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Rinsland, C. P.

Publications and source records attributed to Rinsland, C. P..

At least 19 records

Hydrogen Cyanide in the Upper Troposphere: GEM-AQ Simulation and Comparison with ACE-FTS Observations

We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the threedimensional Gobal multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004-2006 on a 1.5deg x 1.5deg global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May-July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. The comparison with the satellite data shows that in the upper troposphere GEM-AQ perform7s well globally for all seasons, except at northern hi gh and middle latitudes in surnmer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, includin g the interannual variations in the observed mixing ratio. A complementary comparison with daily total columns of HCN from two middle latitude ground-based stations in Northern Japan for the same simulation period shows that the model captures the observed seasonal variation and also points to an underestimation of model emissions in the Northern Hemisphere in the summer. The estimated average global emission equals 1.3 Tg N/yr. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.

Lupu, A.

Tropospheric Vertical Distribution of Tropical Atlantic Ozone Observed by TES during the Northern African Biomass Burning Season

We present vertical distributions of ozone from the Tropospheric Emission Spectrometer (TES) over the tropical Atlantic Ocean during January 2005. Between 10N and 20S, TES ozone retrievals have Degrees of Freedom for signal (DOF) around 0.7 - 0.8 each for tropospheric altitudes above and below 500 hPa. As a result, TES is able to capture for the first time from space a distribution characterized by two maxima: one in the lower troposphere north of the ITCZ and one in the middle and upper troposphere south of the ITCZ. We focus our analysis on the north tropical Atlantic Ocean, where most of previous satellite observations showed discrepancies with in-situ ozone observations and models. Trajectory analyses and a sensitivity study using the GEOS-Chem model confirm the influence of northern Africa biomass burning on the elevated ozone mixing ratios observed by TES over this region.

satellite observations

Infrared Solar Spectroscopic Measurements of Free Tropospheric CO, C2H6, and HCN above Mauna Loa, Hawaii: Seasonal Variations and Evidence for Enhanced Emissions from the Southeast Asian Tropical Fires of 1997-1998

High spectral resolution (0.003 per cm) infrared solar absorption measurements of CO, C2H6, and HCN have been recorded at the Network for the Detection of Stratospheric Change station on Mauna Loa, Hawaii, (19.5N, 155.6W, altitude 3.4 km). The observations were obtained on over 250 days between August 1995 and February 1998. Column measurements are reported for the 3.4-16 km altitude region, which corresponds approximately to the free troposphere above the station. Average CO mixing ratios computed for this layer have been compared with flask sampling CO measurements obtained in situ at the station during the same time period. Both show asymmetrical seasonal cycles superimposed on significant variability. The first 2 years of observations exhibit a broad January-April maximum and a sharper CO minimum during late summer. The C2H6 and CO 3.4-16 km columns were highly correlated throughout the observing period with the C2H6/CO slope intermediate between higher and lower values derived from similar infrared spectroscopic measurements at 32'N and 45'S latitude, respectively. Variable enhancements in CO, C2H6, and particularly HCN were observed beginning in about September 1997. The maximum HCN free tropospheric monthly mean column observed in November 1997 corresponds to an average 3.4-16 km mixing ratio of 0.7 ppbv (1 ppbv = 10(exp -9) per unit volume), more than a factor of 3 above the background level. The HCN enhancements continued through the end of the observational series. Back-trajectory calculations suggest that the emissions originated at low northern latitudes in southeast Asia. Surface CO mixing ratios and the C2H6 tropospheric columns measured during the same time also showed anomalous autumn 1997 maxima. The intense and widespread tropical wild fires that burned during the strong El Nino warm phase of 1997- 1998 are the likely source of the elevated emission products.

Rinsland, C. P.

Observations of the Infrared Solar Spectrum from Space by the ATMOS Experiment

The final flight of the Atmospheric Trace Molecule Spectroscopy experiment as part of the Atmospheric na Laboratory for Applications and Science (ATLAS-3) Space Shuttle mission in 1994 provided a new opportunity to measure broadband 625-4800/ cm, 2.1 - 16 micron infrared solar spectra at an unapodized resolution of 0.0l/ cm from space. The majority of the observations were obtained as exoatmospheric, of near Sun center, absorption spectra, which were later ratioed to grazing atmospheric measurements to compute the atmospheric transmission of the Earth's atmosphere and analyzed for vertical profiles of minor and trace gases. Relative to the SPACELAB-3 mission that produced 4800 high Sun spectra (which were averaged into four grand average spectra), the ATLAS-3 mission produced some 40,000 high Sun spectra (which have been similarly averaged) with an improvement in signal-to-noise ratio of a factor of 3-4 in the spectral region between 1000 and 4800/ cm. A brief description of the spectral calibration and spectral quality is given as well as the location of electronic archives of these spectra.

