SEARCH · Search NASA

Results for “stratospheric halogen”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

SourceResearch connectionFrom yearThrough year

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 37 records · Page 2

All sources NASA NTRS DOE OSTI

NASA NTRS2008

On the Response of Halogen Occultation Experiment (HALOE) Stratospheric Oxone and Temperature to the 11-yr Solar Cycle Forcing

Results are presented on responses in 14-yr time series of stratospheric ozone and temperature from the Halogen Occultation Experiment (HALOE) of the Upper Atmosphere Research Satellite (UARS) to a solar cycle (SC-like) variation. The ozone time series are for ten, 20-degree wide, latitude bins from 45S to 45N and for thirteen "half-Umkehr" layers of about 2.5 km thickness and extending from 63 hPa to 0.7 hPa. The temperature time series analyses were restricted to pressure levels in the range of 2 hPa to 0.7 hPa. Multiple linear regression (MLR) techniques were applied to each of the 130 time series of zonally-averaged, sunrise plus sunset ozone points over that latitude/pressure domain. A simple, 11-yr periodic term and a linear trend term were added to the final MLR models after their seasonal and interannual terms had been determined. Where the amplitudes of the 11-yr terms were significant, they were in-phase with those of the more standard proxies for the solar uv-flux. The max minus min response for ozone is of order 2 to 3% from about 2 to 5 hPa and for the latitudes of 45S to 45N. There is also a significant max minus min response of order 1 K for temperature between 15S and 15N and from 2 to 0.7 hPa. The associated linear trends for ozone are near zero in the upper stratosphere. Negative ozone trends of 4 to 6%/decade were found at 10 to 20 hPa across the low to middle latitudes of both hemispheres. It is concluded that the analyzed responses from the HALOE data are of good quality and can be used to evaluate the responses of climate/chemistry models to a solar cycle forcing.

Remsberg, E. E.↗

NASA NTRS1979

Sulfur and halogen chemistry of the stratosphere and of volcanic eruption plumes

The major eruption of Volcan de Fuego caused an enhancement of 1.6 x 10 to the 9 kg of SO4(-) in the stratosphere 6 months after the eruption. Measurable changes in nitric acid vapor and particulate chloride were not observed. Subsequent data suggests that HCl was not injected into the stratosphere. The first simultaneous measurement of halogen and sulfur content of gases and particles in explosive eruption plumes is reported. The average percents of elements in particles were sulfur, 2.5 + or - 2.1; chlorine, 18 + or - 12; and fluorine, 38 + or - 29. The average molecular ratio of HCl/SO2 and HCl/HF were 0.41 + or - 0.26 and 14 + or - 12 in the Guatemalan eruption plumes.

Lazrus, A. L.↗

NASA NTRS1990

Extraterrestrial halogen and sulfur contents of the stratosphere

Interplanetary dust represents a potential source of environmentally important chemical species in the earth's atmosphere. Previous studies have used computational models of atmospheric evolution of meteor debris to conclude that the steady-state stratospheric component of extraterrestrial matter is a small fraction of the total aerosol load. Observational data suggest such calculations may underestimate stratospheric residence times and, thus, concentrations. Two computational methods were employed here to obtain reasonable limits for the stratospheric contents of halogens and sulfur from extraterrestrial sources. The lower limit was based on the total stratospheric aerosol load and the relative influxes from interplanetary dust and tropospheric sources. The upper limit was obtained using a viscous settling method. These results suggest that the steady-state extraterrestrial influxes of halogens are minor compared to tropospheric sources but the sulfur input may be comparable to the present observed stratospheric content. Temporal enhancements in the meteoroid flux, such as passage through comet debris lanes or impact by large bodies, may produce significant chemical perturbations in the atmosphere.

Sutton, S. R.↗

NASA NTRS1994

Observations of stratospheric hydrogen fluoride by halogen occultation experiment (HALOE)

