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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
NASA NTRS1989

In situ observations of BrO over Antarctica - ER-2 aircraft results from 54 deg S to 72 deg S latitude

Bromine monoxide was observed in situ during nine flights of the NASA ER-2 aircraft from Punta Arenas, Chile (54 deg S latitude), to 72 deg S latitude over the Palmer Peninsula, Antarctica. The first flight for the BrO detection system was on August 28. The distribution of BrO inside the chemically perturbed region defined by greatly elevated ClO abundances was different from that found just outside. Inside, the BrO mixing ratio was 6.1 + or - 1.1 pptv above the 440 K potential temperature surface, 4.7 + or - 2.0 pptv between the 400 and 440 K surfaces, and less than 4 pptv below the 400 K surface. At high latitudes outside the chemically perturbed region, the BrO mixing ratio was 5.4 + or - 1.4 pptv near the 450 K surface, but decreased to 2.9 + or - 1.2 pptv at the 420 K surface. The abundance of BrO showed no discernible temporal trend during the course of the nine flights. Away from the south polar region, at latitudes between 47 deg S and 37 deg N and potential temperatures between 435 and 500 K (18.5- to 20.7-km altitude), the BrO mixing ratio was 0.5-3.0 pptv.

Brune, W. H.↗
NASA NTRS1989

Nitrogen and chlorine species in the spring Antarctic stratosphere - Comparison of models with Airborne Antarctic Ozone Experiment observations

The concentrations and the time development of chlorine and nitrogen trace gases in the Antarctic stratosphere before, during, and after the Airborne Antractic Ozone Experiment (AAOE) were simulated using photochemical models of the Antractic stratosphere during winter/spring. The initial conditions in the calculations were constrained using observations by the AAOE instrument. The comparison of calculated results with the AAOE measurements of HCl and ClO suggest that heterogeneous chemistry was maintained throughout the month of September 1987.

Rodriguez, J. M.↗
NASA NTRS1989

Lagrangian photochemical modeling studies of the 1987 Antarctic spring vortex. II - Seasonal trends in ozone

A photochemical model consisting of 40 species and 107 reactions is integrated along 80-day air parcel trajectories calculated in the lower stratosphere for the springtime Antarctic. For the trajectory starting at 58 deg S, which may be regarded as outside the circumpolar vortex, only a small change in O3 occurs in the model. In contrast, for the air parcel starting in the vortex at 74 deg S, the O3 concentration is reduced by 93 percent during the 80 days from the beginning of August to late October. The model results for several species are compared with measurements from the Airborne Antarctic Ozone Experiment and, in general, good agreement is obtained. In the model, the dentrification of the air parcels in polar stratospheric clouds increases the amount of chlorine present in active form. Heterogeneous reactions maintain high active chlorine which destroys O3 via the formation of the ClO dimer. Results of calculations with reduced concentrations of inorganic chlorine show considerably reduced O3 destruction rates and compare favorably with the behavior of total O3 since the late 1970s. The remaining major uncertainties in the photochemical aspects of the Antarctic ozone hole are highlighted.

Austin, J.↗
NASA NTRS1990

Stratospheric constituent trends from ER-2 profile data

Trend analysis of the Airborne Arctic Stratospheric Expedition's ER-2 profile data reveals an average decrease in N2O on potential temperature isentropes which can be attributed to diabatic cooling of inner vortex air. This conclusion is independently supported by radiative transfer computations. Trends in ozone and water vapor over the same period are not consistent with the magnitude of the diabatic descent. After accounting for the diabatic motion (estimated from N2O), an additional 0.44 + or - 0.3 percent/day average anomalous O3 decrease above 440 K (about 20 km) is needed to balance the continuity equation. This ozone decrease suggests additional photochemical destruction of ozone in the presence of the high amounts of ClO observed during the mission. A 0.4 + or - 0.3 percent/day average anomalous increase in H2O is also observed near 420 K (about 18 km) which may be due to the evaporation of ice crystals falling from higher, colder stratospheric layers.