Abrams, M. C.

Polar Stratospheric Descent of NO(y) and CO and Arctic Denitrification During Winter 1992-1993

Observations inside the November 1994 Antarctic stratospheric vortex and inside the April 1993 remnant Arctic stratospheric vortex by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer are reported. In both instances, elevated volume mixing ratios (VMRS) of carbon monoxide (CO) were measured. A peak Antarctic CO VMR of 60 ppbv (where 1 ppbv = 10(exp -9) per unit Volume) was measured at a potential temperature of 710 K (about 27 km), about 1 km below the altitude of a pocket of elevated NO(y) (total reactive nitrogen) at a deep minimum in N2O (<5 ppbv). The Arctic observations also show a region of elevated vortex CO with a peak VMR of 90 ppbv it 630-670 K (-25 km) but no corresponding enhancement in NO(sub y) perhaps because of stronger dynamical activity in the northern hemisphere polar winter and/or interannual variability in the production of mesospheric or lower thermospheric NO. By comparing vortex and extravortex observations of NO(y) obtained at the same N2O VMR, Arctic vortex denitrification of 5 +/- 2 ppbv at 470 K (at approximately 18 km) is inferred. We show that our conclusion of substantial Arctic winter 1992-1993 denitrification is robust by comparing our extravortex observations with previous polar measurements obtained over a wide range of winter conditions. Correlations of NO(y) with N2O measured at the same potential temperature by ATMOS in the Arctic vortex and at midlatitudes on board the ER-2 aircraft several weeks later lie along the same mixing line. The result demonstrates the consistency of the two data sets and confirms that the ER-2 sampled fragments of the denitrified Arctic vortex following its breakup. An analysis of the ATMOS Arctic measurements of total hydrogen shows no evidence for significant dehydration inside the vortex.

Rinsland, C. P.

Infrared Solar Spectroscopic Measurements of Free Tropospheric CO, C2H6, and HCN above Mauna Loa, Hawaii: Seasonal Variations and Evidence for Enhanced Emissions from the Southeast Asian Fires of 1997-1998

High spectral resolution (0.003/ cm) infrared solar absorption measurements of CO, C2H6, and HCN have been recorded at the Network for the Detection of Stratospheric Change station on Mauna Loa, Hawaii, (19.5 deg N, 155.6 deg W, altitude 3.4 km). The observations were obtained on over 250 days between August 1995 and February 1998. Column measurements are reported for the 3.4 - 16 km altitude region, which corresponds approximately to the free troposphere above the station. Average CO mixing ratios computed for this layer have been compared with flask sampling CO measurements obtained in situ at the station during the same time period. Both show asymmetrical seasonal cycles superimposed on significant variability. The first two years of observations exhibit a broad January-April maximum and a sharper CO minimum during late summer. The C2H6 and CO 3.4 - 16 km columns were highly correlated throughout the observing period with the C2H6/CO slope intermediate between higher and lower values derived from similar infrared spectroscopic measurements at 32 deg N and 45 deg S latitude, respectively. Variable enhancements in CO, C2H6, and particularly HCN were observed beginning in about September 1997. The maximum HCN free tropospheric monthly mean column observed in November 1997 corresponds to an average 3.4 - 16 km mixing ratio of 0.7 ppbv (1 ppbv = 10(exp -9) per unit volume), more than a factor of 3 above the background level. The HCN enhancements continued through the end of the observational series. Back-trajectory calculations suggest that the emissions originated at low northern latitudes in southeast Asia. Surface CO mixing ratios and the C2H6 tropospheric columns measured during the same time also showed anomalous autumn 1997 maxima. The intense and widespread tropical wild fires that burned during 3 the strong El Nino warm phase of 1997-1998 are the likely source of the elevated emission products.

