Search

National Aeronautics and Space Administration's Orbiting Carbon Observatory‐2 (OCO‐2) satellite provides observations of total column‐averaged CO2mole fractions ( XCO2) at high spatial resolution that may enable novel constraints on surface‐atmosphere carbon fluxes. Atmospheric inverse modeling provides an approach to optimize surface fluxes at regional scales, but the accuracy of the fluxes from inversion frameworks depends on key inputs, including spatially and temporally dense CO2observations and reliable representations of atmospheric transport. Since XCO2observations are sensitive to both synoptic and mesoscale variations within the free troposphere, horizontal atmospheric transport imparts substantial variations in these data and must be either resolved explicitly by the atmospheric transport model or accounted for within the error covariance budget provided to inverse frameworks. Here, we used geostatistical techniques to quantify the imprint of atmospheric transport in along‐track OCO‐2 soundings. We compare high‐pass‐filtered (<250 km, spatial scales that primarily isolate mesoscale or finer‐scale variations) along‐track spatial variability in XCO2and XH2Ofrom OCO‐2 tracks to temporal synoptic and mesoscale variability from ground‐based XCO2and XH2Oobserved by nearby Total Carbon Column Observing Network sites. Mesoscale atmospheric transport is found to be the primary driver of along‐track, high‐frequency variability for OCO‐2 XH2O. For XCO2, both mesoscale transport variability and spatially coherent bias associated with other elements of the OCO‐2 retrieval state vector are important drivers of the along‐track variance budget. Numerous efforts have been made to quantify sources and sinks of atmospheric CO2at regional spatial scales. A common approach to infer these sources and sinks requires accurate representation of variability of CO2observations attributed to transport by weather systems. While numerical weather prediction models have a fairly reasonable representation of larger‐scale weather systems, such as frontal systems, representation of smaller‐scale features (<250 km), is less reliable. In this study, we find that the variability of total column‐averaged CO2observations attributed to these fine‐scale weather systems accounts for up to half of the variability attributed to local sources and sinks. Here, we provide a framework for quantifying the drivers of spatial variability of atmospheric trace gases rather than simply relying on numerical weather prediction models. We use this framework to quantify potential sources of errors in measurements of total column‐averaged CO2and water vapor from National Aeronautics and Space Administration's Orbiting Carbon Observatory‐2 satellite. We developed a framework to relate high‐frequency spatial variations to transport‐induced temporal fluctuations in atmospheric tracersWe use geostatistical analysis to quantify the variance budget for XCO2and XH2Oretrieved from NASA's OCO‐2 satelliteAccounting for random errors, systematic errors, and real geophysical coherence in remotely sensed trace gasobservations may yield improved flux constraints

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. In two linear trend time periods ∼2002 to 2008 and ∼2008 to 2016 tropospheric trends range from ∼0.0 to (1.55 ± 0.30%/yr) in contrast to the prior period where all tropospheric trends are negative. Regression analyses show strongest correlation in the free troposphere with anthropogenic emissions. Stratospheric trends in the period ∼2008 to 2016 are positive up to (1.93 ± 0.26%/yr) except notably low latitude stations that have negative stratospheric trends. Since ∼2016, all stations show a free tropospheric decrease to 2020. Stratospheric OCS is regressed with simultaneously measured N2O to derive a trend accounting for dynamical variability. Stratospheric lifetimes are derived and range from (54.1 ± 9.7)yr in the sub‐tropics to (103.4 ± 18.3)yr in Antarctica. These unique long‐term measurements provide new and critical constraints on the global OCS budget. Carbonyl sulfide (OCS) is the most abundant sulfur containing gas in the atmosphere. There are many sources and sinks of OCS and other sulfur species in the atmosphere but most other short lived sulfur species eventually are converted to OCS. It is important to quantify and understand OCS as it can be used to understand CO2and the carbon cycle and also since it eventually is transported into the stratosphere where it maintains the sulfate aerosol layer at about 20 km into the atmosphere. This layer is very important for earth's energy balance and climate change. In contrast with earlier and less comprehensive reports, this global study from 22 observation stations worldwide, shows stratospheric OCS to be increasing north and south of the equator but decreasing near the equator and to be increasing in the troposphere to 2016 and decreasing since. The main drivers of OCS in the troposphere are the cumulative anthropogenic sources. Global distribution of carbonyl sulfide (OCS) measured by NDACC solar absorption FTIR remote sensingTropospheric trends in OCS are non‐monotonic globally, driven by anthropogenic emissionsLongest term stratospheric trends are increasing outside of sub‐tropics Global distribution of carbonyl sulfide (OCS) measured by NDACC solar absorption FTIR remote sensing Tropospheric trends in OCS are non‐monotonic globally, driven by anthropogenic emissions Longest term stratospheric trends are increasing outside of sub‐tropics

Photographs of a 120° parhelion and a 22° parhelion within persistent contrails are presented. These phenomena result from hexagonal plate-shaped ice crystals oriented horizontally with diameters between 300 µm and 2 mm. From our observations and reinvestigation of previous reports, we conclude that a subset of the population in persistent contrails can consist of highly regular, oriented, hexagonal plates or columns comparable to the most regular crystals in natural cirrus clouds. This is explained by measured ambient humidities below the formation conditions of natural cirrus. The resulting strong azimuthal variability of the scattering phase function impacts the radiative transfer through persistent contrails.

