Atmospheric trace gas rotational lineshape parameters near 600 GHz
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AURA-MLS mission atmospheric trace gases↗
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A WRF-Chem Analysis of Flash Rates, Lightning-NOx Production and Subsequent Trace Gas Chemistry of the 29-30 May 2012 Convective Event in Oklahoma During DC3
The Deep Convective Clouds and Chemistry (DC3) field campaign in 2012 provided a plethora of aircraft and ground-based observations (e.g., trace gases, lightning and radar) to study deep convective storms, their convective transport of trace gases, and associated lightning occurrence and production of nitrogen oxides (NOx). This is a continuation of previous work, which compared lightning observations (Oklahoma Lightning Mapping Array and National Lightning Detection Network) with flashes generated by various flash rate parameterization schemes (FRPSs) from the literature in a Weather Research and Forecasting Chemistry (WRF-Chem) model simulation of the 29-30 May 2012 Oklahoma thunderstorm. Based on the Oklahoma radar observations and Lightning Mapping Array data, new FRPSs are being generated and incorporated into the model. The focus of this analysis is on estimating the amount of lightning-generated nitrogen oxides (LNOx) produced per flash in this storm through a series of model simulations using different production per flash assumptions and comparisons with DC3 aircraft anvil observations. The result of this analysis will be compared with previously studied mid-latitude storms. Additional model simulations are conducted to investigate the upper troposphere transport, distribution, and chemistry of the LNOx plume during the 24 hours following the convective event to investigate ozone production. These model-simulated mixing ratios are compared against the aircraft observations made on 30 May over the southern Appalachians.
Cummings, Kristin A.↗
Stratospheric trace gas sampling with chemical absorption filters
Recent interest in stratospheric chemistry, sparked in part by the suggested roles of atomic chlorine (Cl) and nitrogen oxides (NOx) in the catalytic destruction of ozone (O3), has made sampling and measurement of trace constituents above the tropopause highly desirable. An ongoing research program in the In Situ Studies Project at the National Center for Atmospheric Research carries out aircraft and balloon-borne stratospheric chemical sampling at regular intervals by using chemically impregnated filters to collect particles and reactive gases.
Bonelli, J. E.↗
Cloud draft structure and trace gas transport
During the second Amazon Boundary Layer Experiment (ABLE 2B), meteorological observations, chemical measurements, and model simulations are utilized in order to interpret convective cloud draft structure and to analyze its role in transport and vertical distribution of trace gases. One-dimensional photochemical model results suggest that the observed poststorm changes in ozone concentration can be attributed to convective transports rather than photochemical production and the results of a two-dimensional time-dependent cloud model simulation are presented for the May 6, 1987 squall system. The mesoscale convective system exhibited evidence of significant midlevel detrainment in addition to transports to anvil heights. Chemical measurements of O3 and CO obtained in the convective environment are used to predict photochemical production within the troposphere and to corroborate the cloud model results.
Scala, John R.↗
Proposed Trace Gas Measurements Over the Western United States for TROPOMI Validation
The Alpha Jet Atmospheric eXperiment (AJAX), located in the Bay Area of California, is a joint effort between NASA Ames Research Center and H211, LCC. AJAX makes in-situ airborne measurements of trace gases 2-4 times per month, resulting in over 216 flights since 2011. Current measurements include ozone (O3), carbon dioxide (CO2), methane (CH4), water (H2O), formaldehyde (HCHO), and meteorological measurements (i.e., ambient pressure, temperature, and 3D winds). Currently, the AJAX team is working to incorporate nitrogen dioxide (NO2) measurements with a Cavity Attenuated Phase Shift Spectrometer (CAPS). Successful science flights coincident with satellite overpasses have been performed since 2011 by the Alpha Jet, with more than 40 flights under the Greenhouse Observing SATellite (GOSAT) and several flights under the Orbiting Carbon Observatory-2 (OCO-2). Results from these flights, which have covered a range of different surfaces and seasonal conditions, will be presented. In-situ vertical profiles of O3, CO2, CH4, H2O, HCHO, and NO2 from the surface to 28,000 feet made by AJAX will also be valuable for satellite validation of data products obtained from the TROPOspheric Montoring Instrument (TROPOMI). TROPOMI is on board the Copernicus Sentinel-5 precursor (S5p) satellite, with level 2 products including O3, CO, CH4, HCHO, NO2, and aerosols.
Parworth, Caroline L.↗
Design and Performance Assessment of a Stable Astigmatic Herriott Cell for Trace Gas Measurements on Airborne Platforms
The present paper discusses a new, more stable, astigmatic Herriott cell employing carbon fiber stabilizing rods. Laboratory tests using a near-IR absorption feature of CO at 1564.168-nm revealed a factor of two improvement in measurement stability compared with the present commercial design when the sampling pressure was changed by +/-2 Torr around 50 Torr. This new cell should significantly enhance our efforts to measure trace gases employing pathlengths of 100 to 200-meters on airborne platforms with minimum detectable line center absorbances of less than 10(exp -6).
