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At least 127 records · Page 7

Establishing the Dependence of [HO2]/[OH] on Temperature, Halogen Loading, O3, and NO(x) Based on in Situ Measurements from the NASA ER-2

In situ observations of OH and HO2 from the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft (ASHOE/MAESA), Stratospheric TRacers of Atmospheric Transport (STRAT), and Polar Ozone Loss in the Arctic Region in Summer (POLARIS) NASA ER-2 field campaigns are used to examine the partitioning of HO(x) in the lower stratosphere (tropopause to approx.21 km) and upper troposphere (approx.10 km to tropopause). These measurements span a latitude range from 70degS to 90degN and a variety of atmospheric conditions as a result of seasonal changes and altitude. The response of the observed [HO2]/[OH] to changes in temperature, [03], [CO], [NO], [CIO], and [BrO] is investigated. The measured ratio is accurately described (approx.+/-10%) by a steady-state model constrained by the measured mixing ratios of O3, CO, NO, CIO, and BrO, where the model is valid for conditions of HO(x) cycling much faster than HO(x) production and loss. The concentration of HO2 depends on [OH], which, to first order, has been observed to be a simple function of the solar zenith angle in the lower stratosphere. The partitioning between OH and HO2 is controlled by the local chemistry between the HO, radicals and O3, CO, NO, CIO, and BrO. The response of [HO(x)] to changes in [NO(x)] and [O3] is demonstrated. Further observations are necessary to illustrate the response of HO(x) to changes in halogen concentrations. A quantitative understanding of [HO2]/[OH] is important, since many of the reactions that control this ratio are directly involved in catalytic removal of O3 in the lower stratosphere and production of O3 in the upper troposphere.

Lanzendorf, E. J.↗

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 2: Stratospheric and free-tropospheric response

The paper constitutes Part 2 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric aerosol injection (SAI) at various single latitudes in the tropics, as simulated by three state-of-the-art Earth system models – CESM2-WACCM6, UKESM1.0, and GISS-E2.1-G. Building on Part 1 (Visioni et al., 2023) we demonstrate the role of biases in the climatological circulation and specific aspects of the model microphysics in driving the inter-model differences in the simulated sulfate distributions. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface SAI responses discussed in Part 1. We show that the differences in the aerosol spatial distribution can be explained by the significantly faster shallow branches of the Brewer–Dobson circulation in CESM2, a relatively isolated tropical pipe and older tropical age of air in UKESM, and smaller aerosol sizes and relatively stronger horizontal mixing (thus very young stratospheric age of air) in the two GISS versions used. We also find a large spread in the magnitudes of the tropical lower-stratospheric warming amongst the models, driven by microphysical, chemical, and dynamical differences. These lead to large differences in stratospheric water vapor responses, with significant increases in stratospheric water vapor under SAI in CESM2 and GISS that were largely not reproduced in UKESM. For ozone, good agreement was found in the tropical stratosphere amongst the models with more complex microphysics, with lower stratospheric ozone changes consistent with the SAI-induced modulation of the large-scale circulation and the resulting changes in transport. In contrast, we find a large inter-model spread in the Antarctic ozone responses that can largely be explained by the differences in the simulated latitudinal distributions of aerosols as well as the degree of implementation of heterogeneous halogen chemistry on sulfate in the models. The use of GISS runs with bulk microphysics demonstrates the importance of more detailed treatment of aerosol processes, with contrastingly different stratospheric SAI responses to the models using the two-moment aerosol treatment; however, some problems in halogen chemistry in GISS are also identified that require further attention. Overall, our results contribute to an increased understanding of the underlying physical mechanisms as well as identifying and narrowing the uncertainty in model projections of climate impacts from SAI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Satellite Measured Solar Protons from 1963-1993 and Their Influence on Ozone in a Changing Stratosphere

