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Frederick D’Aragon,1,2 Olivier Lachance,1 Vincent Lafleur,1 Ivan Ortega-Deballon,3,4 Marie-Helene Masse,5 Gabrielle Trepanier,6 Daphnee Lamarche,1 Marie-Claude Battista5 1Department of Anesthesiology, Faculty of Medicine and Health Sciences Université de Sherbrooke, Sherbrooke, Quebec, Canada; 2Centre de recherche du Centre hospitalier universitaire de Sherbrooke, Sherbrooke, Quebec, Canada; 3Nursing Department, Faculty of Medicine and Health Sciences, Universidad de Alcalá, Madrid, Spain; 4Helicopter & Nursing Care Unit, Emergency Medical Service SUMMA 112, Madrid, Spain; 5Department of Medicine, Faculty of Medicine and Health Sciences, Université de Sherbrooke, Sherbrooke, Quebec, Canada; 6Department of Family Medicine and Emergency, Faculty of Medicine and Health Sciences, Université de Sherbrooke, Sherbrooke, Quebec, CanadaCorrespondence: Frederick D’Aragon, 3001 12e Avenue N, Sherbrooke, PQ, J1H 5N4, Canada, Tel +1 819 821-8000 ext. 70103, Email Frederick.D’Aragon@USherbrooke.caPurpose: Worldwide, the number of patients waiting for organ transplantation exceeds the number of organs available. Program for uncontrolled donation after circulatory death (uDCD) implemented in Europe has resulted in a 10– 15% expansion of the donor pool. We aimed to describe the number of patients eligible for an uDCD program in a regional tertiary care center.Methods: We conducted a retrospective cohort study in a Canadian tertiary academic center located in a rural area including all adults who received cardiopulmonary resuscitation in 2016 and died in the emergency department (ED) or during their hospitalization. The primary outcome was the number of patients eligible for uDCD defined as aged between 18 and 60 years old whose collapse was witnessed and where the time between cardiac arrest to cardiopulmonary resuscitation and ED arrival was, respectively, less than 30 and 120 minutes. As a secondary outcome, we determined the number of patients eligible for controlled donation after circulatory death.Results: Of the 130 patients included, 84 did not return to spontaneous circulation. We identified 15 potential uDCD candidates, with a mean age of 46.6 (95% Confidence Interval [CI] 41.3 to 52) years. Twelve had an out-of-hospital cardiac arrest with a mean time between collapse and arrival to the ED of 43.2 (29.8 to 56.6) minutes. Among the 46 patients who died after a return of spontaneous circulation, 10 (21.7%) were eligible for organ donation after circulatory death.Conclusion: Implementing an uDCD program in a tertiary hospital covering a rural area could increase the number of donors.Keywords: tissue and organ procurement, out-of-hospital cardiac arrest, donor selection, death, uncontrolled donation after circulatory death

Over the last 20 years, low-Earth orbit (LEO) atmospheric composition observations have provided amazing satellite measurements of atmospheric pollutants, mainly at continental-to-global, weekly-to-seasonal scales. The new-generation geostationary (GEO) satellite perspective, with high spatial resolution and hourly measurements, represents a major step forward in capability for understanding how air quality processes change diurnally at the local scale. South Korea's Geostationary Environment Monitoring Spectrometer (GEMS) was launched in February 2020 over Asia and is the first member of the GEO constellation that will eventually include the Tropospheric Emissions: Monitoring Pollution (TEMPO) mission over North America, and Sentinal-4 over Europe. The measurement hourly time resolution is truly the new perspective that the GEO platform provides, and in this presentation, we use a combination of satellite observations from GEMS and chemical transport model simulations to investigate the diurnal variation of pollution over several Asian regions. When considering the GEMS whole-Asia field-of-regard, the most striking impression of the NO2 diurnal variation is of how large it is in magnitude as well as how much the spatial distribution changes hour-by-hour. This questions our understanding of the distributions of reactive species based on the representativeness of once-a-day LEO observations. To help understand daily differences in diurnal patterns at regional and local scales, we use the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA-V0). This uses a global modeling framework with regional grid refinement to resolve chemistry at emission and exposure relevant scales. The model shows reasonable agreement with the GEMS data and captures the different diurnal patterns at the different spatial scales and the degree of day-to day variability. The model also allows the drivers of variability due to emissions, meteorology, and photochemistry to be considered separately. The results of this analysis are further compared with the NO2 diurnal variability observed by PANDORA sun spectrometer measurements at polluted and less-polluted Korean and other Asian sites. We investigate spatial scale, including the city-scale within Seoul, at which GEMS captures the differences in diurnal variability between the PANDORAs.

Ground-based observations are indispensable for the long-term monitoring of atmospheric constituents. In this work, we take advantage of multiple collocated instruments to analyze potential biases and drifts in ground-based ozone observations, within the context of the HEGIFTOM (Harmonization and Evaluation of Ground-based Instruments for Free Tropospheric Ozone Measurements) working group in the Tropospheric Ozone Assessment Report, Phase II (TOAR-II). This work is performed at Lauder (New Zealand), Boulder (Colorado), and Mauna Loa (Hawaii) where comparisons are made between Fourier Transform Infrared (FTIR) spectroscopy, Dobson Umkehr, and ozonesonde observations. The validation is performed with respect to FTIR as arbitrary reference, while considering the differences between the a priori profile information for the techniques that employ these as well as accounting for the different vertical resolution of each measurement technique. Such intercomparison is done for a handful discrete altitude partial columns, defined to have independent pieces of information also in the case of the low vertical resolution techniques (FTIR and Umkehr). This leads to 4 independent vertical layers to be compared, including one in the troposphere where ozone plays an important role as a greenhouse gas and as a risk to human health. In this tropospheric layer we compare the FTIR, Dobson Umkehr and ozonesonde techniques and derive a consistent bias from the FTIR data of about 5%, which we attribute in part to the assumed spectroscopy. Fitting the time series of the relative measurement differences using multiple linear regression, we obtain a linear trend, which quantifies the drift between pairs of techniques. Within the uncertainties, we find no significant drift between FTIR and Umkehr or ozone sonde data in the troposphere.