Schoeberl, Mark R.↗
NASA NTRS1990

Nitric oxide measurements in the Arctic winter stratosphere

Measurements of NO from five flights of the NASA ER-2 aircraft during the Airborne Arctic Stratospheric Expedition are presented. The NO values and vertical gradient near 60 deg N latitude are similar to previous measurements near 50 deg N in winter (Ridley et al., 1984, 1987). The NO latitudinal gradient is distinctly negative outside of the polar vortex, approaching zero at the boundary of the vortex, and remaining below the 20 pptv detection limit inside the vortex. Steady state NO2 and NO(x) (NO + NO2) are calculated from measured NO, O3, and ClO, and modeled photodissociation rates. NO(x) outside the vortex shows a negative dependence on latitude and solar zenith angle. Low NO(x) and NO(x)/NO(y), inside and near the vortex boundary may be indications of heterogeneous removal of ClONO2 and N2O5.

Fahey, D. W.↗
NASA NTRS1990

In situ measurements of BrO in the Arctic stratosphere

Mixing ratios of BrO have been measured in the Arctic lower statosphere with an instrument mounted on the NASA ER-2 aircraft. Observations from fourteen flights above the Arctic Circle in January and February of 1989 defined mixing ratios within the vortex of 4 + or - 2 parts per trillion by volume (pptv) at a potential temperature of 400 K, rising to 8 + or - 2 pptv at 470 K. These values are twice as large as values found at equivalent potential temperatures at lower latitudes, and are comparable to the mixing ratios found inside the antarctic polar vortex. Within the statistical uncertainty of the measurements, no BrO was observed in darkness at any time either inside or outside of the vortex, indicating that active bromine was sequestered in long-lived reservoirs, probably BrONO2 and BrCl. These measurements, in conjuction with measurements of ClO, demonstrate that the interaction of bromine and chlorine could represent a major sink for ozone in the presence of sunlight.

Toohey, D. W.↗
NASA NTRS1990

Photodissociation of Cl2O2 in the spring Antarctic lower stratosphere

The likely photodissociation pathways of chlorine peroxide are examined. Reasoning by analogy between hydrogen peroxide and chlorine peroxide, it is shown that photodissociation of chlorine peroxide at wavelengths longer than 250 nm is not likely to give chlorine atoms as a primary product. Reasoning by analogy with molecules whose visible spectra are known, it is concluded that chlorine peroxide is also likely to photodissociate in the visible to give ClO radicals as primary products.

Eberstein, Igor J.↗
NASA NTRS1990

Spatial variation of ozone depletion rates in the springtime Antarctic polar vortex

An area-mapping technique, designed to filter out synoptic perturbations of the Antarctic polar vortex such as distortion or displacement away from the pole, was applied to the Nimbus-7 TOMS (Total Ozone Mapping Spectrometer) data. This procedure reveals the detailed morphology of the temporal evolution of column O3. The results for the austral spring of 1987 suggest the existence of a relatively stable collar region enclosing an interior that is undergoing large variations. A simplified photochemical model of O3 loss and the temporal evolution of the area-mapped polar O3 are used to constrain the chlorine monoxide (ClO) concentrations in the springtime Antarctic vortex. The O3 loss rates could be larger than deduced here because of underestimates of total O3 by TOMS near the terminator.