The Halogen Occultation Experiment (HALOE) Hydrogen Fluoride (HF) channel on the Upper Atmospheric Research Satellite (UARS) is providing the first global measurements of stratospheric HF, the dominant flourine reservoir in the atmosphere. This paper describes the latitudinal and seasonal variations of HALOE-observed HF in terms of vertical profiles, altitude/latitude cross sections, and column abundances. The HF global distribution shows a 'tracerlike' structure and its column amount increases with latitude, in agreement with previous aircraft measurements of the HF column amount. A comparison between the HALOE HF column above 20 km and the ATMOS 1985 measurements is used to estimate the annual rate of increase of stratospheric HF. Exponential rates of 4.9-6.6%/yr and linear growth rates of 6-8.6%/yr in 1985 and 4.3-5.5%/yr in 1992-1993 are found. HALOE HF measurements during the 1993 Antarctic spring are briefly described. This species behaves like a conserved tracer and its distribution shows an area of enhanced mixing ratios correlated with the polar vortex that has a clear latitude boundary. Finally, simulated HF distributions by the National Center for Atmospheric Research (NCAR) two-dimensional model are used to compare with HALOE observations of HF. Reasonable agreements in the global structure and the absolute amount of HF are found. The differences between the model and the observed results indicate the need for improving treatment of atmospheric dynamics and fluorine-related chemical parameters in the model simulations.

Luo, M.↗

NASA NTRS1995

Aerosol effects and corrections in the Halogen Occultation Experiment

The eruptions of Mt. Pinatubo in June 1991 increased stratospheric aerosol loading by a factor of 30, affecting chemistry, radiative transfer, and remote measurements of the stratosphere. The Halogen Occultation Experiment (HALOE) instrument on board Upper Atmosphere Research Satellite (UARS) makes measurements globally for inferring profiles of NO2, H2O, O3, HF, HCl, CH4, NO, and temperature in addition to aerosol extinction at five wavelengths. Understanding and removing the aerosol extinction is essential for obtaining accurate retrievals from the radiometer channels of NO2, H2O and O3 in the lower stratosphere since these measurements are severely affected by contaminant aerosol absorption. If ignored, aerosol absorption in the radiometer measurements is interpreted as additional absorption by the target gas, resulting in anomalously large mixing ratios. To correct the radiometer measurements for aerosol effects, a retrieved aerosol extinction profile is extrapolated to the radiometer wavelengths and then included as continuum attenuation. The sensitivity of the extrapolation to size distribution and composition is small for certain wavelength combinations, reducing the correction uncertainty. The aerosol corrections extend the usable range of profiles retrieved from the radiometer channels to the tropopause with results that agree well with correlative measurements. In situations of heavy aerosol loading, errors due to aerosol in the retrieved mixing ratios are reduced to values of about 15, 25, and 60% in H2O, O3, and NO2, respectively, levels that are much less than the correction magnitude.

Hervig, Mark E.↗

NASA NTRS1988

Simulation of the transport of halogen species from the equatorial and mid-latitude stratosphere to the polar stratosphere in a two-dimensional model

The bulk of O sub 3 destruction in the Antarctic stratosphere takes place in the lower stratosphere between 15 and 25 km. Both O sub 3 and the halogen reservoir species have their origins in the higher altitude region (20 to 30 km) in the equatorial and mid-latitude stratosphere. Using the Caltech-JPL two-dimensional residual circulation model, researchers investigate the growth of stratospheric halogen due to the increase of CFCl sub 3 and CF sub 2 Cl sub 2.

Yung, Yuk L.↗

NASA NTRS1987

Infrared spectroscopic measurements of halogenated source gases in the stratosphere with the ATMOS instrument

The volume mixing ratios of the six most important halogenated source species (CH3Cl, CF2Cl2, CFCl3, CHF2Cl, CCl4, and CF4) have been retrieved over the 10- to 30-km altitude range from the analysis of 0.01/cm resolution infrared solar occultation spectra recorded near 30 deg N and 47 deg S latitudes with the ATMOS (Atmospheric Trace Molecule Spectroscopy) instrument, operating from on board Spacelab 3 (April-May 1985). The results reported here, although in satisfactory agreement with recent in situ values obtained from air sampling techniques, are limited in accuracy by the limited absorption representative of most of the species and by uncertainties in the spectroscopic parameters currently available for these gases. They demonstrate, however, the power of the IR remote sensing approach for evaluating on a global scale the total chlorine budget of the atmosphere, and they provide an independent set of simultaneous data acquired for the important source and reservoir halogenated molecular species in the upper atmosphere.