Anomalies of tropospheric columns of ozone (O$_3$), carbon monoxide (CO), acetylene (C$_2$H$_2$), formaldehyde (H$_2$CO), and ethane (C$_2$H$_6$) are quantified during the 2020 stringent COVID-19 world-wide lockdown using multiple ground-based Fourier-transform infrared spectrometers covering urban and remote conditions. We applied an exponential smoothing forecasting approach to the data sets to estimate business-as-usual values for 2020, which are then contrasted with actual observations. The Community Atmosphere Model with chemistry (CAM-chem) is used to simulate the same gases using lockdown-adjusted and business-as-usual emissions. The role of meteorology, or natural variability, is assessed with additional CAM-chem simulations. The tropospheric column of O$_3$ declined between March and May 2020 for most sites with a mean decrease of 9.2% ± 4.7%. Simulations reproduce these anomalies, especially under background conditions where natural variability explains up to 80% of the decline for sites in the Northern Hemisphere. While urban sites show a reduction between 1% and 12% in tropospheric CO, the remote sites do not show a significant change. Overall, CAM-chem simulations capture the magnitude of the anomalies and in many cases natural variability and lockdowns have opposite effects. We further used the long-term record of the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument to capture global anomalies of CO. Reductions of CO vary highly across regions but North America and Europe registered lower values in March 2020. The absence of CO reduction in April and May, concomitant with reductions of anthropogenic emissions, is explained by a negative anomaly in the hydroxyl radical (OH) found with CAM-chem. The implications of these findings are discussed for methane (CH$_4$), which shows a positive lifetime anomaly during the COVID-19 lockdown period. The fossil fuel combustion by-product tracer C2H2 shows a mean drop of 13.6% ± 8.3% in urban Northern Hemisphere sites due to the reduction in emissions and in some sites exacerbated by natural variability. For some sites with anthropogenic influence there is a decrease in C$_2$H$_6$. The simulations capture the anomalies but the main cause may be related to natural variability. H$_2$CO declined during the stringent 2020 lockdown in all urban sites explained by reductions in emissions of precursors.

Este artículo presenta el cálculo, diseño, simulación y validación de los componentes estructurales del prototipo de la aeronave liviana CVAC-001 categoría VLA para uso en aspersión aérea. La reglamentación establecida por la EASA-ADOA (Alternative Design Organization Approval) se definió en el proyecto como modelo de diseño del prototipo de la aeronave para lograr su garantía o aseguramiento. Para el proceso de cálculo, diseño, simulación y validación de los componentes estructurales, se escogieron dos lados de la cuaderna de carga y el conjunto de los tres componentes que la conforman. La simulación por elementos finitos para el estudio estático de esfuerzos, pandeo y los ensayos de validación de la cuaderna de carga permiten concluir que para los componentes analizados se cumple el criterio de factibilidad de diseño. This paper presents the calculation, design, simulation, and validation of structural components of the light aircraft prototype CVAC-001 category VLA for use in aerial spraying. The regulation established by the EASAADOA (Alternative Design Organization Approval) was defined in the project as an aircraft design model to achieve its guarantee or assurance. For the calculation, design, simulation, and validation process of the structural components, two sides of the load frame and the set of three components that make it up were chosen. The finite element simulation for the static study of stress and buckling and the validation tests of the load frame allows us to conclude that the design feasibility criterion is met for the analyzed components

Calciphylaxis is a serious disorder that presents itself as ischemia and ne-crosis of the skin which occurs more frequently in patients with an end-stage chronic kidney disease, but not exclusively. The pathogenesis is a result of the reduction of arteriolar blood flow, caused by calcification, fibrosis, and thrombus formation that primarily involve the arterioles of the dermis and hypodermis, with a poor prognosis. Case presentation: A 44-year-old patient with a previous diagnosis of chronic kidney disease receiving hemodialysis secondary to polycystic kidney disease, with a history of parathyroidectomy due to primary hyperparathyroidism in 2011. In 2014 the patient presented skin lesions, for which a diagnostic biopsy of calciphylaxis was performed and began treatment with sodium thiosulfate with a poor progression and evolution. New histology compatible with the diagnosis of pyoderma gangrenosum and findings of calciphylaxis were performed. The patient begins treatment with corticosteroids and cyclosporine, with poor clinical evolution and the patient eventually passes away. The objective of this manuscript is to understand this pathology better, which is infrequent but with a high rate of morbidity and mortality.

We present a multiyear time series of column abundances of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier-transform infrared (FTIR) spectrometers at 10 sites affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC). Six are high-latitude sites: Eureka, Ny-Ålesund, Thule, Kiruna, Poker Flat, and St. Petersburg, and four are midlatitude sites: Zugspitze, Jungfraujoch, Toronto, and Rikubetsu. For each site, the interannual trends and seasonal variabilities of the CO time series are accounted for, allowing background column amounts to be determined. Enhancements above the seasonal background were used to identify possible wildfire pollution events. Since the abundance of each trace gas emitted in a wildfire event is specific to the type of vegetation burned and the burning phase, correlations of CO to the long-lived wildfire tracers HCN and C2H6 allow for further confirmation of the detection of wildfire pollution. A GEOS-Chem tagged CO simulation with Global Fire Assimilation System (GFASv1.2) biomass burning emissions was used to determine the source attribution of CO concentrations at each site from 2003 to 2018. For each detected wildfire pollution event, FLEXPART back-trajectory simulations were performed to determine the transport times of the smoke plume. Accounting for the loss of each species during transport, the enhancement ratios of HCN and C2H6 with respect to CO were converted to emission ratios. We report mean emission ratios with respect to CO for HCN and C2H6 of 0.0047 and 0.0092, respectively, with a standard deviation of 0.0014 and 0.0046, respectively, determined from 23 boreal North American wildfire events. Similarly, we report mean emission ratios for HCN and C2H6 of 0.0049 and 0.0100, respectively, with a standard deviation of 0.0025 and 0.0042, respectively, determined from 39 boreal Asian wildfire events. The agreement of our emission ratios with literature values illustrates the capability of ground-based FTIR measurements to quantify biomass burning emissions. We provide a comprehensive dataset that quantifies HCN and C2H6 emission ratios from 62 wildfire pollution events. Our dataset provides novel emission ratio estimates, which are sparsely available in the published literature, particularly for boreal Asian sources.

Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and a large sulfur reservoir maintained by both direct oceanic, geologic, biogenic, and anthropogenic emissions and the oxidation of other sulfur-containing source species. It is the largest source of sulfur transported to the stratosphere during volcanically quiescent periods. Data from 22 ground-based globally dispersed stations are used to derive trends in total and partial column OCS. Middle infrared spectral data are recorded by solar-viewing Fourier transform interferometers that are operated as part of the Network for the Detection of Atmospheric Composition Change between 1986 and 2020. Vertical information in the retrieved profiles provides analysis of discreet altitudinal regions. Trends are found to have well-defined inflection points. NASA | Science Mission Directorate (SMD). Grant Numbers: NNX17AE38 G S003, 80NSSC21K0891. Natural Sciences and Engineering Research Council of Canada (NSERC); the Canadian Space Agency (CSA); Environment and Climate Change Canada (ECCC); Sorbonne Université; French Research Center CNRS; French Space Agency CNES. F.R.S.-FNRS. Grant Numbers: J.0147.18, J.0126.21. CONACYT. Grant Number: 290589. PAPIIT. Grant Number: IN111521. NIWA; New Zealand’s Ministry of Business, Innovation and Employment Strategic Science Investment Fund German research foundation. Grant Number: 268020496 German Bundesministerium für Wirtschaft und Energie (BMWi). Grant Numbers: 50EE1711A, 50EE1711D. Helmholtz Society Australian Research Council. Université de La Réunion. Grant Numbers: LACy-UMR8105, UMS3365.

Carbonyl sulfide (OCS) is a non-hygroscopic trace species in the free troposphere and the primary sulfur reservoir maintained by direct oceanic, geologic, biogenic and anthropogenic emissions and t...

We use the global Community Earth System Model to investigate the response of secondary pollutants (ozone O3, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID‐19 pandemic. We quantify the respective effects of the reductions in anthropogenic emissions and meteorological anomalies, including a discussion on long-term changes from the chemical climatology. We show that the level of NOx has been reduced by typically 40 % in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020. Relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx‐saturated regions during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx‐controlled, the concentration of ozone decreased. Zonally averaged ozone concentrations in the free troposphere during Northern Hemisphere spring and summer were 5 to 15 % lower than 19-year climatological values, in good quantitative agreement with observations from ozonesondes and ground-based remote sensing from the Network for the Detection of Atmospheric Composition Change (NDACC). About one third of this anomaly is attributed to the drastic reduction in air traffic during the pandemic, another third to reductions in surface emissions, the remainder to 2020 meteorological conditions, including the exceptional springtime Arctic stratospheric ozone depletion. The overall COVID-19 reduction in mean northern hemisphere tropospheric ozone in June is less than 5 ppb below 400 hPa, but reaches 8 ppb at 250 hPa.

Extended and intense wildfires occurred in Northern Canada and, unexpectedly, on the Greenlandic West coast during summer 2017. The thick smoke plume emitted into the atmosphere was transported to the high Arctic, producing one of the largest impacts ever observed in the region. Evidence of Canadian and Greenlandic wildfires was recorded at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5°N, 68.8°W, www.thuleatmos-it.it) by a suite of instruments managed by ENEA, INGV, Univ. of Florence, and NCAR. Ground-based observations of the radiation budget have allowed quantification of the surface radiative forcing at THAAO. Excess biomass burning chemical tracers such as CO, HCN, H2CO, C2H6, and NH3 were measured in the air column above Thule starting from August 19 until August 23. The aerosol optical depth (AOD) reached a peak value of about 0.9 on August 21, while an enhancement of wildfire compounds was detected in PM10. The measured shortwave radiative forcing was -36.7 W/m2 at 78° solar zenith angle (SZA) for AOD=0.626.MODTRAN6.0 radiative transfer model (Berk et al., 2014) was used to estimate the aerosol radiative effect and the heating rate profiles at 78° SZA. Measured temperature profiles, integrated water vapour, surface albedo, spectral AOD and aerosol extinction profiles from CALIOP onboard CALIPSO were used as model input. The peak aerosol heating rate (+0.5 K/day) was reached within the aerosol layer between 8 and 12 km, while the maximum radiative effect (-45.4 W/m2) is found at 3 km, below the largest aerosol layer.The regional impact of the event that occurred on August 21 was investigated using a combination of atmospheric radiative transfer modelling with measurements of AOD and ground surface albedo from MODIS. The aerosol properties used in the radiative transfer model were constrained by in situ measurements from THAAO. Albedo data over the ocean have been obtained from Jin et al. (2004). Backward trajectories produced through HYSPLIT simulations (Stein et al., 2015) were also employed to trace biomass burning plumes.The radiative forcing efficiency (RFE) over land and ocean was derived, finding values spanning from -3 W/m2 to -132 W/m2, depending on surface albedo and solar zenith angle. The fire plume covered a vast portion of the Arctic, with large values of the daily shortwave RF (< -50 W/m2) lasting for a few days. This large amount of aerosol is expected to influence cloud properties in the Arctic, producing significant indirect radiative effects.