Yung, Yuk L.↗
NASA NTRS1991

The influence of polar heterogeneous processes on reactive chlorine at middle latitudes - Three dimensional model implications

Three-dimensional model calculations with the NASA/GSFC chemistry and transport model have been designed to consider the impact of heterogeneous processes occurring on polar stratospheric clouds (PSCs) in the Arctic vortex on the HCl distribution. By examining the HCl concentration for a calculation with PSCs relative to a calculation with gas phase chemistry only, the impact of polar processing on reactive chlorine species at middle latitudes is inferred. Results from the chemistry and transport model reproduce basic features of the ClO measurements (Toohey et al., 1991), which were made on the ferry flights of the ER-2 from Stavanger, Norway to Moffett Field, California via Wallops Island, Virginia on February 20 and 21, 1989. The model indicates that perturbed air which is contained within the polar vortex during winter is not homogeneously mixed, and that the ferry flights were made through air with the largest conversion of HCl to reactive chlorine that is seen at middle latitudes.

Douglass, Anne R.↗
NASA NTRS1991

Tests of stratospheric models - The reactions of atomic chlorine with O3 and CH4 at low temperature

The rate-constant ratio of the photochemical reactions of atomic chlorine with O3 and CH4 was determined using data from laboratory experiments on competitive chlorination of O3/CH4 mixtures at stratospheric temperatures (197-217 K). Two experimental approaches were used: (1) measuring the k1/k2 ratio for the reactions of atomic chlorine with ozone and methane and (2) testing for some of the ClO/CH3O2 chemistry. The chlorine and ozone concentrations were monitored by UV-Vis spectroscopy, and the CH3Cl concentration was measured by FTIR. The results on the k1/k2 ratio are in excellent agreement with the current NASA recommendation (DeMore et al., 1990), being only 12 percent higher. On the other hand, results on the ClO + CH3O2 reaction do not support the rate constant suggested by Simon et al. (1989).

Demore, W. B.↗
NASA NTRS1991

The potential for ozone depletion in the Arctic polar stratosphere

The nature of the Arctic polar stratosphere is observed to be similar in many respects to that of the Antarctic polar stratosphere, where an ozone hole has been identified. Most of the available chlorine (CHl and ClONO2) was converted by reactions on polar stratospheric clouds to reactive ClO and Cl2O2 thoroughout the Arctic polar vortex before midwinter. Reactive nitrogen was converted to HNO3, and some, with spatial inhomogeneity, fell out of the stratosphere. These chemical changes ensured characteristic ozone losses of 10 to 15 percent at altitudes inside the polar vortex where polar stratospheric clouds had occurred. These local losses can translate into 5 to 8 percent losses in the vertical column abundance of ozone. As the amount of stratospheric chlorine inevitably increases by 50 percent over the next two decades, ozone losses recognizable as an ozone hole may well appear.

Brune, W. H.↗
NASA NTRS1991

Role of heterogeneous conversion of N2O5 on sulphate aerosols in global ozone losses

The reaction rate of N2O5 on sulphate aerosols is included in a model to predict global ozone loss and the column abundances of atmospheric gases. Because the reaction of N2O5 and the aerosols can take place in the stratospheric sulphate aerosol layer, it is included in the 2D model so that the results can be compared to abundances derived from satellite data and ground-based measurements. The N2O5/sulphate reaction is the only heterogeneous reaction in the model, in which aerosol loading is assumed to be constant and only diurnal values are examined. The decadal ozone trends resulting from calculations based on the model are found to be closer to the observed values. An important conclusion is that measurements of OH, ClO, HNO3, NO, and NO2 in the region of about 14-25 km are needed to examine significant changes in their abundances resulting from the inclusion of the N2O5/sulphate aerosol reaction.

Rodriguez, Jose M.↗
NASA NTRS1990

Retrieval methods for ground-based millimeter-wave measurements for the network for the detection of stratospheric change

The fundamental objective is to determine the information available in ground-based millimeter-wave measurements of stratospheric constituent profiles, to identify the optimum method of retrieving this profile information, and to characterize the errors in the final result. A secondary objective is to produce retrieval software for operational use with Network for the Detection of Stratospheric Change (NDSC) measurements of O3, H2O, ClO, and perhaps N2O. Tests were performed on existing ozone retrieval programs in support of ongoing NDSC field measurements. The results show that if random spectral errors and retrieval bias errors are considered, accuracy of the retrieved profile is about 5 percent from 20-50 km, and about 10 percent from 50-60 km.

