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At least 73 records · Page 4

Dynamical and Trace Gas Responses of the Quasi-Biennial Oscillation to Increased CO2

Long-term projections of the Quasi-Biennial Oscillation (QBO) remain uncertain. Using the high-top \Middle Atmosphere" (MA) version of the NASA Goddard Institute for Space Studies (GISS) ModelE (E2.2-AP), we show that increased CO2 reduces the QBO period and weakens its amplitude, consistent with results from recent multimodel studies. The amplitude response is asymmetric, with the easterly phase weakening more than the westerly phase. Results from both coupled atmosphere{ocean and climatologically fixed sea surface temperature simulations link the period response to changes in parameterized convective gravity wave fluxes, whereas the amplitude changes are more closely tied to changes in tropical upwelling. Comparisons of simulations with and without ozone-dynamical feedbacks reveal that ozone feedbacks increase the QBO amplitude and period in pre-industrial control simulations, and reduce the response of the amplitude to increased CO2. The response of stratospheric tracers to projected changes in the QBO is also investigated. Similarity between results using fully interactive (trace gas and aerosol) versus linearized ozone chemical mechanisms suggests that the QBO response to CO2 does not depend on additional chemical feedbacks beyond those associated with ozone, which implies that projected QBO changes may be credibly represented using simpli fied stratospheric ozone schemes.

GISS Model E2.2-AP↗

A Lagrangian View of Stratospheric Trace Gas Distributions

As a result of photochemistry, some relationship between the stratospheric age-of-air and the amount of tracer contained within an air sample is expected. The existence of such a relationship allows inferences about transport history to be made from observations of chemical tracers. This paper lays down the conceptual foundations for the relationship between age and tracer amount, developed within a Lagrangian framework. In general, the photochemical loss depends not only on the age of the parcel but also on its path. We show that under the "average path approximation" that the path variations are less important than parcel age. The average path approximation then allows us to develop a formal relationship between the age spectrum and the tracer spectrum. Using the relation between the tracer and age spectra, tracer-tracer correlations can be interpreted as resulting from mixing which connects parts of the single path photochemistry curve, which is formed purely from the action of photochemistry on an irreducible parcel. This geometric interpretation of mixing gives rise to constraints on trace gas correlations, and explains why some observations are do not fall on rapid mixing curves. This effect is seen in the ATMOS observations.

Schoeberl, M. R.↗

Radon 222 tracing of soil and forest canopy trace gas exchange in an open canopy boreal forest

A set of continuous, high-resolution atmospheric radon (Rn-222) concentration time series and radon soil flux measurements were acquired during the summer of 1990 at a micrometeorological tower site 13 km northwest of Schefferville, Quebec, Canada. The tower was located in a dry upland, open-canopy lichen-spruce woodland. For the period July 23 to August 1, 1990, the mean radon soil flux was 41.1 +/- 4.8 Bq m(exp -2)/h. Radon surface flux from the two end-member forest floor cover types (lichen mat and bare soil) were 38.8 +/- 5.1 and 61.8 +/- 15.6 Bq m(exp -2)/h, respectively. Average total forest canopy resistances computed using a simple 'flux box' model for radon exchange between the forest canopy and the overlying atmosphere range from 0.47 +/- 0.24 s cm(exp -1) to 2.65 +/- 1.61 cm(exp -1) for daytime hours (0900-1700 LT) and from 3.44 +/- 0.91 s cm(exp -1) to 10.55 +/- 7.16 s cm(exp -1) for nighttime hours (2000-0600) for the period July 23 to August 6, 1990. Continuous radon profiling of canopy atmospheres is a suitable approach for determining rates of biosphere/atmosphere trace gas exchange for remote field sites where daily equipment maintenance is not possible. where daily equipment maintenance is not possible.