The Sentinel-5 Precursor (S5P) mission with the TROPOspheric Monitoring Instrument (TROPOMI) onboard has been measuring solar radiation backscattered by the Earth's atmosphere and its surface since its launch on 13 October 2017. Methane (CH4) and carbon monoxide (CO) data with a spatial resolution (initially 7 x 7 km2, upgraded to 5.5 x 7 km2 on 6th of August 2019) have been retrieved from shortwave infrared (SWIR) and near-infrared (NIR) measurements since the end of November 2017 and made available to the experts for early validation and quality checks before the official product release. In this paper, we present for the first time the S5P CH4 and CO validation results (covering a period from November 2017 to September 2020) using global Total Carbon Column Observing Network (TCCON) and Infrared Working Group of the Network for the Detection of Atmospheric Composition Change (NDACC-IRWG) network data, accounting for a priori alignment and smoothing uncertainties in the validation, and testing the sensitivity of validation results towards the application of advanced co-location criteria.We found that the required bias (systematic error) of 1.5 % and random error of 1 % for the S5P standard and bias-corrected methane data are met for measurements over land surfaces with pixels having quality assurance (QA) value > 0.5. The systematic difference between the S5P standard XCH4 and TCCON data is on average −0.69 ± 0.73 %. The systematic difference changes to a value of −0.25 ± 0.57 % for the S5P bias-corrected XCH4 data. We found a correlation of above 0.6 for most stations, which is mostly dominated by the seasonal cycle. The contributions of smoothing uncertainty at the individual stations are estimated and found to be dependent on the location. The highest contribution of the smoothing uncertainty is observed for mid-latitude TCCON stations and high latitude stations for NDACC. A seasonal dependency of the relative bias is seen. We observe a high bias during the springtime measurements at high SZA and a decreasing bias with increasing SZA for the rest of the year.We found that the required bias (systematic error) of 15 % and random error of < 10 % for the S5P carbon monoxide data are met in general for measurements over all surfaces with pixels having quality assurance value of > 0.5. There are a few stations where this is not the case, mostly due to co-location mismatches and the limited availability of co-located data. We compared the S5P XCO data with respect to standard TCCON XCO and unscaled TCCON XCO (without application of the empirical scaling factor) data sets. The systematic difference between the S5P XCO and the TCCON data is on average 9.14 ± 3.33 % (standard TCCON XCO data) and 2.36 ± 3.22 % (unscaled TCCON XCO data). We found that the systematic difference between the S5P CO column and NDACC CO column data (excluding two stations that were obvious outliers) is on average 6.44 ± 3.79 %. We found a correlation of above 0.9 for most TCCON and NDACC stations indicating that the temporal variations in CO column captured by the ground-based instruments are reproduced very similarly by the S5P CO column. The contribution of smoothing uncertainty at the individual stations is estimated and found to be significant. They are found to be dependent on the location with large changes seen for stations located in the Southern Hemisphere as compared to the Northern Hemisphere and at highly polluted stations. A cone co-location criterion, which gives a better match between the ground-based instrument's line-of-sight and satellite pixels, seems to give better results for high latitude stations and stations located close to emission sources. The validation results for the clear-sky and cloud cases of S5P pixels are comparable to the validation results including all pixels with quality assurance value of > 0.5. We observe that the relative bias increases with increasing SZA. We estimated this increase is about 10 % over the complete range of measurement SZAs.The study shows the high quality of S5P CH4 and CO data by validating the products against reference global TCCON and NDACC stations covering a wide range of latitudinal bands, atmospheric conditions, and surface conditions.

Although optical components in Fourier transform infrared (FTIR) spectrometers are preferably wedged, in practice, infrared spectra typically suffer from the effects of optical resonances (“channeling”) affecting the retrieval of weakly absorbing gases. This study investigates the level of channeling of each FTIR spectrometer within the Network for the Detection of Atmospheric Composition Change (NDACC). Dedicated spectra were recorded by more than twenty NDACC FTIR spectrometers using a laboratory mid-infrared source and two detectors. In the InSb detector domain (1900–5000 cm−1), we find that the amplitude of the most pronounced channeling frequency amounts to 0.1 to 2.0 ‰ of the spectral background level, with a mean of (0.68 ± 0.48) ‰ and a median of 0.60 ‰. In the HgCdTe detector domain (700–1300 cm−1), we find even stronger effects, with the largest amplitude ranging from 0.3 to 21 ‰ with a mean of (2.45 ± 4.50) ‰ and a median of 1.2 ‰. For both detectors, the leading channeling frequencies are 0.9 and 0.11 or 0.23 cm−1 in most spectrometers. These observed spectral frequencies correspond to the optical thickness of the air gap in between the beam splitter and compensator plate (0.9 cm−1) and the beam splitter substrate itself (0.11 and 0.23 cm−1). Since the air gap is a significant source of channeling and the corresponding amplitude differs strongly between spectrometers, we propose new beam splitters with the wedge of the air gap increased to at least 0.8°. We tested the insertion of spacers in a beam splitter’s air gap to demonstrate that increasing the wedge of the air gap decreases the 0.9 cm−1 channeling amplitude significantly. This study shows the potential for reducing channeling in the FTIR spectrometers operated by the NDACC, thereby increasing the quality of recorded spectra across the network.

Emissions of C 2 -C 5 alkanes from the U.S. oil and gas sector have changed rapidly over the last decade. We use a nested GEOS-Chem simulation driven by updated 2011NEI emissions with aircraft, surface, and column observations to (1) examine spatial patterns in the emissions and observed atmospheric abundances of C 2 -C 5 alkanes over the United States and (2) estimate the contribution of emissions from the U.S. oil and gas industry to these patterns. The oil and gas sector in the updated 2011NEI contributes over 80% of the total U.S. emissions of ethane (C 2 H 6 ) and propane (C 3 H 8 ), and emissions of these species are largest in the central United States. Observed mixing ratios of C 2 -C 5 alkanes show enhancements over the central United States below 2 km. A nested GEOS-Chem simulation underpredicts observed C 3 H 8 mixing ratios in the boundary layer over several U.S. regions, and the relative underprediction is not consistent, suggesting C 3 H 8 emissions should receive more attention moving forward. Our decision to consider only C 4 -C 5 alkane emissions as a single lumped species produces a geographic distribution similar to observations. Due to the increasing importance of oil and gas emissions in the United States, we recommend continued support of existing long-term measurements of C 2 -C 5 alkanes. We suggest additional monitoring of C 2 -C 5 alkanes downwind of northeastern Colorado, Wyoming, and western North Dakota to capture changes in these regions. The atmospheric chemistry modeling community should also evaluate whether chemical mechanisms that lump larger alkanes are sufficient to understand air quality issues in regions with large emissions of these species., SCOPUS: ar.j, info:eu-repo/semantics/published

