Advancing Regional Air Quality and Atmospheric Composition Analysis: Introducing the TRACER-1 Tropospheric Regional Atmospheric Composition and Emissions Reanalysis
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NASA Ames Research Center is collaborating with the NOAA Chemical Systems Laboratory (NOAA/CSL), the NASA Jet Propulsion Laboratory (JPL), the NASA Goddard Modeling and Assimilation Office, and the National Center for Atmospheric Research to prepare a 20-year Tropospheric Regional Atmospheric Composition and Emissions Reanalysis (2005 – 2024) (TRACER-I) for the continental United States during the summer ozone (O3) and wildfire seasons (April to October). TRACER-I will be a regional complement to JPL’s global Tropospheric Chemistry Reanalyses II and III. We will use WRF-Chem/DART with NOAA/CSL’s WRF-Chem setup at 12 km x 12 km horizontal resolution, 51 vertical levels, and 30 ensemble members. We will assimilate: (i) conventional meteorological observations; (ii) EPA’s Air Quality System in situ measurements of carbon monoxide (CO), O3, nitrogen dioxide (NO2), sulfur dioxide (SO2), particulate matter (PM) with diameters less than 10 µm (PM10), and PM with diameters less than 2.5 µm (PM2.5); and (iii) MOPITT, MODIS, OMI, TROPOMI, GOME-2a, MLS, TES, SCIAMACHY, CrIS, and TEMPO total/partial column and/or profile retrievals of CO, O3, NO2, SO2, aerosol optical depth (AOD), formaldehyde (HCHO), ammonia (NH4), peroxyacetyl nitrate (PAN), and/or nitric acid (HNO3) with 3-hr cycling. We will present an overview of this project, its status, and available results (likely the analysis of sensitivity experiment results from the assimilation/emissions estimation system).
Atmospheric conditions for growth of ice crystals (temperature and ice supersaturation) are often not well constrained and it is necessary to simulate such conditions in the laboratory to investigate such growth under well controlled conditions over many hours. The growth of ice crystals from the vapour in both prism and basal planes was observed at temperatures of -60 C and -70 C under ice supersaturation up to 100% (200% relative humidity) at pressures derived from the standard atmosphere in a static diffusion chamber. Crystals grew outward from a vertical glass filament, thickening in the basal plane by addition of macroscopic layers greater than 2 microns, leading to growth in the prism plane by passing of successive layers conveniently viewed by time lapse video.
Titan, after Venus, is the second example in the solar system of an atmosphere with a global cyclostrophic circulation. The origin and maintenance of these superrotating atmospheres is not well understood, but Titan has a strong seasonal modulation in the middle atmosphere, and the seasonal changes in the winds may offer clues. The pole in winter and early spring is characterized by temperatures 20-30 K cooler at 140-170 km than those at low latitudes, and strong circumpolar winds as high as 190 m/s at 200- 250 km. At these levels the polar region is characterized by enhanced concentrations of several organic gases, and also detectable condensates. All this suggests that the polar vortex provides a mixing barrier between winter polar and lower-latitude air masses, analogous to the polar ozone holes on Earth. Because the concentrations of organic gases increase with altitude in the middle atmosphere, the observed enhancements suggest subsidence over the winter pole. Consistent with this are the observed temperatures approximately 200 K at the winter-polar stratopause (280 km), making it the warmest part of the atmosphere. The warm stratopause likely results from adiabatic heating associated with the subsidence. Recent observations in late northern winter and early spring indicate that the warm anomaly at the winter-polar stratopause is weakening;. In contrast to the middle atmosphere, latitude contrasts in tropospheric temperatures are muted. During the northern winter season, they were approximately 5 K at the tropopause and 3 K or less near the surface, being coldest at high northern latitudes. This is understandable in terms of the long radiative relaxation times in the troposphere, compared to times that are much shorter than a season in the upper stratosphere and higher. Curiously, the transition between the small meridional contrast (and presumably seasonal variations) in temperatures observed in the troposphere and the large variations observed at higher altitudes occurs abruptly above 80 km. Here the temperatures in the lower stratosphere, generally increasing with altitude, exhibit a sudden drop with increasing altitude at high northern latitudes, producing the contrast between low and high northern winter latitudes in the upper stratosphere described above. While the radiative relaxation time associated with infrared gaseous coolants decreases with altitude in the stratosphere, the abrupt transition suggests the presence of an optically thick condensate at thermal-infrared wavelengths. Near the surface, temperature lapse rates are adiabatic over the lowest 2 km, with the suggestion of a nocturnal stable inversion over the lowest 200 m in radio-occultation soundings near the morning terminator. At mid and high latitudes in both winter and summer hemispheres, the profiles are more statically stable (i.e., subadiabatic). This is most pronounced in the winter hemisphere.