Connor, Brian J.↗
NASA NTRS1990

ATLAS: Airborne Tunable Laser Absorption Spectrometer for stratospheric trace gas measurements

The ATLAS instrument is an advanced technology diode laser based absorption spectrometer designed specifically for stratospheric tracer studies. This technique was used in the acquisition of N2O tracer data sets on the Airborne Antarctic Ozone Experiment and the Airborne Arctic Stratospheric Expedition. These data sets have proved valuable for comparison with atmospheric models, as well as in assisting in the interpretation of the entire ensemble of chemical and meteorological data acquired on these two field studies. The N2O dynamical tracer data set analysis revealed several ramifications concerning the polar atmosphere: the N2O/NO(y) correlation, which is used as a tool to study denitrification in the polar vertex; the N2O Southern Hemisphere morphology, showing subsidence in the winter polar vortex; and the value of the N2O measurements in the interpretation of ClO, O3, and NO(y) measurements and of the derived dynamical tracer, potential vorticity. Field studies also led to improved characterization of the instrument and to improved accuracy.

Loewenstein, Max↗
NASA NTRS1989

Trends in stratospheric minor constituents

Photochemical models predict that increasing source gas concentrations are also expected to lead to changes in the concentrations of both catalytically active radical species (such as NO2, ClO, and OH) and inactive reservoir species (such as HNO3, HCl, and H2O). For simplicity, we will refer to all these as trace species. Those species that are expected to have increasing concentration levels are investigated. Additionally, the trace species concentration levels are monitored for unexpected changes on the basis of the measure increase in source gases. Carrying out these investigations is difficult due to the limited data base of measurements of stratospheric trace species. In situ measurements are made only infrequently, and there are few satelliteborne measurements, most over a time space insufficient for trend determination. Instead, ground-based measurements of column content must be used for many species, and interpretation is complicated by contributions from the troposphere or mesosphere or both. In this chapter, we examine existing measurements as published or tabulated.

Stolarski, R. S.↗
NASA NTRS1992

Heterogeneous conversion of N2O5 to HNO3 on background stratospheric aerosols - Comparisons of model results with data

The effects of heterogeneous processing by a parameterized lower stratospheric sulfate aerosol layer on model calculations were examined using a 2D photochemical model. Model results were compared with zonally averaged LIMS data on HNO3 and NO2 and in situ measurements of NO, NO(y), and ClO, taken by the ER-2 aircraft. The results obtained are contradictory: some comparisons favor heterogeneous chemistry, and some do not. It is suggested that the assumptions made to parameterize the sulfate aerosol chemistry result in a rate of heterogeneous processing that is too vigorous.

Considine, David B.↗
NASA NTRS1992

Polar stratospheric cloud processed air and potential vorticity in the Northern Hemisphere lower stratosphere at mid-latitudes during winter

The present study compares small-scale (less than 100 km) features in ER-2 measurements of ClO, O3, H2O, N2O, and NO(y) outside the lower stratospheric Arctic vortex of 1988-1989 with features on potential vorticity maps from ECMWF. The potential vorticity maps are obtained from T106 analyses and forecasts. Some of the plots were truncated to lower resolution (T63 or T42) which smooths out the finer-scale structure. Comparison of these lower resolution plots shows how much detail is lost by excessive smoothing. It is also evident that the forecast plots lose fine-scale structure due to dissipation in the model resulting mainly from horizontal diffusion. It is concluded that blobs of air on the maps at latitudes between the vortex edge and 25 deg N having potential vorticities characteristic of the vortex did indeed originate from the vortex, but that the real atmosphere is more sharply differentiated than the meteorological analyses, implying that the potential vorticity maps underestimate the amount of peeled-off material.

Tuck, A. F.↗