TROPOMI (the TROPOspheric Monitoring Instrument), on-board the Sentinel-5 Precursor satellite, has been monitoring the Earth's atmosphere since October 2017, with an unprecedented horizontal resolution (initially 7×3.5 km2, upgraded to 5.5×3.5 km2 since August 2019). Monitoring air quality is one of the main objectives of TROPOMI, with the measurements of important pollutants such as nitrogen dioxide, carbon monoxide, and formaldehyde (HCHO). In this paper we assess the quality of the latest HCHO TROPOMI products (version 1.1.[5-7]), using ground-based solar-absorption FTIR (Fourier Transform Infrared) measurements of HCHO from twenty-five stations around the world, including high, mid, and low latitude sites. Most of these stations are part of the Network for the Detection of Atmospheric Composition Change (NDACC), and they provide a wide range of observation conditions from very clean remote sites to those with high HCHO levels from anthropogenic or biogenic emissions. The ground-based HCHO retrieval settings have been optimized and harmonized at all the stations, ensuring a consistent validation among the sites. In this validation work, we first assess the accuracy of TROPOMI HCHO tropospheric columns, using the median of the relative differences between TROPOMI and FTIR ground-based data (BIAS). We observe that, at all sites, the TROPOMI accuracy is below the upper limit of the pre-launch requirements of 80 %, and below the lower limit of 40 % for 20 of the 25 stations. The provided TROPOMI systematic uncertainties are well in agreement with the observed biases at most of the stations, except for the highest HCHO levels site where it is found to be underestimated. We find that, while the BIAS has no latitudinal dependence, it is dependent on the HCHO concentration levels: an overestimation (+26 &pm; 5 %) of TROPOMI is observed for very small HCHO levels ( 8.0 × 1015 molec/cm2). This demonstrates the great value of such a harmonized network covering a wide range of concentration levels, the sites with high HCHO concentrations being crucial for the determination of the satellite bias at the regions of emissions, and the clean sites allowing a small TROPOMI offset to be determined. The wide range of sampled HCHO levels within the network allows the robust determination of the significant constant and proportional TROPOMI HCHO biases (TROPOMI=+ 1.10 (&pm; 0.05) × 1015+ 0.64 (&pm; 0.03) × FTIR, in molec/cm2). Second, the precision of TROPOMI HCHO data is estimated by the median absolute deviation (MAD) of the relative differences between TROPOMI and FTIR ground-based data. The clean sites are especially useful to minimize a possible additional collocation error. The precision requirement of 1.2 × 1016 molec/cm2 for a single pixel is reached at most of the clean sites, where it is found that the TROPOMI precision can even be twice better (0.5–0.8 × 1015 molec/cm2 for a single pixel). However, we find that the provided TROPOMI random uncertainties may be underestimated by a factor of 1.6 (for clean sites) to 2.3 (for high HCHO levels). The correlation is very good between TROPOMI and FTIR data (R = 0.88 for 3 hours-mean coincidences; R = 0.91 for monthly means coincidences). Using about 17 months of data (from May 2018 to September 2019), we show that the TROPOMI seasonal variability is in very good agreement at all of the FTIR sites. The FTIR network demonstrates the very good quality of the TROPOMI HCHO products which is well within the pre-launch requirements for both accuracy and precision. This paper advises for a refinement of the TROPOMI random uncertainty budget and of the TROPOMI quality assurance values for a better filtering of the remaining outliers.

Among the more than 20 ground-based FTIR (Fourier transform infrared) stations currently operating around the globe, only a few have provided formaldehyde (HCHO) total column time series until now. Although several independent studies have shown that the FTIR measurements can provide formaldehyde total columns with good precision, the spatial coverage has not been optimal for providing good diagnostics for satellite or model validation. Furthermore, these past studies used different retrieval settings, and biases as large as 50 % can be observed in the HCHO total columns depending on these retrieval choices, which is also a weakness for validation studies combining data from different ground-based stations.For the present work, the HCHO retrieval settings have been optimized based on experience gained from past studies and have been applied consistently at the 21 participating stations. Most of them are either part of the Network for the Detection of Atmospheric Composition Change (NDACC) or under consideration for membership. We provide the harmonized settings and a characterization of the HCHO FTIR products. Depending on the station, the total systematic and random uncertainties of an individual HCHO total column measurement lie between 12 % and 27 % and between 1 and 11×1014 molec cm−2, respectively. The median values among all stations are 13 % and 2.9×1014 molec cm−2 for the total systematic and random uncertainties.This unprecedented harmonized formaldehyde data set from 21 ground-based FTIR stations is presented and its comparison with a global chemistry transport model shows consistency in absolute values as well as in seasonal cycles. The network covers very different concentration levels of formaldehyde, from very clean levels at the limit of detection (few 1013 molec cm−2) to highly polluted levels (7×1016 molec cm−2). Because the measurements can be made at any time during daylight, the diurnal cycle can be observed and is found to be significant at many stations. These HCHO time series, some of them starting in the 1990s, are crucial for past and present satellite validation and will be extended in the coming years for the next generation of satellite missions.