Ussler, William, III↗

TROPOMI Geometry-dependent Lambertian-Equivalent surface Reflectivity (GLER) Product for Improved Trace-Gas Retrieval

Accurate information about the reflectivity of the Earth's surface is required for most satellite retrievals of atmospheric composition, and this information is generally taken from monthly surface reflectivity climatology that neglects angular dependence. Previously we introduced Geometry-dependent Lambertian-equivalent surface reflectivity (GLER) which captures solar and satellite viewing angle dependence as well as daily and seasonal changes. GLER is calculated from simulations of Rayleigh-only top-of-atmosphere (TOA) radiances over non-Lambertian surfaces. We use NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) bidirectional reflectance distribution function (BRDF) product over land and the wind-dependent Cox–Munk wave-facet slope distribution including water-leaving radiance over water to accounts for surface BRDF. We have developed global GLER product, previously for the Ozone Monitoring Instrument (OMI) and recently for Sentinel-5 Precursor (S5P) TROPOspheric Monitoring Instrument (TROPOMI) with several new improvements and updates. We have implemented the near real time daily V006 MODIS MCD43C1 BRDF data and gap-filled with a daily BRDF coefficient climatology created from 2002-2017 V006 MCD43GF data. The NASA’s Global Modelling Initiative hourly 0.25 x 0.25 deg Replay simulations are used for more accurate determination of pixel specific terrain pressure. To improve detection of seasonal snow/ice scenes, we use the 4-km snow cover product from the Interactive Multi-sensor Snow and Ice Mapping System (IMS). Finally, we use an improved version of the vector linearized discrete ordinate radiative transfer (VLIDORT) for update of the top-of-atmosphere (TOA) radiance look-up-tables (LUTs). We demonstrate how the use of GLER is beneficial to TROPOMI’s high spatial resolution (up to 3.5 km x 3.5 km) measurements to monitor atmospheric trace gas pollutants down to the sub-city scale.

TROPOMI↗

Decoupling in the Vertical Shape of HCHO During a Sea Breeze Event: the Effect on Trace Gas Satellite Retrievals and Column-to-Surface Translation

The effect of sea breeze circulation on stratification of the vertical formaldehyde (HCHO) concentration vertical profiles is explored using a regional atmospheric chemical transport model (CTM) for three synoptically stagnant days focused on the east coast of the U.S in June 2018. During this event, a significant thermal contrast between the Atlantic Ocean and the terrestrial regions (12–17 °C), observed by moderate resolution imaging spectroradiometer (MODIS) and well-captured by the WRF-CMAQ model (15–18 °C), is conducive to monsoon-like flow, perpendicular to the shorelines, carrying clean marine air masses over the land within a few hundreds of meters above the surface. In contrast, the westerly continental polluted air masses prevail in higher altitudes. These two conflicting flows result in atypical vertical shapes of HCHO concentrations increasing with altitude. This decoupling pattern is so pronounced that we observe total column HCHO negatively correlate with surface concentrations. Comparisons of an accredited global model, GEOS-CF, to surface wind measurements and MODIS skin temperature indicate its poor representation of the sea breeze timing and strength, resulting in GEOS-CF HCHO vertical shapes being drastically different from the WRF-CMAQ. Based on radiative transfer calculations, the differences in the vertical distribution of HCHO between the WRF-CMAQ and that of GEOS-CF in the first 3 km are sufficient to induce a 20–30% error in air mass factors (thus total vertical HCHO column abundances). Through an experiment involving converting HCHO total columns to surface mixing ratios, we demonstrate that GEOS-CF allocates noticeably more HCHO molecules (40–150%) to the surface layer due to the misrepresentation of the vertical shape of HCHO during the sea breeze event. It is known that a significant fraction of the human population lives in coastal areas prone to detrimental effects caused by air pollution, and elevated pollutant concentrations usually occur in synoptically stagnant atmospheric conditions when local circulation patterns come into play; accordingly, our experiments emphasize the importance of the effect a priori profiles can have on satellite-derived applications under such conditions. To ensure that the quantitative representation of satellite-based trace gas retrievals on a daily basis is trustworthy and useable for air quality applications, atmospheric models providing a priori profiles for satellite retrievals should be well-tuned to reproduce complex local circulation such as sea-land breezes.