The fluxes of solar protons have been measured by a series of Interplanetary Monitoring Platform (IMP) satellites since 1963. Eight IMP satellites have been launched since 1963 providing excellent coverage of solar protons with energies from a few MeV to several hundred MeV. IMP 8, launched in October 1973, continues to provide proton measurements, twenty-six and a half (26 1/2) years after launch. These high energy solar protons rain down on the earth's polar atmosphere sporadically, primarily during solar proton events (SPEs) which typically last a few days. Solar protons with energies of 30 MeV or greater are capable of reaching the stratosphere and causing increases in odd nitrogen (NO(y)) constituents at polar latitudes ($>$ 60 degrees geomagnetic) which last for several months to years past the events. These enhanced NO(y) species can lead to significant upper stratospheric ozone depletions $ greater than $10\% during the gigantic SPEs that occurred in August 1972 and October 1989. We studied the effects of SPEs on the stratosphere from 1963 to the mid 1990s. During this time period, the stratospheric chlorine levels changed from relatively small in 1963 ($\sim$ 1 ppbv) to fairly substantial amounts in the mid-1990s ($\sim$ 3.3 ppbv). Our recently improved two-dimensional chemistry and transport atmospheric model was used to compute the effects of SPEs in this changing stratosphere. The long-lived SPE-produced NO(y) constituents were transported to lower stratospheric levels during winter after the events and caused impacts in the middle and lower stratosphere. Generally, the SPEs resulted in a decrease in ozone. However, during periods of high halogen loading these impacts resulted in interference with the chlorine and bromine loss cycles for ozone destruction. This interference actually led to a predicted total ozone increase that was especially notable in the time period 1992-4, a few years after the October 1989 SPE.

Jackman, Charles H.↗

Evaluation of SAGE II and Balloon-Borne Stratospheric Aerosol Measurements

Under funding from this proposal we evaluated measurements of stratospheric sulfate aerosols from three platforms. Two were satellite platforms providing solar extinction measurements, the Stratospheric Aerosol and Gas Experiment (SAGE) II using wavelengths from 0.386 - 1.02 microns, and the Halogen Occultation Experiment (HALOE) using wavelengths from 2.45 to 5.26 microns. The third set of measurements was from in situ sampling by balloonborne optical particle counters (OPCs). The goal was to determine the consistency among these data sets. This was accomplished through analysis of the existing measurement records, and through additional balloonborne OPC flights coinciding with new SAGE II observations over Laramie, Wyoming. All analyses used the SAGE II v 6.0 data. This project supported two balloon flights per year over Laramie dedicated to SAGE II coincidence. Because logistical factors, such as poor surface weather or unfavorable payload impact location, can make it difficult to routinely obtain close coincidences with SAGE II, we attempt to conduct nearly every Laramie flight (roughly one per month) in conjunction with a SAGE II overpass. The Laramie flight frequency has varied over the years depending on field commitments and funding sources. Current support for the Laramie measurements is from the National Science Foundation in addition to support from this NASA grant. We have also completed a variety of comparisons using aerosol measurements from SAGE II, OPCs, and HALOE. The instruments were compared for their various estimates of aerosol extinction at the SAGE II wavelengths and for aerosol surface area. Additional results, such as illustrated here, can be found in a recently accepted manuscript describing comparisons between SAGE II, HALOE, and OPCs for the period 1982 - 2000. While overall, the impression from these results is encouraging, the agreement of the measurements changes with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount is low SAGE II and HALOE extinctions are higher than the OPC estimates, while the SAGE II surface areas are lower than HALOE and the OPCS. Under high loading conditions, all three instruments mutually agree to within 50%.

Source record↗

Comparison of satellite ozone observations in coincident air masses in early November 1994

Ozone observed by seven satellite instruments, the Atmospheric Trace Molecule Spectroscopy instrument (ATMOS), Stratospheric Aerosol and Gas Experiment (SAGE) II, Polar Ozone and Aerosol Measurement (POAM) II instrument, Halogen Occultation Experiment (HALOE), Microwave Limb Sounder (MLS), Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA), and Millimeter-wave Atmospheric Sounder (MAS), during early November 1994 is mapped in equivalent latitude/potential temperature (EqL/ theta )space to facilitate nearly global comparisons of measurements taken in similar air masses.

atmospheric↗

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.↗

Continuous Lidar Monitoring of Polar Stratospheric Clouds at the South Pole

Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.

OZONE DESTRUCTION↗

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.↗

Extrapolation of earth-based solar irradiance measurements to exoatmospheric levels for broad-band and selected absorption-band observations

Techniques for extrapolating earth-based spectral band measurements of directly transmitted solar irradiance to equivalent exoatmospheric signal levels were used to aid in determining system gain settings of the Halogen Occultation Experiment (HALOE) sunsensor being developed for the NASA Upper Atmosphere Research Satellite and for the Stratospheric Aerosol and Gas (SAGE) 2 instrument on the Earth Radiation Budget Satellite. A band transmittance approach was employed for the HALOE sunsensor which has a broad-band channel determined by the spectral responsivity of a silicon detector. A modified Langley plot approach, assuming a square-root law behavior for the water vapor transmittance, was used for the SAGE-2 940 nm water vapor channel.