Multiple tropospheric gases are analyzed in ten years of observations (2010–2019) using a high-resolution ground-based solar absorption Fourier Transform InfraRed (FTIR) instrument in the Colorado Northern Front Range (CNFR). The first year of measurements in 2010 coincides with the start of the remarkable increase of oil and natural (O&NG) extraction in the region. We show seasonal variations and trends of atmospheric gases related to O&NG (C2H6), cattle feedlot activities (NH3), urban emissions (CO, C2H2), biomass burning (HCN), and volatile organic compounds related to photochemistry and ozone production (H2CO, HCOOH). The long-term time series of C2H6 shows clear episodic peak-enhancements related to local O&NG emissions that contribute to a positive trend of 0.9 ± 0.3% ⋅yr−1. NH3 also shows episodic enhancements and has the greatest rate of change for the gases studied here (2.7 ± 0.7% ⋅yr−1). Simulations of all gases are presented using the Community Atmosphere Model with chemistry (CAM-chem) within the Community Earth System Model (CESM) framework. Modeled gases are compared to the observations using different combinations of global emissions in order to determine the best combination for the CNFR. For most gases, using best emissions, the annual rate of change obtained with CAM-chem agrees with the FTIR observations, except for NH3, which is underestimated by a factor of 6. Nevertheless, simulations of NH3 show that the positive trend in NH3 is due to a decrease in its removal via reaction with H2SO4 from a reduction in coal power plant emissions. The seasonal variations of all gases are generally well represented in the model, although magnitudes are often underestimated. The anthropogenic emissions of CO, C2H2, and C2H6 are underestimated by about 20%, 40%, and 65%, respectively, independent of emission inventories. While NH3 summer values are underestimated significantly, other months show low relative mean difference between FTIR observations and CAM-chem simulations. Excellent agreement is found for H2CO, but for HCOOH a factor of 2–3 is needed in the simulations to match observations, pointing to a significant missing source. HCN, a tracer for biomass burning emissions, is well reproduced by the NCAR Fire Inventory (FINN). Furthermore, we show here a simple approach to identify local enhancements of gases related to nearby O&NG and concentrated animal feeding operations. These enhancements above ambient levels are used to estimate emission ratios (ER) of C2H6, H2CO, and HCOOH relative to CO from O&NG air masses. A median ER (and standard deviation) of 0.48 ± 0.41, 0.26 ± 0.15, and 0.13 ± 0.09 [ppb/ppb] are estimated for C2H6, H2CO, and HCOOH, respectively and are representative of the ten years of observations. ER can be used to estimate emission factors (EF), although CO emissions from O&NG need to be well-known. To complement the FTIR observations, we show results derived with airborne observations during The Front Range Air Pollution and Photochemical Experiment (FRAPPE) in 2014. Even though FTIR and FRAPPE observations can not be compared easily they both yield similar median ER. Finally, plumes of fires originated in the western United States in August 2015 were identified and EF are estimated.

Presented here is the validation of the CrIS (Cross-track Infrared Sounder) fast physical NH3 retrieval (CFPR) column and profile measurements using ground-based Fourier transform infrared (FTIR) observations. We use the total columns and profiles from seven FTIR sites in the Network for the Detection of Atmospheric Composition Change (NDACC) to validate the satellite data products. The overall FTIR and CrIS total columns have a positive correlation of r = 0.77 (N = 218) with very little bias (a slope of 1.02). Binning the comparisons by total column amounts, for concentrations larger than 1.0 × 1016 molecules cm−2, i.e. ranging from moderate to polluted conditions, the relative difference is on average ∼ 0–5 % with a standard deviation of 25–50 %, which is comparable to the estimated retrieval uncertainties in both CrIS and the FTIR. For the smallest total column range (

Formic (HCOOH) and acetic acids (CH3COOH) are the most abundant carboxylic acids in the Earth's atmosphere and key compounds to aqueous-phase chemistry. Here we present the first distributions of CH3COOH retrieved from the 2007–2018 satellite observations of the nadir-looking infrared atmospheric sounding interferometer (IASI), using a neural network-based retrieval approach. A joint analysis with the IASI HCOOH product reveals that the two species exhibit similar distributions, seasonality, and atmospheric burden, pointing to major common sources. We show that their abundance is highly correlated to isoprene and monoterpenes emissions, as well as to biomass burning. Over Africa, evidence is provided that residual smoldering combustion might be a major driver of the HCOOH and CH3COOH seasonality. Earlier seasonal enhancement of HCOOH at Northern Hemisphere middle and high latitudes and late seasonal secondary peaks of CH3COOH in the tropics suggest that sources and production pathways specific to each species are also at play., SCOPUS: ar.j, info:eu-repo/semantics/published

TROPOMI (the TROPOspheric Monitoring Instrument), on board the Sentinel-5 Precursor (S5P) satellite, has been monitoring the Earth's atmosphere since October 2017 with an unprecedented horizontal resolution (initially 7 km2×3.5 km2, upgraded to 5.5 km2×3.5 km2 in August 2019). Monitoring air quality is one of the main objectives of TROPOMI; it obtains measurements of important pollutants such as nitrogen dioxide, carbon monoxide, and formaldehyde (HCHO). In this paper we assess the quality of the latest HCHO TROPOMI products versions 1.1.(5-7), using ground-based solar-absorption FTIR (Fourier-transform infrared) measurements of HCHO from 25 stations around the world, including high-, mid-, and low-latitude sites. Most of these stations are part of the Network for the Detection of Atmospheric Composition Change (NDACC), and they provide a wide range of observation conditions, from very clean remote sites to those with high HCHO levels from anthropogenic or biogenic emissions. The ground-based HCHO retrieval settings have been optimized and harmonized at all the stations, ensuring a consistent validation among the sites. In this validation work, we first assess the accuracy of TROPOMI HCHO tropospheric columns using the median of the relative differences between TROPOMI and FTIR ground-based data (BIAS). The pre-launch accuracy requirements of TROPOMI HCHO are 40 %–80 %. We observe that these requirements are well reached, with the BIAS found below 80 % at all the sites and below 40 % at 20 of the 25 sites. The provided TROPOMI systematic uncertainties are well in agreement with the observed biases at most of the stations except for the highest-HCHO-level site, where it is found to be underestimated. We find that while the BIAS has no latitudinal dependence, it is dependent on the HCHO concentration levels: an overestimation (+26±5 %) of TROPOMI is observed for very low HCHO levels (<2.5×1015 molec. cm−2), while an underestimation (-30.8%±1.4 %) is found for high HCHO levels (>8.0×1015 molec. cm−2). This demonstrates the great value of such a harmonized network covering a wide range of concentration levels, the sites with high HCHO concentrations being crucial for the determination of the satellite bias in the regions of emissions and the clean sites allowing a small TROPOMI offset to be determined. The wide range of sampled HCHO levels within the network allows the robust determination of the significant constant and proportional TROPOMI HCHO biases (TROPOMI =+1.10±0.05 ×1015+0.64±0.03 × FTIR; in molecules per square centimetre). Second, the precision of TROPOMI HCHO data is estimated by the median absolute deviation (MAD) of the relative differences between TROPOMI and FTIR ground-based data. The clean sites are especially useful for minimizing a possible additional collocation error. The precision requirement of 1.2×1016 molec. cm−2 for a single pixel is reached at most of the clean sites, where it is found that the TROPOMI precision can even be 2 times better (0.5–0.8×1015 molec. cm−2 for a single pixel). However, we find that the provided TROPOMI random uncertainties may be underestimated by a factor of 1.6 (for clean sites) to 2.3 (for high HCHO levels). The correlation is very good between TROPOMI and FTIR data (R=0.88 for 3 h mean coincidences; R=0.91 for monthly means coincidences). Using about 17 months of data (from May 2018 to September 2019), we show that the TROPOMI seasonal variability is in very good agreement at all of the FTIR sites. The FTIR network demonstrates the very good quality of the TROPOMI HCHO products, which is well within the pre-launch requirements for both accuracy and precision. This paper makes suggestions for the refinement of the TROPOMI random uncertainty budget and TROPOMI quality assurance values for a better filtering of the remaining outliers.