sea breeze↗

Trace Gas Measurements on Mars and Earth Using Optical Parametric Generation

Trace gases and their isotopic ratios in planetary atmospheres offer important but subtle clues as to the origins of a planet's atmosphere, hydrology, geology, and potential for biology. An orbiting laser remote sensing instrument is capable of measuring trace gases on a global scale with unprecedented accuracy, and higher spatial resolution that can be obtained by passive instruments. We have developed an active sensing instrument for the remote measurement of trace gases in planetary atmospheres (including Earth). The technique uses widely tunable, seeded optical parametric generation (OPG) to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planets. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but recent observations indicate that methane levels may be on the rise. Increasing methane concentrations may trigger a positive feedback loop and a subsequent runaway greenhouse effect, where increasing temperatures result in increasing methane levels. The NRC Decadal Survey recognized the importance of global observations of greenhouse gases and called for simultaneous CH4, CO, and CO2 measurements but also underlined the technological limitations for these observations. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can identify and localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. It can identify the dynamics of methane generation over time and latitude and identify future lander mission sites for more detailed in-situ analysis. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micron and 1.65 micron. The OPG is pumped by a passively q-switched single frequency laser (3ns, 5KHz, 50uJ) and seeded by a diode laser. The spectral width of both signal and idler of seeded OPG is nearly Fourier transform limited. The output of seeded OPG is single frequency with high spectral purity and is widely tunable. Both 1650 nm and 3300 nm can be generated with a conversion efficiency of more than 30%. We have demonstrated detection of methane at 3274 nm and 1650 nm in a cell and also performed open path atmospheric measurements of methane at the same wavelengths. Finally, we were able to demonstrate simultaneous detection of methane at 3270.4 nm and CO2 at 1578.2 nm. In this paper we will discuss the OPG performance and atmospheric open path measurement results.

Numata, Kenji↗

Trace gas emissions from burning Florida wetlands

Measurements of biomass burn-produced trace gases were obtained using a helicopter at low altitudes above burning Florida wetlands on November 9, 1987, and from both helicopter and light-aircraft samplings on November 7, 1988. Carbon dioxide normalized emission ratios for carbon monoxide, hydrogen, methane, total nonmethane hydrocarbons, and nitrous oxide were obtained over burning graminoid wetlands consisting primarily of Spartina bakeri and Juncus roemerianus. Some interspersed scrub oak and saw palmetto were also burned. No significant differences were observed in the emission ratios determined for these gases from samples collected over flaming, mixed, and smoldering phases of combustion during the 1987 fire. Combustion-categorized differences in emission ratios were small for the 1988 fire. Combustion efficiency was relatively good (low emission ratios for reduced gases) for both fires. It is believed that the consistently low emission ratios were a unique result of graminoid wetlands fires, in which the grasses and rushes burned rapidly down to standing water and were quickly extinguished. Consequently, the efficiency of the combustion was good and the amount and duration of smoldering combustion was greatly deminished.

Cofer, Wesley R., III↗

On the Assessment and Uncertainty of Atmospheric Trace Gas Burden Measurements with High Resolution Infrared Solar Occultation Spectra from Space by the ATMOS Experiment

The Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument is a high resolution Fourier transform spectrometer that measures atmospheric composition from low Earth orbit with infrared solar occultation sounding in the limb geometry. Following an initial flight in 1985, ATMOS participated in the Atmospheric Laboratory for Applications and Science (ATLAS) 1, 2, and 3 Space Shuttle missions in 1992, 1993, and 1994 yielding a total of 440 occultation measurements over a nine year period. The suite of more than thirty atmospheric trace gases profiled includes CO2, O3, N2O, CH4, H2O, NO, NO2, HNO3, HCl, HF, ClONO2, CCl3F, CCl2F2, CHF2Cl, and N2O5. The analysis method has been revised throughout the mission years culminating in the 'version 2' data set. The spectroscopic error analysis is described in the context of supporting the precision estimates reported with the profiles; in addition, systematic uncertainties assessed from the quality of the spectroscopic database are described and tabulated for comparisons with other experiments.

Abrams, M. C.↗

Monitoring complex trace-gas mixtures by long-path laser absorption spectrometry

Laser-based spectrophotometric methods, which have been proposed for the detection of trace concentrations of gaseous contaminants, include Raman and passive radiometry. The paper discusses a simple long-path laser absorption method which is capable of resolving complex mixtures of closely related trace contaminants at ppm levels. A number of species were selected which are most likely to accumulate in closed environments, such as submarines or long-duration manned space flights. Absorption coefficients at CO2 laser wavelengths were measured, accurate to + 3 per cent or better, for each of these species. This data base was then used to determine the presence and concentration of the contaminants in prepared mixtures of 12 to 15 gases. Computer programs have been developed which will permit a real-time analysis of the monitored atmosphere. Minimum detectable concentrations for individual species are generally in the ppm range, and are not seriously degraded by interferences even in complex mixtures. Estimates of the dynamic range of this monitoring technique for various system configurations and comparison with other methods of analysis are discussed

