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Webster, C. R.

Publications and source records attributed to Webster, C. R..

At least 55 records · Page 3
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NASA NTRS1998

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3 in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO(sub x) required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of O3 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day. This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more O3 than expected.

Wennberg, P. O.↗
NASA NTRS1998

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

The concentrations of the hydrogen radicals OH and HO2 in the middle and upper troposphere were measured simultaneously with those of NO, O3, CO, H2O, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field. The data allow a direct examination of the processes that produce O3, in this region of the atmosphere. Comparison of the measured concentrations of OH and HO2 with calculations based on their production from water vapor, ozone, and methane demonstrate that these sources are insufficient to explain the observed radical concentrations in the upper troposphere. The photolysis of carbonyl and peroxide compounds transported to this region from the lower troposphere may provide the source of HO(x) required to sustain the measured abundances of these radical species. The mechanism by which NO affects the production of 03 is also illustrated by the measurements. In the upper tropospheric air masses sampled, the production rate for ozone (determined from the measured concentrations of HO2 and NO) is calculated to be about 1 part per billion by volume each day.This production rate is faster than previously thought and implies that anthropogenic activities that add NO to the upper troposphere, such as biomass burning and aviation, will lead to production of more 03 than expected.

Wennberg, P. O.↗
NASA NTRS1996

A Comparison of Measurements from ATMOS and Instruments Aboard the ER-2 Aircraft: Tracers of Atmospheric Transport and Halogenated Gases

We compare volume mixing ratio profiles of N2O, O3, NO(y), H2O, CH4, and CO in the mid-latitude lower stratosphere measured by the ATMOS Fourier transform spectrometer on the ATLAS-3 Space Shuttle Mission with in situ measurements acquired from the NASA ER-2 aircraft during Nov 1994. ATMOS and ER-2 observations of (N2O) show good agreement, as do measured correlations of (O3), (NO(y)), (H2O), and (CH4) with (N2O). Thus a consistent measure of the hydrogen (H2O, CH4) content of the lower stratosphere is provided by the two platforms. The similarity of (NO(y)) determined by detection of individual species by ATMOS and the total (NOy) measurement on the ER-2 provides strong corroboration for the accuracy of both techniques. A 25% discrepancy in lower stratospheric (CO) observed by ATMOS and the ER-2 remains unexplained. Otherwise, the agreement for measurements of long-lived tracers demonstrates the ability to combine ATMOS data with in situ observations for quantifying atmospheric transport.

Chang, A. Y.↗
NASA NTRS1996

A Comparison of Measurements from ATMOS and Instruments Aboard the ER-2 Aircraft: Halogenated Gases

We compare volume mixing ratio profiles of N2O, CFC-11, CFC-12, CCl4, SF6, and HCl in the mid-latitude lower stratosphere measured by the ATMOS Fourier transform spectrometer on the ATLAS-3 Space Shuttle Mission with in situ measurements acquired from the NASA ER-2 aircraft during Nov. 1994. Good agreement is found between ATMOS and in situ correlations of [CFC-11], [CFC-12], and [SF6] with [N2O]. ATMOS measurements of [CCl4] are 15% high compared to ER-2 data, but agree within the systematic uncertainties. ATMOS observations of [HCl] vs [N2O] are within approximately 10% of ER-2 data for [HCl] > 1 ppbv, but exceed in situ measurements by larger fractional amounts for smaller [HCl]. ATMOS measurements of [ClONO2] agree well with values inferred from in situ observations of [ClO], [NO], and [O3]. The sum of [HCl] and [ClONO2] observed by ATMOS, supplemented by a minor contribution from [ClO] estimated with a photochemical model, is consistent with the levels of inorganic chlorine inferred from in situ measurements of chlorine source gases.