Rinsland, C. P.

Correlations of Stratospheric Abundances of CH4 and N2O Derived from ATMOS Measurements

Atmospheric Trace MOlecule Spectroscopy (ATMOS) measurements made over a wide range of altitudes and latitudes demonstrate compact correlations between mixing ratios of CH, and N,O. Tight but distinct correlations are observed for the tropics, the springtime Arctic vortex, and the extra-tropics/extra-vortex regions, indicating dynamical isolation between these regions. Little variability is apparent in correlations between CH4 and N20 from measurements made in different years (1992, 1993, and 1994), seasons (March/April and November), and hemispheres.

Rinsland, C. P.

Atmos/Atlas 3 Infrared Profile Measurements of Clouds in the Tropical and Subtropical Upper Troposphere

Vertical profiles of infrared cirrus extinction have been derived from tropical and subtropical upper tropospheric solar occultation spectra. The measurements were recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Sciences (ATLAS) 3 shuttle flight in November 1994. The presence of large numbers of small ice crystals is inferred from the appearance of broad extinction features in the 8-12 micron region. These features were observed near the tropopause and at lower altitudes. Vertical profiles of the ice extinction (/km) in microwindows at 831, 957, and 1204/cm have been retrieved from the spectra and analyzed with a model for randomly oriented spheroidal ice crystals. An area-equivalent spherical radius of 6 gm is estimated from the smallest ice crystals observed in the 8-12 micron region. Direct penetration of clouds into the lower stratosphere is inferred from observations of cloud extinction extending from the upper troposphere to 50 mbar (20 km altitude). Cloud extinction between 3 and 5 micron shows very little wavelength dependence, at least for the cases observed by the ATMOS instrument in the tropics and subtropics during ATLAS 3.

Rinsland, C. P.

Atmos/Atlas 3 Infrared Profile Measurements of Trace Gases in The November 1994 Tropical and Subtropical Upper Troposphere

Vertical mixing ratio profiles of four relatively long-lives gases, HCN, C2H2, CO, and C2H6, have been retrieved from 0.01/cm resolution infrared solar occultation spectra recorded between latitudes of 5.3degN and 31.4degN. The observations were obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Science (ATLAS) 3 shuttle flight, 3-12 November 1994. Elevated mixing ratios below the tropopause were measured for these gases during several of the occultations. The positive correlations obtained between the simultaneously measured mixing ratios suggest that the enhancements are likely the result of surface emissions, most likely biomass burning and/or urban industrial activities, followed by common injection via deep convective transport of the gases to the upper troposphere. The elevated levels of HCN may account for at least part of the "missing NO," in the upper troposphere. Comparisons of the observations with values measured during a recent aircraft campaign are presented.

Rinsland, C. P.

ATMOS/ATLAS 3 Infrared Profile Measurements of Clouds in the Tropical and Subtropical Upper Troposphere

Vertical profiles of infrared cirrus extinction have been derived from tropical and subtropical upper tropospheric solar occultation spectra. The measurements were recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Sciences (ATLAS) 3 shuttle flight in November 1994. The presence of large numbers of small ice crystals is inferred from the appearance of broad extinction features in the 8-12 micron region. These features were observed near the tropopause and at lower altitudes. Vertical profiles of the ice extinction (/km) in microwindows at 831, 957, and 1204/cm have been retrieved from the spectra and analyzed with a model for randomly oriented spheroidal ice crystals. An area-equivalent spherical radius of 6 microns is estimated from the smallest ice crystals observed in the 8-12 gm region. Direct penetration of clouds into the lower stratosphere is inferred from observations of cloud extinction extending from the upper troposphere to 50 mbar (20 km altitude). Cloud extinction between 3 and 5 microns shows very little wavelength dependence, at least for the cases observed by the ATMOS instrument in the tropics and subtropics during ATLAS 3.

Rinsland, C. P.

Spectroscopic Parameters for Ozone and its Isotopes: Current Status, Prospects for Improvement, and the Identification of 16O16O17O and O-16O-16O-17 and O-16O-17O-16 Lines in Infrared Ground-Based and Stratospheric Solar Absorption Spectra

We describe the updates to the spectroscopic parameters of ozone and its isotopes in the 1996 HITRAN compilation. Recent published studies not included in HITRAN are also summarized. Finally, we report the identification of infrared lines of the v(sub 3) bands of O-16O-16O-17 and O-16O-17O-16 in high-resolution solar spectra recorded by stratospheric balloon-borne and ground-based Fourier transform spectrometers.