Reagan, John A.↗

Are models of catalytic removal of O3 by HO(x) accurate? Constraints from in situ measurements of the OH to HO2 ratio

Measurements of the ratio OH/HO2, NO, O3, ClO, and BrO were obtained at altitudes from 15-20 km and latitudes from 15-60 deg N. A method is presented for interpreting the rates of chemical transformations that (1) are responsible for over half the ozone removal rate in the lower stratosphere via reactions of HO2; and (2) control the abundance of HO2 through coupling to nitrogen and halogen radicals. The results show our understanding of the chemical reactions controlling the partitioning of OH and HO2 is complete and accurate and that the potential effects of 'missing chemistry' are strickly constrained in the region of the atmosphere encompassed by the observations. The analysis demonstrates that the sensitivity of the ratio OH/HO2 to changes in NO is described to within 12% by current models. This reduces by more than a factor of 2 the effect of uncertainty in the coupling of hydrogen and nitrogen radicals on the analysis of the potential effects of perturbations to odd notrogen in the lower statosphere.

Cohen, R. C.↗

Airborne Arctic Stratospheric Expedition 2: Air Parcel Trajectories

An overview of Airborne Arctic Stratospheric Expedition 2 is given. Effects of Pinatubo aerosol on stratospheric ozone at mid-latitudes, in situ measurements of ClO and ClO/HCl ratio, balloon-borne measurements of ClO, NO, and O3 in a volcanic cloud, and new observations of the NO(y)/N2O correlation in the lower stratosphere are discussed. Among other topics addressed are the following: in situ tracer correlations of methane, nitrous oxide, and ozone as observed aboard the DC-8, in situ measurements of changes in stratospheric aerosol and the N2O-aerosol relationship inside and outside of the polar vortex, measurements of halogenated organic compounds near the tropical tropopause, and airborne brightness measurements of the polar winter troposphere.

Source record↗

Data Comparison: Satellite and Falling Sphere Temperatures

Small meteorological rocketsondes providing temperature data have beam used for comparison with, and validation of measurements from satellite-borne instruments. A significant number of rocket-borne falling spheres were launched in conjunction with the Upper Atmosphere Research Satellite (UARS) for validation of the Halogen Occultation Experiment (HALOE), High Resolution Doppler Interferometer (HRDI), and the Microwave Limb Sounder (MLS) instruments. Upper stratosphere and mesosphere temperatures measured with these instruments on UARS are compared with inflatable spheres launched from Wallops Island (1992-1999), Brazil (1994), Hawaii (1992), Norway (1992), and Sweden (1993 and 1996). Time and space differences varied between the satellite measurement and the rocketsonde launch, for example HALOE overpasses occurred within 5 days and in some cases there were spatial differences of up to 30 degrees longitude. Validation measurements of the HRDI instrument occurred at Wallops Island when it passed within 20 minutes and 330 kilometers of the launch site. Because of discontinuity in the falling sphere drag coefficients when fall speed neared MACH 1 falling sphere temperatures near 70 kilometers attitude are biased toward lower temperatures. Availability of improved software and a new atmospheric model have helped to reduce this bias. The validated remote instrument measurements permit a new perspective of atmospheric structure to be formed, not always possible with the limited number of falling sphere measurements. Features of the remote measurement temperature profiles and their possible use to extend the climatological data base at the rocketsonde sites will be discussed.

Schmidlin, Francis J.↗

Thermal-vacuum testing and in-situ optical alignment measurements of the HALOE telescope/sun sensor assembly

Design features, test data and projected performance levels of the telescope/sun sensor assembly for the Halogen Occultation Experiment (HALOE) on board the Upper Atmosphere Research Satellite are described. HALOE will gather data on stratospheric chemical species with an IR telescope pointed through the atmosphere at the sun during occultation periods. The pointing accuracy will need to be 1 arcmin elevation and 1.6 arcmin azimuthal. Adjustments of the gimbaled instrument are guided by a sun sensor and its associated electronics. The components were subjected to thermal-vacuum, optical boresight stability tests and the data generated were compared with a finite element model of the telescope and sun sensor. The tests consisted of exposure to various thermal gradients while the telescope and sun sensor alignments were tracked by optical deflectometry. The thermal behavior was compared with predictions made with a finite difference model. Alignments were within tolerable ranges and the thermal behavior model was concluded valid for predicting the thermal behavior of orbiting instruments.