Dyroff, Christoph↗
Warm Molecular Gas Traced with CO J = 7 --> 6 in the Galaxy's Central 2 Parsecs: Dynamical Heating of the Circumnuclear Disks
We present an 11" resolution map of the central 2 pc of the Galaxy in the CO J = 7 --> 6 rotational transition. The CO emission shows rotation about Sgr A* but also evidence for noncircular turbulent motion and a clumpy morphology. We combine our data set with available CO measurements to model the physical conditions in the disk. We find that the molecular gas in the region is both warm and dense, with T approx. 200-300 K and n(sub H2) approx. (5-7) x 10(exp 4) cm(exp -3). The mass of warm molecular gas we measure in the central 2 pc is at least 2000 M(solar), about 20 times the UV-excited atomic gas mass, ruling out a UV heating scenario for the molecular material. We compare the available spectral tracers with theoretical models and conclude that molecular gas is heated with magnetohydrodynamic shocks with v approx. 10-20 km s(exp -1) and B approx. 0.3- 0.5 mG. Using the conditions derived with the CO analysis, we include the other important coolants, neutral oxygen and molecular hydrogen, to estimate the total cooling budget of the molecular material. We derive a mass-to-luminosity ratio of approx. 2-3 M(solar)(L(solar)exp -1), which is consistent with the total power dissipated via turbulent decay in 0.1 pc cells with v(sub rms) approx. 15 kilometers per second. These size and velocity scales are comparable to the observed clumping scale and the velocity dispersion. At this rate, the material near Sgr A* is dissipating its orbital energy on an orbital timescale and cannot last for more than a few orbits. Our conclusions support a scenario in which the features near Sgr A* such as the circumnuclear disk and northern arm are generated by infalling clouds with low specific angular momentum.
galatic nuclei↗
Interpretation of Trace Gas Data Using Inverse Methods and Global Chemical Transport Models
This is a theoretical research project aimed at: (1) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for long lived gases important in ozone depletion and climate forcing, (2) utilization of inverse methods to determine these source/sink strengths which use the NCAR/Boulder CCM2-T42 3-D model and a global 3-D Model for Atmospheric Transport and Chemistry (MATCH) which is based on analyzed observed wind fields (developed in collaboration by MIT and NCAR/Boulder), (3) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple titrating gases, and, (4) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3-D models. Important goals include determination of regional source strengths of methane, nitrous oxide, and other climatically and chemically important biogenic trace gases and also of halocarbons restricted by the Montreal Protocol and its follow-on agreements and hydrohalocarbons used as alternatives to the restricted halocarbons.
Prinn, Ronald G.↗
Studies of Trace Gas Chemical Cycles Using Inverse Methods and Global Chemical Transport Models
We report progress in the first year, and summarize proposed work for the second year of the three-year dynamical-chemical modeling project devoted to: (a) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for long lived gases important in ozone depletion and climate forcing, (b) utilization of inverse methods to determine these source/sink strengths using either MATCH (Model for Atmospheric Transport and Chemistry) which is based on analyzed observed wind fields or back-trajectories computed from these wind fields, (c) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple titrating gases, and (d) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3D models. Important goals include determination of regional source strengths of methane, nitrous oxide, methyl bromide, and other climatically and chemically important biogenic/anthropogenic trace gases and also of halocarbons restricted by the Montreal protocol and its follow-on agreements and hydrohalocarbons now used as alternatives to the restricted halocarbons.
Prinn, Ronald G.↗
Atmospheric Trace Gas Abundances and Stable Isotope Ratios via IR-LIF
We propose to develop new technologies with support provided by PIDDP that will enable the in situ measurements of abundances and stable isotope ratios in important radiatively and biogenically active gases such as carbon dioxide, carbon monoxide, water, methane, nitrous oxide, and hydrogen sulfide to very high precision (0.1 per mil or better for the isotopic ratios, for example). Such measurements, impossible at present, could provide pivotal new constraints on the global (bio)geochemical budgets of these critical species, and could also be used to examine the dynamics of atmospheric transport on Mars, Titan, and other solar system bodies. We believe the combination of solid state light sources with imaging of the IR laser induced fluorescence (IR-LIF) via newly available detector arrays will make such in situ measurements possible for the first time. Even under ambient terrestrial conditions, the LIF yield from vibrational excitation of species such as water and carbon dioxide should produce emission measures well in excess of ten billion photons/sec from samples volumes of order 1 c.c. These count rates can, in principle, yield detection limits into the sub-ppt range that are required for the in situ isotopic study of atmospheric trace gases. While promising, such technologies are relatively immature, but developing rapidly, and there are a great many uncertainties regarding their applicability to in situ IR-LIF planetary studies. We therefore feel PIDDP support will be critical to developing these new tools, and propose a three-year program to combine microchip near-IR lasers with low background detection axes and state-of-the-art HgCdTe detectors developed for astronomical spectroscopy to investigate the sensitivity of IR-LIF under realistic planetary conditions, to optimize the optical pumping and filtering schemes for important species, and to apply the spectrometer to the non-destructive measurement of stable isotopes in a variety of test samples. These studies form the necessary precursors to the development of compact, lightweight stable isotope/trace gas sensors for future planetary missions.