Zander, R.↗

NASA NTRS2009

Trends and Solar Cycle Effects in Temperature Versus Altitude From the Halogen Occultation Experiment for the Mesosphere and Upper Stratosphere

Fourteen-year time series of mesospheric and upper stratospheric temperatures from the Halogen Occultation Experiment (HALOE) are analyzed and reported. The data have been binned according to ten-degree wide latitude zones from 40S to 40N and at 10 altitudes from 43 to 80 km-a total of 90 separate time series. Multiple linear regression (MLR) analysis techniques have been applied to those time series. This study focuses on resolving their 11-yr solar cycle (or SC-like) responses and their linear trend terms. Findings for T(z) from HALOE are compared directly with published results from ground-based Rayleigh lidar and rocketsonde measurements. SC-like responses from HALOE compare well with those from lidar station data at low latitudes. The cooling trends from HALOE also agree reasonably well with those from the lidar data for the concurrent decade. Cooling trends of the lower mesosphere from HALOE are not as large as those from rocketsondes and from lidar station time series of the previous two decades, presumably because the changes in the upper stratospheric ozone were near zero during the HALOE time period and did not affect those trends.

Remsberg, Ellis E.↗

NASA NTRS2013

Evaluating Global Emission Inventories of Biogenic Bromocarbons

Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38 %) to 0.78 (115 %) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24 %) to 1.25 (167 %) ppt. We also use aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (Br(VSLS/y)). Our simulations show Br(VSLS/y) ranges from approximately 4.0 to 8.0 ppt depending on the inventory. We report an optimized estimate at the lower end of this range (approximately 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

bromocarbons↗

NASA NTRS1999

An Evaluation of the Quality of Halogen Occultation Experiment Ozone Profiles in the Lower Stratosphere

The archived ozone profiles from the Halogen Occultation Experiment (HALOE) have already been corrected for the effects of the spectrally varying, interfering absorption due to aerosols composed of aqueous sulfuric acid, and agreement with correlative measurements in the stratosphere is generally excellent. However, comparisons of sets of coincident HALOE and ozonesonde profiles indicate occasional large differences at the lowest levels of the stratosphere. Most of those instances occur at altitudes just below a well-defined minimum in the 5.26 microns channel aerosol extinction profile, whose wavelength dependence is not represented by a sulfuric acid aerosol model. Further, when the aerosol extinction exceeds about 10(exp 3)/ km, the aerosol correction to the ozone channel transmittances is both large and uncertain. After screening out the HALOE ozone profile segments whose corresponding aerosol/cirrus corrections are likely uncertain and after averaging lie ozonesonde profiles into 2.5 km thick layers, we find that the HALOE ozone areas, on average, to within 10% of their coincident ozonesonde measurements down to 100 hPa at tropical/subtropical latitudes and to 200 hPa at extratropical latitudes. A tightening of the coincidence criteria for the comparisons does not improve the mean differences for the sets nearly as much. Part of the variance of the paired differences was also accounted for when the ozonesonde profile values were integrated into those 2.5 km layers, prior to taking differences. This improvement is due mainly to the vertical averaging of the local, higher-resolution ozonesonde data, matching the lower resolution for HALOE ozone in the lower stratosphere. It is concluded that HALOE is providing accurate ozone profiles throughout the lower stratosphere, when its correction for interfering aerosols has been well characterized and when cirrus layers are not indicated.

Bhatt, Praful P.↗

NASA NTRS2014

Reconciliation of Halogen-Induced Ozone Loss with the Total-Column Ozone Record

The observed depletion of the ozone layer from the 1980s onwards is attributed to halogen source gases emitted by human activities. However, the precision of this attribution is complicated by year-to-year variations in meteorology, that is, dynamical variability, and by changes in tropospheric ozone concentrations. As such, key aspects of the total-column ozone record, which combines changes in both tropospheric and stratospheric ozone, remain unexplained, such as the apparent absence of a decline in total-column ozone levels before 1980, and of any long-term decline in total-column ozone levels in the tropics. Here we use a chemistry-climate model to estimate changes in halogen-induced ozone loss between 1960 and 2010; the model is constrained by observed meteorology to remove the eects of dynamical variability, and driven by emissions of tropospheric ozone precursors to separate out changes in tropospheric ozone. We show that halogen-induced ozone loss closely followed stratospheric halogen loading over the studied period. Pronounced enhancements in ozone loss were apparent in both hemispheres following the volcanic eruptions of El Chichon and, in particular, Mount Pinatubo, which significantly enhanced stratospheric aerosol loads. We further show that approximately 40% of the long-term non-volcanic ozone loss occurred before 1980, and that long-term ozone loss also occurred in the tropical stratosphere. Finally, we show that halogeninduced ozone loss has declined by over 10% since stratospheric halogen loading peaked in the late 1990s, indicating that the recovery of the ozone layer is well underway.