Vibration-rotation absorptions in high-resolution Fourier-transform infrared spectra from a 246-m horizontal path were used to derive local concentrations of trace gases at the Alpine observatory at the Zugspitze summit, Germany (2964 m above sea level). The analysis was performed by using the line-by-line nonlinear least-squares spectral fitting software, sfit, based on the 1992 hitran line parameter compilation. (hitran is a high-resolution transmission molecular absorption database.) A comparison to in situ measurements shows an agreement of better than 4.3% for the species CO, CO_2, and CH_4. Using the same spectrometer and analysis software, we obtained the vertical column density of N_2O together with an adjusted vertical volume mixing ratio distribution. This translates to a local N_2O concentration at the altitude of Zugspitze that agrees with the horizontal path-derived value to within 1%.

Throughout spring and summer 2020, ozone stations in the northern extratropics recorded unusually low ozone in the free troposphere. From April to August, and from 1 to 8 kilometers altitude, ozone was on average 7% (≈4 nmol/mol) below the 2000–2020 climatological mean. Such low ozone, over several months, and at so many stations, has not been observed in any previous year since at least 2000. Atmospheric composition analyses from the Copernicus Atmosphere Monitoring Service and simulations from the NASA GMI model indicate that the large 2020 springtime ozone depletion in the Arctic stratosphere contributed less than one‐quarter of the observed tropospheric anomaly. The observed anomaly is consistent with recent chemistry‐climate model simulations, which assume emissions reductions similar to those caused by the COVID‐19 crisis. COVID‐19 related emissions reductions appear to be the major cause for the observed reduced free tropospheric ozone in 2020. Worldwide actions to contain the COVID‐19 virus have closed factories, grounded airplanes, and have generally reduced travel and transportation. Less fuel was burnt, and less exhaust was emitted into the atmosphere. Due to these measures, the concentration of nitrogen oxides and volatile organic compounds (VOCs) decreased in the atmosphere. These substances are important for photochemical production and destruction of ozone in the atmosphere. In clean or mildly polluted air, reducing nitrogen oxides and/or VOCs will reduce the photochemical production of ozone and result in less ozone. In heavily polluted air, in contrast, reducing nitrogen oxides can increase ozone concentrations, because less nitrogen oxide is available to destroy ozone. In this study, we use data from three types of ozone instruments, but mostly from ozonesondes on weather balloons. The sondes fly from the ground up to 30 kilometers altitude. In the first 8 km, we find significantly reduced ozone concentrations in the northern extratropics during spring and summer of 2020, less than in any other year since at least 2000. We suggest that reduced emissions due to the COVID‐19 crisis have lowered photochemical ozone production and have caused the observed ozone reductions in the troposphere. In spring and summer 2020, stations in the northern extratropics report on average 7% (4 nmol/mol) less tropospheric ozone than normalSuch low tropospheric ozone, over several months, and at so many sites, has not been observed in any previous year since at least 2000Most of the reduction in tropospheric ozone in 2020 is likely due to emissions reductions related to the COVID‐19 pandemic In spring and summer 2020, stations in the northern extratropics report on average 7% (4 nmol/mol) less tropospheric ozone than normal Such low tropospheric ozone, over several months, and at so many sites, has not been observed in any previous year since at least 2000 Most of the reduction in tropospheric ozone in 2020 is likely due to emissions reductions related to the COVID‐19 pandemic

Total columns of the trace gases nitric acid (HNO3) and hydrogen chloride (HCl) are sensitive to variations in the lower stratospheric age of air, a quantity that describes transport time scales in the stratosphere. Analyses of HNO3and HCl columns from the Network for the Detection of Atmospheric Composition Change panning 77°S to 79°N have detected changes in the extratropical stratospheric transport circulation from 1994 to 2018. The HNO3and HCl analyses combined with the age of air from a simulation using the MERRA2 reanalysis show that the Southern Hemisphere lower stratosphere has become 1 month/decade younger relative to the Northern Hemisphere, largely driven by the Southern Hemisphere transport circulation. The analyses reveal multiyear anomalies with a 5‐ to 7‐year period driven by interactions between the circulation and the quasi‐biennial oscillation in tropical winds. This hitherto unrecognized variability is large relative to hemispheric transport trends and may bias ozone trend regressions. Our analyses of the 25‐year Network for the Detection of Atmospheric Composition Change column HNO3and HCl data records from nine stations provide observational evidence that air in the Southern Hemisphere lower stratosphere has been getting younger relative to the Northern Hemisphere at a rate of 1 month/decade since 1994. This stands in contrast to several model studies that predict that Antarctic ozone hole recovery in this century will increase the Southern Hemisphere age of air relative to the Northern Hemisphere. The analyses also reveal extratropical variability with a 5‐ to 7‐year period driven by interactions between the circulation and tropical winds. This previously unrecognized, low‐frequency variability is much larger than hemispheric transport trends and is likely to cause bias in trends calculated using data records shorter than about two decades. Understanding and quantifying changes in the transport circulation matters to our ability to model how our protective O3layer will evolve in the future. Trace gas data show southern stratospheric air is getting younger relative to the Northern Hemisphere, in contrast to model predictionsBoth extratropical hemispheres have dynamically driven 5‐ to 7‐year periodicity with large amplitude relative to the age trendMultidecadal data sets are required to quantify transport trends that are not confounded by large extratropical variability