The main findings of this research project have been the following: (1) there is a significant feedback from the stratosphere on tropospheric dynamics, and (2) a detailed analysis of the interaction between tropical and polar wave breaking in controlling stratospheric mixing. Two papers are were written and are included. The first paper is titled, "A New Perspective on the Dynamical Link Between the Stratosphere and Troposphere." Atmospheric processes of tropospheric origin can perturb the stratosphere, but direct feedback in the opposite direction is usually assumed to be negligible, despite the troposphere's sensitivity to changes in the release of wave activity into the stratosphere. Here, however, we present evidence that such a feedback exists and can be significant. We find that if the wintertime Arctic polar stratospheric vortex is distorted, either by waves propagating upward from the troposphere or by eastward-travelling stratospheric waves, then there is a concomitant redistribution of stratospheric potential vorticity that induces perturbations in key meteorological fields in the upper troposphere. The feedback is large despite the much greater mass of the troposphere: it can account for up to half of the geopotential height anomaly at the tropopause. Although the relative strength of the feedback is partly due to a cancellation between contributions to these anomalies from lower altitudes, our results imply that stratospheric dynamics and its feedback on the troposphere are more significant for climate modelling and data assimilation than was previously assumed. The second article is titled "Diagnosing the Polar Excitation of Subtropical Waves in the Stratosphere". The poleward migration of planetary scale tongues of subtropical air has often been associated with intense polar vortex disturbances in the stratosphere. This question of vortex influence is reexamined from a potential vorticity (PV) perspective. Anomalous geopotential height and wind fields associated solely with vortex PV anomalies are derived and their impact on the stratospheric subtropical circulation is evaluated. Combined PV inversion and Contour Advection (CA) calculations indicate that transient large scale disturbances of the polar vortex do have a far reaching impact that extends beyond the midlatitude surf zone all the way to the subtropics. This vortex influence is clearly non-local so that even simple wave 2 distortions that leave the vortex well confined within the midlatitudes are observed to excite subtropical waves. Treating subtropical PV as active tracers also showed that upon entrainment, these large scale tongues of low PV air also influenced the dynamics of their own poleward migration.
The EOS-Aura atmospheric chemistry mission is scheduled for launch in June 2004. Aura is the third of the large EOS observatories. The spacecraft carries an international instrument payload that has a planned six year lifetime. The Aura mission will collect data to help answer stratospheric and tropospheric atmospheric chemistry questions. The mission has the following four major objectives: 1) Track the ozone layer to determine if it is recovering as predicted. The four Aura instruments, HIRDLS, OMI, MLS, and TES will measure ozone, key source, radical, reservoir, tracer gases, and aerosols. Aura's unique design allows for major ozone controlling gases to be measured within the same air mass within a few minutes. The OMI instrument will continue the trends fiom NASA's TOMS series. 2) Track tropospheric pollutant sources and measure tropospheric ozone precursors. Major pollution sources include urban, industrial and biomass burning regions. Tropospheric trace gases will be measured, using TES and OMI, at an average spatial resolution of about approximately 15 km with near global coverage. 3) Measure key upper tropospheric atmospheric constituents that influence climate. The Aura instruments will monitor O3, H2O, CO, cirrus ice, and aerosols. EOS-Aura will fly in a sun-synchronous polar orbit about 15 minutes behind Aqua and make near coincident and synergistic measurements with the EOS- Aqua, Cloudsat, OCO, PARASOL and Calipso missions. Aura launched July 15,2004.