Shepherd, T. G.↗

NASA NTRS1983

Latitudinal distributions and temporal changes of stratospheric HCl and HF

Hydrogen chloride and hydrogen fluoride are important sinks in the stratosphere for free halogens. The major sources of chlorine and fluorine in the stratosphere are anthropogenic; therefore, a measurement of HCl and HF gives information about the magnitude of anthropogenic effects on stratospheric chemistry and may give some information about the stratospheric hydroxyl concentration as well. The total column amount of HCl and HF above 12 km has been determined by measuring infrared absorption spectra with a high-resolution Fourier transform spectrometer flown on a jet aircraft. The HCl column varies from 0.7 x 10 to the 15th molecules/ sq cm near the equator to 2.7 x 10 to the 15th molecules/sq cm at 70 N; the HF column is about a factor of 5 lower. The HCl:HF ratio is almost independent of latitude, and neither constituent shows substantial seasonal or diurnal variation. At mid-latitudes, the data from 1978 to 1982 show an annual increase of 5 percent per year for HCl and 12 percent per year for HF.

Mankin, W. G.↗

NASA NTRS2007

Estimating When the Antarctic Ozone Hole Will Recover

The Antarctic ozone hole develops each year and culminates by early spring (late September - early October). The severity of the hole has been assessed from satellites using the minimum total ozone value from the October monthly mean (depth of the hole) and by calculating the average area coverage during this September-October period. Profile information shows that ozone is completely destroyed in the 14-21 km layer by early October. Ozone is mainly destroyed by halogen (chlorine and bromine) catalytic cycles, and these losses are modulated by temperature variations. Because atmospheric halogen levels are responding to international agreements that limit or phase out production, the amount of halogens in the stratosphere should decrease over the next few decades. Using projections of halogen levels combined with age-of-air estimates, we find that the ozone hole is recovering at an extremely slow rate and that large ozone holes will regularly recur over the next 2 decades. We estimate that the ozone hole will begin to show first signs of size decrease in about 2023, and the hole will fully recover to pre-1980 levels in approximately 2070. Estimates of the ozone hole's recovery from models reveal important differences that will be discussed.

Newman, Paul A.↗

NASA NTRS2007

Estimating when the Antarctic Ozone Hole will Recover

The Antarctic ozone hole develops each year and culminates by early spring (late September - early October). The severity of the hole has been assessed from satellites using the minimum total ozone value from the October monthly mean (depth of the hole) and by calculating the average area coverage during this September-October period. Profile information shows that ozone is completely destroyed in the 14-2 1 km layer by early October. Ozone is mainly destroyed by halogen (chlorine and bromine) catalytic cycles, and these losses are modulated by temperature variations. Because atmospheric halogen levels are responding to international a'greements that limit or phase out production, the amount of halogens in the stratosphere should decrease over the next few decades. Using projections of halogen levels combined with age-of-air estimates, we find that the ozone hole is recovering at an extremely slow rate and that large ozone holes will regularly recur over the next 2 decades. We estimate that the ozone hole will begin to show first signs of size decrease in about 2023, and the hole will fully recover to pre-1980 levels in approximately 2070. Estimates of the ozone hole's recovery from models reveal important differences that will be discussed.

Newman, Paul A.↗

NASA NTRS2000

A Simulation of Bromoform's Contribution to Stratospheric Bromine

Many chlorinated and brominated compounds that are inert in the troposphere are destroyed in the stratosphere and act as an in-situ source of stratospheric reactive chlorine and bromine. Other halogenated compounds that are reactive in the troposphere might contribute to the stratosphere's halogen budget in two ways. First, like their unreactive companions, rapid convective transport might carry them to the upper troposphere and make them available for subsequent advection by the mean circulation into the stratosphere before they are oxidized or photolyzed. Second, it is more likely that they are destroyed in the troposphere, and the chlorine and bromine that is released might then be transported to the stratosphere. We evaluate the relative influence of these processes on stratospheric bromine in a three-dimensional chemistry and transport model which simulates the distribution of bromoform (CHBr3). CHBr3 is parameterized as a short-lived, ocean-surface source gas whose destruction by photolysis and reaction with hydroxyl (OH) in the troposphere and stratosphere yields inorganic bromine (Br(sub y)). Many of the observed features of CHBr3 are simulated well, and comparisons with observations are used to show that the model represents aspects of transport in the upper troposphere and lower stratosphere that are critical to the evaluation. In particular, the model maintains the observed troposphere-stratosphere distinctness in transport pathways and reproduces the observed seasonal dependence of the mixture of air in the middle- and high-latitude lowermost stratosphere. We estimate that adding CHBr3 to models which already include the long-lived organic brominated compounds (halons and methyl bromide) will increase the simulated stratospheric mass of Br(sub y) by about 15 percent. In-situ stratospheric destruction of CHBr3 produces Br(sub y) in amounts which are comparable to that transported into the stratosphere after photolysis and oxidation of CHBr3 in the troposphere. In our simulations the mass of Br(sub y) produced from the destruction of CHBr3 does not exceed the mass of Br(sub y) produced from the destruction of the long-lived compounds at any level in the stratosphere. However, Br(sub y) from the loss of CHBr3 accounts for approximately one-third of the total Br(sub y) in the lowest kilometer of the stratosphere.