Chang, A. Y.↗
NASA NTRS1996

A Comparison of Measurements from ATMOS and Instruments Aboard the ER-2 Aircraft: Tracers of Atmospheric Transport

We compare volume mixing ratio profiles of N2O, O3, NO(y) H2O, CH4, and CO in the mid-latitude lower stratosphere measured by the ATMOS Fourier transform spectrometer on the ATLAS-3 Space Shuttle Mission with in situ measurements acquired from the NASA ER-2 aircraft during Nov 1994. ATMOS and ER-2 observations of [N2O] show good agreement, as do measured correlations of [O3], [NO(y)], [H2O], and [CH4] with [N2O]. Thus a consistent measure of the hydrogen (H2O, CH4) content of the lower stratosphere is provided by the two platforms. The similarity of [NO(y)] determined by detection of individual species by ATMOS and the total [NO(y)] measurement on the ER-2 provides strong corroboration for the accuracy of both techniques. A 25% discrepancy in lower stratospheric [CO] observed by ATMOS and the ER-2 remains unexplained. Otherwise, the agreement for measurements of long-lived tracers demonstrates the ability to combine ATMOS data with in situ observations for quantifying atmospheric transport.

Chang, A. Y.↗
NASA NTRS1996

A Comparison of Measurements from ATMOS and Instruments Aboard the ER-2 Aircraft: Halogenated Gases

We compare the mixing rations of N 2 O, CFC-11, CFC-12, CCI 4 , SF 6 , and HCI in the mid-latitude stratosphere measured by the ATMOS Fourier transform spectrometer with in situ measurements acquired aboard the NASA ER-2 aircraft during November 1994. Good agreement is found between ATMOS and in situ correlations of CFC-11, CFC-12, and SF 6 with N 2 O. ATMOS observations of CCI 4 are approx. 15 percent higher than the ER-2 data, but within the systematic uncertainties.

N2O↗
NASA NTRS1994

In situ measurements of the NO2/NO ratio for testing atmospheric photochemical models

Simultaneous in situ measurements of NO2, NO, O3, ClO, pressure and temperature have been made for the first time, presenting a unique opportunity to test our current understanding of the photochemistry of the lower stratospere. Data were collected from several flights of the ER-2 aircraft at mid-latitudes in May 1993 during NASA's Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE). The daytime ratio of NO2/NO remains fairly constant at 19 km with a typical value of 0.68 and standard deviation of +/- 17. The ratio observations are compared with simple steady-state calculations based on laboratory-measured reaction rates and modeled NO2 photolysis rates. At each measurement point the daytime NO2/NO with its measurements uncertainty overlap the results of steady-state caculations and associated uncertainty. Possible sources of error are examined in both model and measurements. It is shown that more accurate laboratory determinations of the NO + 03 reaction rate and of the NO2 cross-sections in the 200-220 K temperature range characteristic of the lower stratosphere would allow for a more robust test of our knowledge of NO(X) phtochemistry by reducing significant sources if uncertainties in the interpretation of statospheric measurements.

Jaegle, L.↗
NASA NTRS1994

An examination of the total hydrogen budget of the lower stratosphere

We analyze the hydrogen budget of the lower stratosphere using simultaneous in situ measurements of northern hemispheric water vapor (H2O) and methane (CH4) obtained during the spring Stratospheric Photochemistry, Aerosols, and Dynamics Expedition (SPADE), as well as previously published in situ H2 data. Based on this data, we conclude that approximately two H2O molecules are produced for each CH4 molecule destroyed. This implies that H2 production from CH4 oxidation is balanced by H2 oxidation. The uncertainty in this analysis is greatly reduced by the use of multiple data sets. Additionally, we infer that, on an annual and global average, H2O enters the stratosphere with a mixing ratio of 4.2 +/- 0.5 ppmv, and that the quasi-conserved quantity 2 x CH4 + H2O has a value of 7.6 +/- 0.6 ppmv in these northern hemishere air parcels (where xi denotes the mixing ratio of the constituent xi).

