The abundance of chlorine in the Earth's atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably ...the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale, before they reach the stratosphere where they release chlorine atoms that cause ozone depletion. The large ozone loss over Antarctica was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine- and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year, in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996, then a decrease of close to one per cent per year, in agreement with the surface observations of the chlorine source gases and model calculations. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer.
Celotno besedilo
Dostopno za:
DOBA, IJS, IZUM, KILJ, KISLJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
We use 2009-2011 space-borne methane observations from the Greenhouse Gases Observing SATellite (GOSAT) to estimate global and North American methane emissions with 4 degree 5 degree and up to 50 km ...50 km spatial resolution, respectively. GEOS-Chem and GOSAT data are first evaluated with atmospheric methane observations from surface and tower networks (NOAA/ESRL, TCCON) and aircraft (NOAA/ESRL, HIPPO), using the GEOS-Chem chemical transport model as a platform to facilitate comparison of GOSAT with in situ data. This identifies a high-latitude bias between the GOSAT data and GEOS-Chem that we correct via quadratic regression. Our global adjoint-based inversion yields a total methane source of 539 Tg a-1 with some important regional corrections to the EDGARv4.2 inventory used as a prior. Results serve as dynamic boundary conditions for an analytical inversion of North American methane emissions using radial basis functions to achieve high resolution of large sources and provide error characterization. We infer a US anthropogenic methane source of 40.2-42.7 Tg a-1, as compared to 24.9-27.0 Tg a-1 in the EDGAR and EPA bottom-up inventories, and 30.0-44.5 Tg a-1 in recent inverse studies. Our estimate is supported by independent surface and aircraft data and by previous inverse studies for California. We find that the emissions are highest in the southern-central US, the Central Valley of California, and Florida wetlands; large isolated point sources such as the US Four Corners also contribute. Using prior information on source locations, we attribute 29-44 % of US anthropogenic methane emissions to livestock, 22-31 % to oil/gas, 20 % to landfills/wastewater, and 11-15 % to coal. Wetlands contribute an additional 9.0-10.1 Tg a-1.
Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2% but also independent partial column amounts in about ...four vertical layers, one in the troposphere and three in the stratosphere up to about 45km, with a precision of 5-6%. We use eight of the Network for the Detection of Atmospheric Composition Change (NDACC) stations having a long-term time series of FTIR ozone measurements to study the total and vertical ozone trends and variability, namely, Ny-Aalesund (79 degree N), Thule (77 degree N), Kiruna (68 degree N), Harestua (60 degree N), Jungfraujoch (47 degree N), Izana (28 degree N), Wollongong (34 degree S) and Lauder (45 degree S). The length of the FTIR time series varies by station but is typically from about 1995 to present. We applied to the monthly means of the ozone total and four partial columns a stepwise multiple regression model including the following proxies: solar cycle, quasi-biennial oscillation (QBO), El Nino-Southern Oscillation (ENSO), Arctic and Antarctic Oscillation (AO/AAO), tropopause pressure (TP), equivalent latitude (EL), Eliassen-Palm flux (EPF), and volume of polar stratospheric clouds (VPSC). At the Arctic stations, the trends are found mostly negative in the troposphere and lower stratosphere, very mixed in the middle stratosphere, positive in the upper stratosphere due to a large increase in the 1995-2003 period, and non-significant when considering the total columns. The trends for mid-latitude and subtropical stations are all non-significant, except at Lauder in the troposphere and upper stratosphere and at Wollongong for the total columns and the lower and middle stratospheric columns where they are found positive. At Jungfraujoch, the upper stratospheric trend is close to significance (+0.9 plus or minus 1.0% decade-1). Therefore, some signs of the onset of ozone mid-latitude recovery are observed only in the Southern Hemisphere, while a few more years seem to be needed to observe it at the northern mid-latitude station.
This study investigates the use of total column CH4 (XCH4) retrievals from the SCIAMACHY satellite instrument for quantifying large-scale emissions of methane. A unique data set from SCIAMACHY is ...available spanning almost a decade of measurements, covering a period when the global CH4 growth rate showed a marked transition from stable to increasing mixing ratios. The TM5 4DVAR inverse modelling system has been used to infer CH4 emissions from a combination of satellite and surface measurements for the period 2003–2010. In contrast to earlier inverse modelling studies, the SCIAMACHY retrievals have been corrected for systematic errors using the TCCON network of ground-based Fourier transform spectrometers. The aim is to further investigate the role of bias correction of satellite data in inversions. Methods for bias correction are discussed, and the sensitivity of the optimized emissions to alternative bias correction functions is quantified. It is found that the use of SCIAMACHY retrievals in TM5 4DVAR increases the estimated inter-annual variability of large-scale fluxes by 22% compared with the use of only surface observations. The difference in global methane emissions between 2-year periods before and after July 2006 is estimated at 27–35 Tg yr−1. The use of SCIAMACHY retrievals causes a shift in the emissions from the extra-tropics to the tropics of 50 ± 25 Tg yr−1. The large uncertainty in this value arises from the uncertainty in the bias correction functions. Using measurements from the HIPPO and BARCA aircraft campaigns, we show that systematic errors in the SCIAMACHY measurements are a main factor limiting the performance of the inversions. To further constrain tropical emissions of methane using current and future satellite missions, extended validation capabilities in the tropics are of critical importance.