Nielsen, J. Eric↗

NASA NTRS1989

Airborne measurements of stratospheric constituents over Antarctica in the austral spring, 1987. II - Halogen and nitrogen trace gases

The IR absorption spectra of the polar stratosphere, recorded by a Fourier transform spectrometer aboard the NASA DC-8 aircraft during the Airborne Antarctic Ozone Experiment, were used to derive vertical column amounts above flight altitude of HCl, HF, NO, NO2, ClONO2, and HNO3 in the region of disturbed ozone chemistry during September 1987. Significant reductions in the amounts of HCl, NO, NO2, and HNO3 were observed within the confines of the polar vortex, compared with amounts outside the vortex. When compared with the springtime observations by the same instrument in the Northern Hemisphere, the HCl and NO2 species displayed the most dramatic depletions. The results obtained are generally in agreement with the earlier ground measurements conducted at the McMurdo Station.

Coffey, M. T.↗

NASA NTRS1987

Infrared spectroscopic measurements of halogenated sink and reservoir gases in the stratosphere with the ATMOS instrument

The Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument recorded 19 sets of interferograms during solar occultations in both the Northern and Southern Hemispheres over the course of the Spacelab 3 mission. The resulting IR spectra furnish concentration profiles for over 25 atmospheric species. Attention is presently given to the volume mixing ratio profiles for HCl and HF in the 15-60-km altitude region, retrieved from northern sunsets and southern sunrises. The HF/HCl ratios deduced are in good agreement with model predictions. The total atmospheric chlorine at 50 km is nearly all in the form of HCl.

Raper, O. F.↗

NASA NTRSDate not supplied

The Impact of Atmospheric Dynamics and Anthropogenic Very Short-Lived Chlorine Species on the Recovery of Extra-Polar Ozone

The successful implementation of the Montreal Protocol has led to a decrease in the atmospheric abundance of ozone-depleting substances and a slowing in the destruction of the ozone layer. Previous studies have suggested that atmospheric dynamics, or a rise in compounds not regulated by the Montreal Protocol, such as very short-lived chlorine species (VSL Cl), may lead to a slower than expected recovery of the ozone layer. In this presentation, we examine the expected recovery of total column ozone (TCO) and stratospheric column ozone (SCO) to values observed in 1980 using a novel multiple linear regression (MLR) model that involves a month-by-month regression. The MLR model is trained to TCO anomalies from six data records (SBUV v8.7 MOD, SBUV v8.6 COH, WOUDC, GSG, GTO-ECV, MSR-2) over 1979 to 2021 for the Northern Hemisphere (35N – 60N), the Southern Hemisphere (60S – 35S) and the Tropics (20S – 20N), and SCO anomalies from ML-TOMCAT for these same zonal bands. The MLR includes the effect of halogens (equivalent effective stratospheric chlorine (EESC)), total solar irradiance, stratospheric aerosol optical depth, quasi-biennial oscillation, and the El Niño Southern Oscillation as regressors. We also include the effect of atmospheric dynamics such as the Brewer-Dobson Circulation, Arctic Oscillation, and the Antarctic Oscillation, and VSL Cl species in the formulation of EESC. We use a novel approach to the MLR framework, by separating the observed and regressor time series into the respective months (separating all of the Januarys, Februarys, etc.). Then we conduct a regression for each month from 1979 to 2021 for the three zonal bands denoted above. The model results for each month are combined together to achieve a full monthly time series from 1979 to 2021. We use this novel approach to ascertain the effect of atmospheric dynamics on TCO and SCO, since the dynamical proxies affect ozone in a distinctly different manner for various months. In this presentation, we will quantify the role of both the inclusion of VSL Cl species in the formulation of EESC as well as atmospheric dynamics in explaining the slower than expected recovery of extra-polar TCO and SCO over the past decade.

Laura A. McBride↗