Green, B. D.↗

The potential impact on atmospheric ozone and temperature of increasing trace gas concentrations

The response of the atmosphere to emission of chlorofluorocarbons and other chlorocarbons and to increasing concentrations of other radiatively active trace gases is calculated using a coupled, one-dimensional, time-dependent chemical-radiative-transport model. The model predicts future changes in the ozone content and in the temperature based on several possible time-dependent scenarios of future atmospheric emissions. The sensitivity of the atmospheric responses to the values adopted for parameters such as the eddy diffusion coefficient for vertical transport and the atmospheric budget of nitrogen oxides is estimated and discussed.

Brasseur, Guy↗

The potential impact on atmospheric ozone and temperature of increasing trace gas concentrations

The response of the atmosphere to emissions of chlorofluorocarbons (CFCs) and other chlorocarbons, and to increasing concentrations of other radiatively active trace gases such as CO2, CH4, and N2O is calculated by a coupled chemical-radiative transport one-dimensional model. It is shown that significant reductions in the ozone concentration and in the temperature are expected in the upper stratosphere as a result of increasing concentrations of active chlorine produced by photodecomposition of the CFCs. The ozone content is expected to increase in the troposphere, as a consequence of increasing concentrations of methane and nitrogen oxides. Due to enhanced greenhouse effects, the Earth's surface should warm up by several degrees. The amplitude and even the sign of future changes in the ozone column are difficult to predict as they are strongly scenario-dependent. An early detection system to prevent noticeable ozone changes as a result of increasing concentrations of source gases should thus be based on a continuous monitoring of the ozone amount in the upper stratosphere rather than on measurements of the ozone column only. Measurements of NOx, Clx, and HOx are also required for unambiguous trend detection and interpretation.

Brasseur, G.↗

Correcting for Trace Gas Absorption When Retrieving Aerosol Optical Depth from Satellite Observations of Reflected Shortwave Radiation

Retrieving aerosol optical depth (AOD) from top-of-atmosphere (TOA) satellite measured radiance requires separating the aerosol signal from the total observed signal. Total TOA radiance includes signal from underlying surface and from atmospheric constituents such as aerosols, clouds and gases. Multispectral retrieval algorithms, such as the dark-target (DT) algorithm that operates upon Moderate Resolution Imaging Spectroradiometer (MODIS, onboard Terra and Aqua satellites) and Visible Infrared Imaging Radiometer Suite (VIIRS, onboard Suomi-NPP) sensors, use wavelength bands in "window" regions. However, while small, the gas absorptions in these bands are non-negligible and require correction. In this paper we use High-resolution TRANsmission (HITRAN) database and Line-by-Line Radiative Transfer Model (LBLRTM) to derive consistent gas corrections for both MODIS and VIIRS wavelength bands. Absorptions from H2O, CO2 and O3 are considered, as well as other trace gases. Even though MODIS and VIIRS bands are "similar", they are different enough that applying MODIS specific gas corrections to VIIRS observations results in an underestimate of global mean AOD (by 0.01), but with much larger regional AOD biases up to 0.07. As recent studies are attempting to create a long-term data record by joining multiple satellite datasets, including MODIS and VIIRS, the consistency of gas correction becomes even more crucial.

Satellite Remote Sensing↗

Trace Gas Transport in the Arctic Vortex Inferred from ATMOS ATLAS-2 Observations During April 1993

Measurements of the long-lived tracers CH4, N2O, and HF from the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during the Atmospheric Laboratory for Science and Applications-2 (ATLAS-2) Space Shuttle mission in April 1993 are used to infer average winter descent rates ranging from 0.8 km/month at 20 km to 3.2 km/month at 40 km in the Arctic polar vortex during the 1992-93 winter. Descent rates in the mid-stratosphere are similar to those deduced for the Antarctic vortex using ATMOS/ATLAS-3 measurements in November 1994, but the shorter time period of descent in the Arctic leads to smaller total distances of descent. Strong horizontal gradients observed along the vortex edge indicate that the Arctic vortex remains a significant barrier to transport at least until mid-April in the lower to middle stratosphere.

Abrams, M. C.↗