The EOS-Aura atmospheric chemistry mission is scheduled for launch in June 2004. Aura is the third of the large EOS observatories. The spacecraft carries an international instrument payload that has a planned six year lifetime. The Aura mission will collect data to help answer stratospheric and tropospheric atmospheric chemistry questions. The mission has the following four major objectives: 1) Track the ozone layer to determine if it is recovering as predicted. The four Aura instruments, HIRDLS, OMI, MLS, and TES will measure ozone, key source, radical, reservoir, tracer gases, and aerosols. Aura's unique design allows for major ozone controlling gases to be measured within the same air mass within a few minutes. The OMI instrument will continue the trends from NASA's TOMS series. 2) Track tropospheric pollutant sources and measure tropospheric ozone precursors. Major pollution sources include urban, industrial and biomass burning regions. Tropospheric trace gases will be measured, using TES and OMI, at an average spatial resolution of about approx. 15 km with near global coverage. 3) Measure key upper tropospheric atmospheric constituents that influence climate. The Aura instruments will monitor O3, H2O, CO, cirrus ice, and aerosols. EOS-Aura will fly in a sun-synchronous polar orbit about 15 minutes behind Aqua and make near coincident and synergistic measurements with the EOS-Aqua, Cloudsat, OCO, PARASOL and Calipso missions. Aura launched July 15,2004.
Research supported under this grant was aimed at attacking unanswered scientific questions that lie at the intersection of radiation, dynamics, chemistry, and climate. Considerable emphasis was placed on scientific collaboration and the innovative development of instruments required to address these issues. Specific questions include water vapor distribution in the tropical troposphere, atmospheric radiation, thin cirrus clouds, stratosphere-troposphere exchange, and correlative science with satellite observations.
The effect of tropospheric aerosols on atmospheric infrared cooling rates is investigated by the use of recent models of infrared gaseous absorption. A radiative model of the atmosphere that incorporates dust as an absorber and scatterer of infrared radiation is constructed by employing the exponential kernel approximation to the radiative transfer equation. Scattering effects are represented in terms of a single scattering albedo and an asymmetry factor. The model is applied to estimate the effect of an aerosol layer made of spherical quartz particles on the infrared cooling rate. Calculations performed for a reference wavelength of 0.55 microns show an increased greenhouse effect, where the net upward flux at the surface is reduced by 10% owing to the strongly enhanced downward emission. There is a substantial increase in the cooling rate near the surface, but the mean cooling rate throughout the lower troposphere was only 10%.
This work focuses on determining the latitudinal structure of ammonia vapor in Saturn's cloud layer near 1.5 bars using the brightness temperature maps derived from the Cassini RADAR (Elachi et al., 2004) instrument, which works in a passive mode to measure thermal emission from Saturn at 2.2-cm wavelength. We perform an analysis of five brightness temperature maps that span epochs from 2005 to 2011, which are presented in a companion paper by Janssen et al. (2013a, this issue). The brightness temperature maps are representative of the spatial distribution of ammonia vapor, since ammonia gas is the only effective opacity source in Saturn's atmosphere at 2.2-cm wavelength. Relatively high brightness temperatures indicate relatively low ammonia relative humidity (RH), and vice versa. We compare the observed brightness temperatures to brightness temperatures computed using the Juno atmospheric microwave radiative transfer (JAMRT) program which includes both the means to calculate a tropospheric atmosphere model for Saturn and the means to carry out radiative transfer calculations at microwave frequencies. The reference atmosphere to which we compare has a 3x solar deep mixing ratio of ammonia (we use 1.352x10(exp -4) for the solar mixing ratio of ammonia vapor relative to H2; see Atreya, 2010) and is fully saturated above its cloud base. The maps are comprised of residual brightness temperatures-observed brightness temperature minus the model brightness temperature of the saturated atmosphere.