Dessler, A. E.↗
NASA NTRS1994

Hydrochloric acid and the chlorine budget of the lower statosphere

Concentrations of HCl measurements in the lower stratosphere in 1993 by the ALIAS instrument on the ER-2 aircraft reveal that only 40% of inorganic chlorine (Cl(y), inferred from in situ measurements of organic chlorinated sources gases) is present as HCl, significantly lower than model predictions. Although the sum of measured HCl, ClO and ClONO2, the latter inferred from measurements of ClO and NO2 equals Cl(y) to within the incertainty of measurement, it is systematically less than Cl(y) by 30-50%. This discrepancy suggests that concentrations of ClONO2 may exceed those of HC; near 20 km altitude, consistent with a slower photolysis rate for ClONO2 than calculated using recommended cross sections. Comparison of profiles of HCl measured during 1992 and 1193 at mid-latitudes by balloon (BLISS and MARKIV), space shuttle (ATMOS), and satellite (HALOE) instruments with the aircraft data reveal an apparent pressure dependence to the HCl to Cl(y) ratio, consistent with a factor of 3-10 reduction in the photolysis rate for ClONO2 at ER-2 altitudes. However, the diurnal variation of ClO is well-simulated by models using the recommended photolysis rate, and simulations measurements of ClONO2 and HCl at mid-latitudes by ATMOS and MARKIV report HCl (HCL+ ClONO2) ratios greater than or equal to 50%. Premliminary measurements by ALIAS in the southern hemisphere report HCl/Cl(y) values of about 75%.

Webster, C. R.↗
NASA NTRS1994

The Diurnal Variation of Hydrogen, Nitrogen, and Chlorine Radicals: Implications for the Heterogeneous Production of HNO2

In situ measurements of hydrogen, nitrogen, and chlorine radicals obtained through sunrise and sunset in the lower stratosphere during SPADE are compared to results from a photochemical model constrained by observed concentrations of radical precursors and environmental conditions. Models allowing for heterogeneous hydrolysis of N205 on sulfate aerosols agree with measured concentrations of NO, NO2, and ClO throughout the day, but fail to account for high concentrations of OH and H02 observed near sunrise and sunset. The morning burst of [OH] and [HO2] coincides with the rise of [NO] from photolysis of N02, suggesting a new source of HO, that photolyzes in the near UV (350 to 400 nm) spectral region. A model that allows for the heterogeneous production of HN02 results in an excellent simulation of the diurnal variations of [OH] and [HO2].

Salawitch, R. J.↗
NASA NTRS1994

The Distribution of Hydrogen, Nitrogen, and Chlorine Radicals in the Lower Stratosphere: Implications for Changes in O3 due to Emission of NO(y) from Supersonic Aircraft

In situ measurements of hydrogen, nitrogen, and chlorine radicals obtained in the lower stratosphere during the Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE) are compared to results from a photochemical model that assimilates measurements of radical precursors and environmental conditions. Models allowing for heterogeneous hydrolysis of N2O5 agree well with measured concentrations of NO and ClO, but concentrations of HO2 and OH are underestimated by 10 to 25%, concentrations of NO2 are overestimated by 10 to 30%, and concentrations of HCl are overestimated by a factor of 2. Discrepancies for [OH] and [HO2] are reduced if we allow for higher yields of O(sup 1)D) from 03 photolysis and for heterogeneous production of HNO2. The data suggest more efficient catalytic removal of O3 by hydrogen and halogen radicals relative to nitrogen oxide radicals than predicted by models using recommended rates and cross sections. Increases in [O3] in the lower stratosphere may be larger in response to inputs of NO(sub y) from supersonic aircraft than estimated by current assessment models.

Salawitch, R. J.↗
NASA NTRS1994

In Situ Measurements of the NO2/NO Ratio for Testing Atmospheric Photochemical Models

Simultaneous in situ measurements of NO2, NO, O3, ClO, pressure and temperature have been made for the first time, presenting a unique opportunity to test our current understanding of the photochemistry of the lower stratosphere. Data were collected from several flights of the ER-2 aircraft at mid-latitudes in May 1993 during NASA's Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE). The daytime ratio of NO2/NO remains fairly constant at 19 km with a typical value of 0.68 and standard deviation of +/- 0.17. The ratio observations are compared with simple steady-state calculations based on laboratory-measured reaction rates and modeled NO2 photolysis rates. At each measurement point the daytime NO2/NO with its measurement uncertainty overlap the results of steady-state calculations and associated uncertainty. However, over all the ER-2 flights examined, the model systematically overestimates the ratio by 40% on average. Possible sources of error are examined in both model and measurements. It is shown that more accurate laboratory determinations of the NO + O3 reaction rate and of the NO2 cross-sections in the 200-220 K temperature range characteristic of the lower stratosphere would allow for a more robust test of our knowledge of NO(x) photochemistry by reducing significant sources of uncertainties in the interpretation of stratospheric measurements. The present measurements are compared with earlier observations of the ratio at higher altitudes.