The chemical processes in daytime sprite streamers in the altitude range of 30–54 km are investigated by means of a detailed ion–neutral chemistry model (without consideration of transport). The ...focus lies on nitrogen, hydrogen and oxygen species, and in particular on ozone perturbations. Initial effects of the breakdown electric fields at the tip of sprite streamers include a short-term loss of ozone due to ion–chemical reactions, a production of nitrogen radicals, and a liberation of atomic oxygen. The latter leads to a formation of ozone. In terms of relative ozone change, this effect decreases with altitude. The model results indicate that the subsequent ozone perturbations due to daytime sprites streamers differ considerably from the ones of night-time events. For night-time conditions, reactive nitrogen produced at the streamer heads is rapidly converted into significantly less reactive NO2, and there is basically no ozone depletion. The situation is different for daytime conditions where NOx causes catalytic ozone destruction. As a consequence, there is significant ozone loss in sprite streamers in the daytime atmosphere, in particular at higher altitudes. At an altitude of 54 km, ozone in the streamer column has decreased by about 15% fifteen minutes after the sprite event.
The column-averaged dry-air mole fractions of carbon dioxide and methane (XCO2 and XCH4 ) have been retrieved from Greenhouse gases Observing SATellite (GOSAT) Short-Wavelength InfraRed (SWIR) ...observations and released as a SWIR L2 product from the National Institute for Environmental Studies (NIES). XCO2 and XCH4 retrieved using the version 01.xx retrieval algorithm showed large negative biases and standard deviations (-8.85 and 4.75 ppm for XCO2 and -20.4 and 18.9 ppb for XCH4 , respectively) compared with data of the Total Carbon Column Observing Network (TCCON). Multiple reasons for these error characteristics (e.g., solar irradiance database, handling of aerosol scattering) are identified and corrected in a revised version of the retrieval algorithm (version 02.xx). The improved retrieval algorithm shows much smaller biases and standard deviations (-1.48 and 2.09 ppm for XCO2 and -5.9 and 12.6 ppb for XCH4 , respectively) than the version 01.xx. Also, the number of post-screened measurements is increased, especially at northern mid- and high-latitudinal areas.
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.
The column‐average dry air mole fractions of atmospheric carbon dioxide and methane and are inferred from observations of backscattered sunlight conducted by the Greenhouse gases Observing SATellite ...(GOSAT). Comparing the first year of GOSAT retrievals over land with colocated ground‐based observations of the Total Carbon Column Observing Network (TCCON), we find an average difference (bias) of −0.05% and −0.30% for and with a station‐to‐station variability (standard deviation of the bias) of 0.37% and 0.26% among the 6 considered TCCON sites. The root‐mean square deviation of the bias‐corrected satellite retrievals from colocated TCCON observations amounts to 2.8 ppm for and 0.015 ppm for Without any data averaging, the GOSAT records reproduce general source/sink patterns such as the seasonal cycle of suggesting the use of the satellite retrievals for constraining surface fluxes.
Key Points
Improved quality of XCO2 and XCH4 satellite retrievals due to refined methods
Source/sink patterns are dentifiable in the data record without averaging
Constrained surface flux modeling is the logical next step
The waterline method is used to derive the topography of the tidal flats along the German coast by evaluation of synthetic aperture radar (SAR) images. A series of about 70 European Remote Sensing ...Satellites SAR images of the German Bight taken at different water levels within four years is analyzed to detect the borderline between tidal flats and adjacent water areas using a wavelet-based edge-detection algorithm. After geocoding, the waterlines are combined with the corresponding water levels to represent the topography on an irregularly spaced grid. The water levels are taken from a numerical tide model and corrected with the measured gauge data. Interpolation of these data into a regular grid yields a topographic map of the intertidal zone. While the general practicability of this method has been demonstrated in previous studies for smaller test areas, this paper is the first attempt to generate maps of a large area on a yearly basis.
Hydrogen cyanide (HCN) is an important tracer of biomass burning, but there are significant uncertainties in its atmospheric budget, especially its photochemical and ocean sinks. Here we use a tracer ...version of the TOMCAT global 3-D chemical transport model to investigate the physical and chemical processes driving the abundance of HCN in the troposphere and stratosphere over the period 2004–2016.
The modelled HCN distribution is compared with version 4.1 of the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) HCN satellite data, which provide profiles up to around 42 km, and with ground-based column measurements from the Network for the Detection of Atmospheric Composition Change (NDACC). The long-term ACE-FTS measurements reveal the strong enhancements in upper-tropospheric HCN due to large wildfire events in Indonesia in 2006 and 2015. Our 3-D model simulations confirm previous lower-altitude balloon comparisons that the currently recommended NASA Jet Propulsion Laboratory (JPL) reaction rate coefficient of HCN with OH greatly overestimates the HCN loss. The use of the rate coefficient proposed by Kleinböhl et al. (2006) in combination with the HCN oxidation by O(1D) gives good agreement between ACE-FTS observations and the model. Furthermore, the model photochemical loss terms show that the reduction in the HCN mixing ratio with height in the middle stratosphere is mainly driven by the O(1D) sink with only a small contribution from a reaction with OH.
From comparisons of the model tracers with ground-based HCN observations we test the magnitude of the ocean sink in two different published schemes (Li et al., 2000, 2003). We find that in our 3-D model the two schemes produce HCN abundances which are very different to the NDACC observations but in different directions. A model HCN tracer using the Li et al. (2000) scheme overestimates the HCN concentration by almost a factor of 2, while a HCN tracer using the Li et al. (2003) scheme underestimates the observations by about one-third. To obtain good agreement between the model and observations, we need to scale the magnitudes of the global ocean sinks by factors of 0.25 and 2 for the schemes of Li et al. (2000) and Li et al. (2003), respectively. This work shows that the atmospheric photochemical sinks of HCN now appear well constrained but improvements are needed in parameterizing the major ocean uptake sink.
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