The objective of this work was to attack unanswered questions that lie at the intersection of radiation, dynamics, chemistry and climate. Considerable emphasis was placed on scientific collaboration and the innovative development of instruments required to address these scientific issues. The specific questions addressed include: Water vapor distribution in the Tropical Troposphere: An understanding of the mechanisms that dictate the distribution of water vapor in the middle-upper troposphere; Atmospheric Radiation: In the spectral region between 200 and 600/cm that encompasses the water vapor rotational and continuum structure, where most of the radiative cooling of the upper troposphere occurs, there is a critical need to test radiative transfer calculations using accurate, spectrally resolved radiance observations of the cold atmosphere obtained simultaneously with in situ species concentrations; Thin Cirrus: Cirrus clouds play a central role in the energy and water budgets of the tropical tropopause region; Stratosphere-Troposphere Exchange: Assessment of our ability to predict the behavior of the atmosphere to changes in the boundary conditions defined by thermal, chemical or biological variables; Correlative Science with Satellite Observations: Linking this research to the developing series of EOS observations is critical for scientific progress.
The primary objective of this project was to apply the tropospheric atmospheric radon (Rn222) measurements to the development and verification of the global 3-D atmospheric chemical transport model under development by NASA's Atmospheric Effects of Aviation Project (AEAP). The AEAP project had two principal components: (1) a modeling effort, whose goal was to create, test and apply an elaborate three-dimensional atmospheric chemical transport model (the NASA/AEAP Core model to an evaluation of the possible short and long-term effects of aircraft emissions on atmospheric chemistry and climate--and (2) a measurement effort, whose goal was to obtain a focused set of atmospheric measurements that would provide some of the observational data used in the modeling effort. My activity in this project was confined to the first of these components. Both atmospheric transport and atmospheric chemical reactions (as well the input and removal of chemical species) are accounted for in the NASA/AEAP Core model. Thus, for example, in assessing the effect of aircraft effluents on the chemistry of a given region of the upper troposphere, the model must keep track not only of the chemical reactions of the effluent species emitted by aircraft flying in this region, but also of the transport into the region of these (and other) species from other, remote sources--for example, via the vertical convection of boundary layer air to the upper troposphere. Radon, because of its known surface source and known radioactive half-life, and freedom from chemical production or loss, and from removal from the atmosphere by physical scavenging, is a recognized and valuable tool for testing the transport components of global transport and circulation models.
The Tropospheric Emission Spectrometer (TES) is an infrared, high spectral resolution Fourier transform spectrometer with a 3.3 to 15.4 micron wavelength coverage. TES is a scanning instrument intended for determining the chemical state of the Earth's lower atmosphere (troposphere) from the surface to 30+ km. TES produces vertical profiles of important pollutant and greenhouse gases such as carbon monoxide, ozone, methane, and water vapor on a global scale every other day. TES was launched into orbit onboard NASA's earth Observing System Aura spacecraft on July 15, 2004 from Vandenberg Air Force Base, California.
The GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS) was developed at NASA’s Goddard Space Flight Center (GSFC) and has flown in multiple field campaigns to perform mapping of the regional-scale EPA criteria pollutants nitrogen dioxide, ozone, and formaldehyde. GCAS will also participate invalidation campaigns for NASA’s Tropospheric Emissions: Monitoring POllution (TEMPO) mission and the Korean Geostationary Environment Monitoring Spectrometer (GEMS) mission, both scheduled to launch in the early 2020s. GCAS houses two commercial Offner-type grating spectrometers that measure backscattered solar spectral radiance from the near-ultraviolet to near-infrared at high spatial resolution (typically 250 meters at 8.5 kilometer altitude). These radiances are used to retrieve spatial and temporal distributions of trace gases relevant to the boundary layer and free tropospheric atmospheric chemistry cycles. In this paper, we describe the field calibration techniques employed to characterize the spectral and temporal radiometric stability of the system during its most recent deployment in the 2018 Long Island Sound Trace Ozone Study (LISTOS) field campaign. Overall measurement uncertainty, retrieval impacts, and lessons learned for future deployments will also be described.