We present a multi-year time series of column abundances of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier transform infrared (FTIR) spectrometers at ten sites affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Six are high-latitude sites: Eureka, Ny-Alesund, Thule, Kiruna, Poker Flat, and St. Petersburg , and four are mid-latitude sites: Zugspitze, Jungfraujoch, Toronto, and Rikubetsu. For each site, the inter-annual trends and seasonal variabilities of the CO time series are accounted for, allowing ambient concentrations to be determined. Enhancements above ambient levels were used to identify possible wildfire pollution events. Since the abundance of each trace gas emitted in a wildfire event is specific to the type of vegetation burned and the burning phase, correlations of CO to the long-lived wildfire tracers HCN and C2H6 allow for further confirmation of the detection of wildfire pollution, while complementary measurements of aerosol optical depth from nearby AERONET sites confirm the presence of wildfire smoke. A GEOS-Chem tagged CO simulation with Global Fire Assimilation System (GFAS) biomass burning emissions was used to determine the source attribution of CO concentrations at each site from 2003–2018. The influence of the various wildfire sources is found to differ between sites while North American and Asian boreal wildfires fires were found to be the greatest contributors to episodic CO enhancements in the summertime at all sites.

Retrievals of vertical profiles of key atmospheric gases provide a critical long-term record from ground-based Fourier transform infrared (FTIR) solar absorption measurements. However, the characterization of the retrieved vertical profile structure can be difficult to validate, especially for gases with large vertical gradients and spatial–temporal variability such as water vapor. In this work, we evaluate the accuracy of the most common water vapor isotope (H216O, hereafter WV) FTIR retrievals in the lower and upper troposphere–lower stratosphere. Coincident high-quality vertically resolved WV profile measurements obtained from 2010 to 2016 with balloon-borne NOAA frost point hygrometers (FPHs) are used as reference to evaluate the performance of the retrieved profiles at two sites: Boulder (BLD), Colorado, and at the mountaintop observatory of Mauna Loa (MLO), Hawaii. For a meaningful comparison, the spatial–temporal variability has been investigated. We present results of comparisons among FTIR retrievals with unsmoothed and smoothed FPH profiles to assess WV vertical gradients. Additionally, we evaluate the quantitative impact of different a priori profiles in the retrieval of WV. An orthogonal linear regression analysis shows the best correlation among tropospheric layers using ERA-Interim (ERA-I) a priori profiles and biases are lower for unsmoothed comparisons. In Boulder, we found a negative bias of 0.02±1.9 % (r=0.95) for the 1.5–3 km layer. A larger negative bias of 11.1±3.5 % (r=0.97) was found in the lower free troposphere layer of 3–5 km attributed to rapid vertical change of WV, which is not always captured by the retrievals. The bias improves in the 5–7.5 km layer (1.0±5.3 %, r=0.94). The bias remains at about 13 % for layers above 7.5 km but below 13.5 km. At MLO the spatial mismatch is significantly larger due to the launch of the sonde being farther from the FTIR location. Nevertheless, we estimate a negative bias of 5.9±4.6 % (r=0.93) for the 3.5–5.5 km layer and 9.9±3.7 % (r=0.93) for the 5.5–7.5 km layer, and we measure positive biases of 6.2±3.6 % (r=0.95) for the 7.5–10 km layer and 12.6 % and greater values above 10 km. The agreement for the first layer is significantly better at BLD because the air masses are similar for both FTIR and FPH. Furthermore, for the first time we study the influence of different WV a priori profiles in the retrieval of selected gas profiles. Using NDACC standard retrievals we present results for hydrogen cyanide (HCN), carbon monoxide (CO), and ethane (C2H6) by taking NOAA FPH profiles as the ground truth and evaluating the impact of other WV profiles. We show that the effect is minor for C2H6 (bias  % for all WV sources) among all vertical layers. However, for HCN we found significant biases between 6 % for layers close to the surface and 2 % for the upper troposphere depending on the WV profile source. The best results (reduced bias and precision and r values closer to unity) are always found for pre-retrieved WV. Therefore, we recommend first retrieving WV to use in subsequent retrieval of gases.

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurements during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.