Foss, R. A.↗

Extrapolation of Earth-based solar irradiance measurements to exoatmospheric levels for broad-band and selected absorption-band observations

Techniques for extrapolating Earth-based spectral band measurements of directly transmitted solar irradiance to equivalent exoatmospheric signal levels were used to aid in determining system gain settings of the Halogen Occultation Experiment (HALOE) sunsensor system being developed for the NASA Upper Atmosphere Research Satellite and for the Stratospheric Aerosol and Gas (SAGE) 2 instrument on the Earth Radiation Budget Satellite. A band transmittance approach was employed for the HALOE sunsensor which has a broad-band channel determined by the spectral responsivity of a silicon detector. A modified Langley plot approach, assuming a square-root law behavior for the water vapor transmittance, was used for the SAGE-2 940 nm water vapor channel.

Reagan, J. A.↗

Evaluation of a Multi-Decadal Simulation of Stratospheric Ozone by Comparison with Total Ozone Mapping Spectrometer (TOMS) Observations

One key application of atmospheric chemistry and transport models is prediction of the response of ozone and other constituents to various natural and anthropogenic perturbations. These include changes in composition, such as the previous rise and recent decline in emission of man-made chlorofluorcarbons, changes in aerosol loading due to volcanic eruption, and changes in solar forcing. Comparisons of hindcast model results for the past few decades with observations are a key element of model evaluation and provide a sense of the reliability of model predictions. The 25 year data set from Total Ozone Mapping Spectrometers is a cornerstone of such model evaluation. Here we report evaluation of three-dimensional multi-decadal simulation of stratospheric composition. Meteorological fields for this off-line calculation are taken from a 50 year simulation of a general circulation model. Model fields are compared with observations from TOMS and also with observations from the Stratospheric Aerosol and Gas Experiment (SAGE), Microwave Limb Sounder (MLS), Cryogenic Limb Array Etalon Spectrometer (CLAES), and the Halogen Occultation Experiment (HALOE). This overall evaluation will emphasize the spatial, seasonal, and interannual variability of the simulation compared with observed atmospheric variability.

Douglass, Anne R.↗

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↗

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 statosphere during 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((1)D) from O2 photolysis and for heterogeneous production of HNO2. The data suggest more efficent catalytic removal of O3 by hydrogen and halogen radicals relative to nitrogen oxide radicals than predicted by models using recommendend rates and cross sections. Increased in (O3) in the lower stratosphere may be larger in response to inputs of NO(y) from supersonic aircraft than estimated by current assessment models.

Salawitch, R. J.↗

The Effect of Transport and Circulation Differences on Stratospheric Ozone Recovery in Two 35-year Three-dimensional Simulations

The NASA Global Modeling Initiative (GMI) has completed two 35-year simulations with WMO future baseline boundary conditions that simulate increasing N2O and CH4 emissions and decreasing organic chlorine and bromine emissions. Simulations were done with the GMI offline chemistry and transport model using 1) 1 year of winds from the Finite-Volume General Circulation Model (FV-GCM), repeated for the 35 years, and 2) 1 year of winds from the Finite-Volume Data Assimilation System (FV-DAS), repeated for 35-years. The simulations have full stratospheric chemistry. To understand differences in simulated ozone recoveries, basic transport and circulation differences between these models are evaluated. The distribution of mean age of stratospheric air in the FV-GCM run agrees well with observations in the lower stratosphere but the FV-DAS ages are generally too low. This implies circulation and mixing differences that will affect the distributions of other trace species such as CH4, NO, and the organic halogens, all of which are responding to changing boundary conditions and are involved in ozone loss. Realism of model transport is evaluated, with particular attention given to regions and seasons where ozone recovery is expected. Preliminary results indicate increasing ozone trends in the lowermost stratosphere in summer and in the Antarctic and Arctic lower stratosphere in winter and spring.

Bhartia, P. K.↗