Jaegle, L.↗
NASA NTRS1994

Transport out of the lower stratospheric Arctic vortex by Rossby wave breaking

The fine-scale structure in lower stratospheric tracer transport during the period of the two Arctic Airborne Stratospheric Expeditions (January and February 1989; December 1991 to March 1992) is investigated using contour advection with surgery calculations. These calculations show that Rossby wave breaking is an ongoing occurrence during these periods and that air is ejected from the polar vortex in the form of long filamentary structures. There is good qualitative agreement between these filaments and measurements of chemical tracers taken aboard the NASA ER-2 aircraft. The ejected air generally remains filamentary and is stretched and mixed with midlatitude air as it is wrapped around the vortex. This process transfers vortex air into midlatitudes and also produces a narrow region of fine-scale filaments surrounding the polar vortex. Among other things, this makes it difficult to define a vortex edge. The calculations also show that strong stirring can occur inside as well as outside the vortex.

Waugh, D. W.↗
NASA NTRS1994

Balloon profiles of stratospheric NO2 and HNO3 for testing the heterogeneous hydrolysis of N2O5 on sulfate aerosols

Simultaneous in situ measurements of stratospheric NO2, HNO3, HCl, and CH4 from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO2, HNO3, and NO2/HNO3 agree well with gas-phase model calculations near 34 km where Stratospheric Aerosol and Gas Experiment (SAGE) 2 data show little sulfate aerosol, this is not true at the lower altitudes where SAGE 2 shows high aerosol loadings. At 24 km the BLISS NO2 and HNO3 measurements are 70% lower and 50% higher, respectively, than the gas phase model predictions, with a measured NO2/HNO3 ratio 5 times smaller. When the heterogeneous hydrolysis of N2O5 and ClONO2 on sulfate aerosol of surface area densities matching the SAGE 2 measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range.

Webster, C. R.↗
NASA NTRS1993

In situ measurements of the ClO/HCl ratio: Heterogeneous processing on sulfate aerosols and polar stratospheric clouds

Simultaneous in situ measurements of stratospheric ClO and HCl have been made for the first time, during numerous flights of the ER-2 aircraft covering latitudes 24-90 deg N from October 1991 through March 1992. The ClO/HCl ratio is identified as a key indicator of heterogeneous processing both outside and within the Arctic polar vortex. For ClO mixing ratios below about 120 pptv, remarkably constant ClO/HCl values of about 15% characterize the lower stratosphere. The observed values are significantly higher than those derived from a 2-D model using either gas phase photochemistry alone (2%), or including heterogeneous sulfate chemistry (5-10%). During the Arctic early spring, after conversion of HCl into reactive chlorine has taken place, the vortex edge is poorly defined by ClO levels. Loss of HCl and its slow recovery following low-temperature polar heterogeneous chemistry distinguishes HCl as a new and unique dynamical tracer of polar stratospheric clouds (PSC)-processed air.

Webster, C. R.↗
NASA NTRS1993

A case study of the mountain lee wave event of January 6, 1992

A mountain wave event, observed at the southern tip of Greenland on January 6, 1992, was corroborated by three experiments: the Meteorological Measurement System (MMS), the Microwave Temperature Profiler (MTP), and the Reactive Nitrogen Instrument (NO/NO(y)). Gravity wave signatures with classical phase relationship between wind and temperature were observed on both the outbound and inbound legs at different altitudes. The waves showed both vertically propagating and evanescent properties. Characteristics of the dominant wave mode are: wavelength about = 35 km; vertical displacement about = 0.8 km, and peak-to-peak vertical wind about = 6/ms. With the prevailing wind at about = 37/ms, the stratospheric temperature was reduced by 6K to 195.5 K within 8 minutes. The implication and potential impact of mountain lee waves on the formation of polar stratospheric clouds (PSC's) are discussed.

Chan, K. R.↗