The multiannual global mean of aerosol optical depth at 550 nm (AOD550) over land is ∼ 0.19, and that over oceans is ∼ 0.13. About 45 % of the Earth surface shows AOD550 smaller than 0.1. There is a need for measurement techniques that are optimized to measure aerosol optical properties under low AOD conditions. We present an inherently calibrated retrieval (i.e., no need for radiance calibration) to simultaneously measure AOD and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman scattering probability (RSP), the near-absolute rotational Raman scattering (RRS) intensity. We employ radiative transfer model simulations to show that for solar azimuth RSP measurements at solar elevation and solar zenith angle (SZA) smaller than 80°, RSP is insensitive to the vertical distribution of aerosols and maximally sensitive to changes in AOD and g under near-molecular scattering conditions. The University of Colorado two-dimensional Multi-AXis Differential Optical Absorption Spectroscopy (CU 2-D-MAX-DOAS) instrument was deployed as part of the Two Column Aerosol Project (TCAP) at Cape Cod, MA, during the summer of 2012 to measure direct sun spectra and RSP from scattered light spectra at solar relative azimuth angles (SRAAs) between 5 and 170°. During two case study days with (1) high aerosol load (17 July, 0.3 430 430 430 and g with data from a co-located CIMEL sun photometer, Multi-Filter Rotating Shadowband Radiometer (MFRSR), and an airborne High Spectral Resolution Lidar (HSRL-2). The average difference (relative to DOAS) for AOD430 is +0.012 ± 0.023 (CIMEL), −0.012 ± 0.024 (MFRSR), −0.011 ± 0.014 (HSRL-2), and +0.023 ± 0.013 (CIMELAOD − MFRSRAOD) and yields the following expressions for correlations between different instruments: DOASAOD = −(0.019 ± 0.006) + (1.03 ± 0.02) × CIMELAOD (R2 = 0.98), DOASAOD = −(0.006 ± 0.005) + (1.08 ± 0.02) × MFRSRAOD (R2 = 0.98), and CIMELAOD = (0.013 ± 0.004) + (1.05 ± 0.01) × MFRSRAOD (R2 = 0.99). The average g measured by DOAS on both days was 0.66 ± 0.03, with a difference of 0.014 ± 0.05 compared to CIMEL. Active steps to minimize the error in the RSP help to reduce the uncertainty in retrievals of AOD and g. As AOD decreases and SZA increases, the RSP signal-to-noise ratio increases. At AOD430 ∼ 0.4 and 0.10 the absolute AOD errors are ∼ 0.014 and 0.003 at 70° SZA and 0.02 and 0.004 at 35° SZA. Inherently calibrated, precise AOD and g measurements are useful to better characterize the aerosol direct effect in urban polluted and remote pristine environments.

The oxygen collisional complex (O2–O2, or O4) is a greenhouse gas, and a calibration trace gas used to infer aerosol and cloud properties by Differential Optical Absorption Spectroscopy (DOAS). Recent reports suggest the need for an O4 correction factor (CFO4) when comparing simulated and measured O4 differential slant column densities (dSCD) by passive DOAS. We investigate the sensitivity of O4 dSCD simulations at ultraviolet (360nm) and visible (477nm) wavelengths towards separately measured aerosol extinction profiles. Measurements were conducted by the University of Colorado 2D-MAX-DOAS instrument and NASA׳s multispectral High Spectral Resolution Lidar (HSRL-2) during the Two Column Aerosol Project (TCAP) at Cape Cod, MA in July 2012. During two case study days with (1) high aerosol load (17 July, AOD~0.35 at 477nm), and (2) near molecular scattering conditions (22 July, AOD

We have constructed and deployed a fast digital solar tracker aboard a moving ground-based platform. The tracker consists of two rotating mirrors, a lens, an imaging camera, and a motion compensation system that provides the Euler angles of the mobile platform in real time. The tracker can be simultaneously coupled to UV–Vis and Fourier transform infrared spectrometers, making it a versatile tool to measure the absorption of trace gases using solar incoming radiation. The integrated system allows the tracker to operate autonomously while the mobile laboratory is in motion. Mobile direct sun differential optical absorption spectroscopy (mobile DS-DOAS) observations using this tracker were conducted during summer 2014 as part of the Front Range Air Pollution and Photochemistry Experiment (FRAPPE) in Colorado, USA. We demonstrate an angular precision of 0.052° (about 1/10 of the solar disk diameter) during research drives and verify this tracking precision from measurements of the center to limb darkening (CLD, the changing appearance of Fraunhofer lines) in the mobile DS-DOAS spectra. The high photon flux from direct sun observation enables measurements of nitrogen dioxide (NO2) slant columns with high temporal resolution and reveals spatial detail in the variations of NO2 vertical column densities (VCDs). The NO2 VCD from DS-DOAS is compared with a co-located MAX-DOAS instrument. Overall good agreement is observed amid a highly heterogeneous air mass.

We developed a new nitrogen oxide (NOx) and carbon monoxide (CO) emission inventory for the Los Angeles-South Coast Air Basin (SoCAB) expanding the Fuel-based Inventory for motor-Vehicle Emissions and applied it in regional chemical transport modeling focused on the California Nexus of Air Quality and Climate Change (CalNex) 2010 field campaign. The weekday NOx emission over the SoCAB in 2010 is 620 t d−1, while the weekend emission is 410 t d−1. The NOx emission decrease on weekends is caused by reduced diesel truck activities. Weekday and weekend CO emissions over this region are similar: 2340 and 2180 t d−1, respectively. Previous studies reported large discrepancies between the airborne observations of NOx and CO mixing ratios and the model simulations for CalNex based on the available bottom-up emission inventories. Utilizing the newly developed emission inventory in this study, the simulated NOx and CO mixing ratios agree with the observations from the airborne and the ground-based in situ and remote sensing instruments during the field study. The simulations also reproduce the weekly cycles of these chemical species. Both the observations and the model simulations indicate that decreased NOx on weekends leads to enhanced photochemistry and increase of O3 and Ox (=O3 + NO2) in the basin. The emission inventory developed in this study can be extended to different years and other urban regions in the U.S. to study the long-term trends in O3 and its precursors with regional chemical transport models.