourier and Legendre expansions for the basis function fit coefficients, and (iii) the derivation of methodological and measurement uncertainties on each database value are traced through all data modification steps. Comparisons with the ozone database from SWOOSH (Stratospheric Water and OzOne Satellite Homogenized data set) show good agreement in many regions of the globe. Minor differences are caused by different bias adjustment procedures for the two databases. However, compared to SWOOSH, BSVertOzone additionally covers the troposphere. [ABSTRACT FROM AUTHOR]