Blake, Geoffrey A.↗
Dynamical and Trace Gas Responses of the Quasi-Biennial Oscillation to Historical and Future Climate Change
The Quasi-Biennial Oscillation (QBO) dominates the variability of the tropical stratosphere. The QBO can be seen in stratospheric zonal wind, temperature, and composition, but it also has a number of teleconnections—including to the polar vortices, extratropical surface winter climate, and the Madden-Julian Oscillation. Thus, its future trends will have a signature on the surface. Recent multi-model investigations (Richter et al. 2019, Butchart et al. 2020) suggest that a weakening of the QBO amplitude is very likely, but changes to QBO period and stability remain unclear, due in part to its highly parameterized nature. We investigate these aspects using multiple configurations of the NASA Goddard Institute for Space Studies Model E2.2 (Rind et al., 2020; Orbe et al. 2020). As a high-top model with gravity wave drag partly sourced from (parameterized) convection, Model E2.2 includes key pathways for climate forcings to influence the QBO. Overall, both the period and amplitude decrease in response to increased CO2, with convection feedbacks critical for the period response, and ozone feedbacks enhancing the amplitude response. We use these results to interpret QBO trends in the historical and SSP integrations. Lastly, we examine the effect of volcanic eruptions on the QBO
Quasi-Biennial Oscillation↗
Spatial and Temporal Variability of Trace Gas Columns Derived from WRF/Chem Regional Model Output: Planning for Geostationary Observations of Atmospheric Composition
We quantify both the spatial and temporal variability of column integrated O3, NO2, CO, SO2, and HCHO over the Baltimore / Washington, DC area using output from the Weather Research and Forecasting model with on-line chemistry (WRF/Chem) for the entire month of July 2011, coinciding with the first deployment of the NASA Earth Venture program mission Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Using structure function analyses, we find that the model reproduces the spatial variability observed during the campaign reasonably well, especially for O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) instrument will be the first NASA mission to make atmospheric composition observations from geostationary orbit and partially fulfills the goals of the Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission. We relate the simulated variability to the precision requirements defined by the science traceability matrices of these space-borne missions. Results for O3 from 0- 2 km altitude indicate that the TEMPO instrument would be able to observe O3 air quality events over the Mid-Atlantic area, even on days when the violations of the air quality standard are not widespread. The results further indicated that horizontal gradients in CO from 0-2 km would be observable over moderate distances (≥ 20 km). The spatial and temporal results for tropospheric column NO2 indicate that TEMPO would be able to observe not only the large urban plumes at times of peak production, but also the weaker gradients between rush hours. This suggests that the proposed spatial and temporal resolutions for these satellites as well as their prospective precision requirements are sufficient to answer the science questions they are tasked to address.
TEMPO↗
Apportionment and Inventory Optimization of Agriculture and Energy Sector Methane Emissions Using Multi‐Month Trace Gas Measurements in Northern Colorado
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Griffin J. Mead↗
A Geostatistical Framework for Quantifying the Imprint of Mesoscale Atmospheric Transport on Satellite Trace Gas Retrievals
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Anthony D. Torres↗
Deriving Tropospheric Transit Time Distributions Using Airborne Trace Gas Measurements: Uncertainty and Information Content
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Sofia M. Chelpon↗
Development of trace gas detection instrumentation
Breadboard hardware was constructed to demonstrate detection of a gaseous species by the heterodyne principle. The characteristics of the component parts were investigated and preliminary measurements were made to establish the sensitivity and selectivity of the method for gas analysis of CO, CO2, and N2O. A prototype heterodyne gas analyzer was designed, built, and brought into operational condition. Performance parameters of the prototype analyzer were investigated and its sensitivity to CO2 measured. Further development was undertaken for both the optical bench and the electronic processor components. A three-gas prototype analyzer, capable of measuring the gases CO, CO2, and CH4 was also constructed and tested. Detailed descriptions of the work and results are presented.
Source record↗
Dynamic delta method for trace gas analysis
Method has been developed in which measurements are made only over viscous flow range, eliminating fractionation before the molecular leak and problems due to surface elution.
Wood, G. M.↗
Effect of aerosol emission on the inference of trace gas concentrations from limb radiance data
This note reports on an analysis of atmospheric emission spectra in the 10-12 micron region measured with a limb-oriented balloon-borne spectrometer. Data clearly show the existence of an additional feature at 10.8 microns which is probably due to measurement contamination from aerosols. The 10.8 micron emitter has a strong reducing effect on the HNO3 mixing ratio profile as determined by application of a symmetrical band shape model to the 10.8 spectral feature.
Remsberg, E. E.↗