Rinsland, C. P.

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 +/- 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 +/- 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July-August.

Abbas, M. M.

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.

ATMOS/ATLAS-3 Observations of Long-Lived Tracers and Descent in the Antarctic Vortex in November 1994

Observations of the long-lived tracers N2O, CH4 and HF obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument in early November 1994 are used to estimate average descent rates during winter in the Antarctic polar vortex of 0.5 to 1.5 km/month in the lower stratosphere, and 2.5 to 3.5 km/month in the middle and upper stratosphere. Descent rates inferred from ATMOS tracer observations agree well with theoretical estimates obtained using radiative heating calculations. Air of mesospheric origin (N2O less than 5 ppbV) was observed at altitudes above about 25 km within the vortex. Strong horizontal gradients of tracer mixing ratios, the presence of mesospheric air in the vortex in early spring, and the variation with altitude of inferred descent rates indicate that the Antarctic vortex is highly isolated from midlatitudes throughout the winter from approximately 20 km to the stratopause. The 1994 Antarctic vortex remained well isolated between 20 and 30 km through at least mid-November.

Abrams, M. C.

Trends of OCS, HCN, SF6, CHClF2 (HCFC-22) in the Lower Stratosphere from 1985 and 1994 Atmospheric Trace Molecule Spectroscopy Experiment Measurements Near 30 deg. North Latitude

Volume mixing ratio (VMR) profiles of OCS, HCN, SF6, and CHClF2 (HCFC-22) have been measured near 30 deg N latitude by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer during shuttle flights on 29 April - 6 May 1985 and 3-2 November 1994. The change in the concentration of each molecule in the lower stratosphere has been derived for this 9 1/2-year period by comparing measurements between potential temperatures of 395 to 800 K (approximately 17 to 30 km altitude) relative to simultaneously measured values of the long-lived tracer N2O. Exponential rates of increase inferred for 1985-to 1994 from these comparisons are (0.1 plus or minus 0.4)% yr(exp-1) for OCS, (1.0 plus or minus 1.0)% yr(exp-1) for HCN, (8.0 +/- 0.7)% yr(exp-1) for SF6, and (8.0 +/- 1.0)% yr(exp-1) for CHClF2 (HCFC-22), 1 sigma. The lack of an appreciable trend for OCS suggests the background (i.e. nonvolcanic) source of stratospheric aerosol was the same during the two periods. These results are compared with trends reported in the literature.

Rinsland, C. P.

Increase of Stratospheric Carbon Tetrafluoride (CF4) Based on ATMOS Observations from Space

Stratospheric volume mixing ratio profiles of carbon tetrafluoride, CF4, obtained with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during the ATLAS (Atmospheric Laboratory for Applications and Science) -3 mission of 1994 are reported. Overall the profiles are nearly constant over the altitude range 20 to 50 km, indicative of the very long lifetime of CF4 in the atmosphere. In comparison to the stratospheric values of CF4 inferred from the ATMOS/Spacelab 3 mission of 1985, the 1994 concentrations are consistent with an exponential increase of (1.6 +/- 0.6)% yr(exp -1). This increase is discussed with regard to previous results and likely sources of CF4 at the ground. Further, it is shown that simultaneous measurements of N2O and CF4 provide a means of constraining the lower limit of the atmospheric lifetime of CF4 at least 2,300 years, two sigma.

Zander, R.

Stratospheric Chlorine partitioning: Constraints from Shuttle-borne Measurements of [HCl], [ClNO3] and [ClO]

Measured stratospheric mixing ratios of HCl, ClNO3, and ClO from ATMOS and MAS are poorly reproduced by models using recommended kinetic parameters. This discrepancy is not resolved by new rates for the reactions Cl+CH4 and OH+HCl derived from weighted fits to laboratory measurements. A deficit in modeled [HCl] and corresponding overprediction of [ClNO3] and [ClO], which increases with altitude, suggests that production of HCl between 20 and 50 km is much faster than predicted from recommended rates.

Michelsen, H. A.