In determining the global methane budget the sources of methane must be balanced with the sinks and atmospheric inventory. The approximate contribution of the different methane sources to the budget has been establish showing the major terrestrial inputs as rice, wetlands, bogs, fens, and tundra. Measurements and modeling of production in these sources suggest that temperature, water table height and saturation along with substratum composition are important in controlling methane production and emission. The isotopic budget of 13 C and D/H in methane can be used as a tool to clarify the global budget. This approach has achieved success at constraining the inputs. Studies using the isotopic approach place constraints on global methane production from different sources. Also, the relation between the two biogenic production pathways, acetate fermentation and CO2 reduction, and the effect of substratum composition can be made using isotope measurements shows the relation between the different biogenic, thermogenic and anthropogenic sources of methane as a function of the carbon and hydrogen isotope values for each source and the atmosphere, tropospheric composition. Methane emissions from ponds and fens are a significant source in the methane budget of the boreal region. An initial study in 1993 and 1994 on the isotopic composition of this methane source and the isotopic composition in relation to oxidation of methane at the sediment surface of the ponds or fen was conducted as part of our BOREAS project. The isotopic composition of methane emitted by saturated anoxic sediment is dependent on the sediment composition and geochemistry, but will be influenced by in situ oxidation, in part, a function of rooted plant activity. The influence of oxidation mediated by rooted plant activities on the isotopic composition of methane is not well known and will depend on the plant type, sediment temperature, and numerous other variables. Information on this isotopic composition is important in both understanding the bio-geochemistry of the system and also in determining the regional and global inputs for the methane isotope budget. In determining the destruction of methane for balancing the atmospheric methane budget soil oxidation must be considered.
A photochemical model for the atmosphere of Jupiter, including 1-D vertical eddy diffusive transport, was developed. It extends from the upper troposphere through the homopause. The hydrocarbon chemistry involves species containing up to four carbon atoms (and polyynes through C8H2). The calculations show that a large fraction of photochemical carbon may be contained in molecules with more than two carbon atoms. At the tropopause, C2H6 is the major photochemical species and C2H2, C3H8, and C4H10 are of comparable abundance and down from C2H6 by a factor of ten. These species may be detectable with the mass spectrometer of the Galileo Probe. The vertical distributions of the photochemical species are sensitive to the magnitude of eddy diffusive mixing in the troposphere and stratosphere and the details of the interface region.
The thermal structure of Titan's atmosphere is reviewed, with particular emphasis on recent Cassini-Huygens results. Titan's has a similar troposphere-stratosphere-mesosphere pattern like Earth, but with a much more extended atmosphere, because of the weaker gravity, and also much lower temperatures, because of its greater distance from the sun. Titan's atmosphere exhibits an unusually large range in radiative relaxation times. In the troposphere, these are long compared to seasonal time scales, but in the stratosphere they are much shorter than a season. An exception is near the winter pole, where the stratospheric relaxation times at 100-170 km become comparable to the seasonal time scale; at the warm stratopause, they are comparable to a Titan day. Hence, seasonal behavior in the troposphere should be muted, but significant in the stratosphere. This is reflected in the small meridional contrast observed in temperatures in the troposphere and the large stratospheric contrasts noted above. A surprising feature of the vertical profiles of temperature is the abrupt transition between these regimes in at high northern latitudes in winter, where the temperatures in the lower stratosphere exhibit a sudden drop with increasing altitude. This could be a radiative effect, not associated with spatial variations in gaseous opacity, but rather from an optically thick condensate at thermal-infrared wavelengths. A curious aspect of Titan's middle atmosphere is that the axis of symmetry of the temperature field is tilted by several degrees relative to the rotational axis of the moon itself. Whether this is driven by solar heating or gravitational perturbations is not known. Titan's surface exhibits weak contrasts in temperature, approximately 3 K in the winter hemisphere. At low latitudes, there is evidence of a weak nocturnal boundary layer on the morning terminator, which is not radiatively controlled, but can be explained in terms of vertical mixing with a small eddy viscosity.