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At least 289 records · Page 16

The effect of increased carbon dioxide concentrations on stratospheric ozone

Consideration is given to the influence on ozone of an increased carbon dioxide concentration, for which a measurable growth has been observed in the recent past. Increased carbon dioxide can indirectly affect ozone by perturbing atmospheric temperatures, which will alter ozone production, whose rate displays a fairly strong temperature dependence. This paper presents one-dimensional model results for the steady state ozone behavior when the CO2 concentration is twice its ambient level; the results account for coupling between chemistry and temperature. When the CO2 level doubled, the total ozone burden increased in relation to the ambient burden by 1.2-2.5%, depending on the vertical diffusion coefficient used. Above 30 km, ozone concentrations were larger than the ambient values, a maximum increase of 16% being reached at 43 km. In this region the relative variations were insensitive to the choice of diffusion coefficient. Below 30 km, ozone concentrations were smaller than the unperturbed values and were sensitive to the vertical diffusion profile in this region (10-30 km).

Boughner, R. E.↗

Examination of stratospheric ozone photochemistry in light of recent data

The consistency of stratospheric ozone photochemistry is examined using data from the Atmospheric Trace Molecule Spectroscopy (ATMOS) and LIMS experiments. The ATMOS experiment measured vertical profiles of important trace constituents and temperature in the stratosphere during 1985. These observations have been used to constrain the levels of odd nitrogen and odd chlorine in a photochemical model. This model yields O3 mixing ratios that are in good agreement with the observations. The deviation in ozone is less than 20 percent except near 52 km. The updated model has also been used in conjunction with the LIMS data to simulate the stratospheric photochemistry corresponding to the 1979 time period.

Natarajan, Murali↗

Atmospheric Transport and Photochemistry of Ozone Over Central Southern Africa During the Southern Africa Fire-Atmosphere Research Initiative

Vertically integrated back and forward trajectories for the 300-200, 700-500 and surface-800 hPa levels are calculated using Pretoria as point of origin for the Southern Africa Fire-Atmosphere Research Initiative (SAFARI) period September-October 1992. The transport fields are then combined to show both horizontal and vertical transport of air to and from Pretoria at the different levels. Air transport patterns in the vertical are linked to the occurrence of absolutely stable layers which are also evident in the 16 ozonesonde profiles recorded at Pretoria during SAFARI. The coherence of the stratification based on dynamical and ozone analysis permits the use of mean ozone profiles with air volume fluxes to interpret the ozone in terms of photochemistry and transport within stable layers. Extensive recirculation across the meridional plane at Pretoria implies that advection of ozone is slow and that photochemistry is responsible for the observed vertical structure over central southern Africa in September and October 1992. Requisite ozone formation rates are supported by model analysis of ozone and ozone precursors measured from SAFARI and Transport and Atmospheric Research Chemistry near the Equator-Atlantic aircraft.

Tyson, P. D.↗

Gravity and Rossby Wave Signatures in the Tropical Troposphere and Lower Stratosphere Based on Southern Hemisphere Additional Ozonesondes (SHADOZ), 1998-2007

Prior investigations attempted to determine the relative influence of advection and convective processes on ozone and water vapor distributions in the tropical tropopause layer (TTL) through analyses of tracers, related physical parameters (e.g., outgoing long-wave radiation, precipitable water, and temperature), or with models. In this study, stable laminae in Southern Hemisphere Additional Ozonesonde Network (SHADOZ) ozone profIles from 1998 to 2007 are interpreted in terms of gravity waves (GW) or Rossby waves (RW) that are identified with vertical and quasi-horizontal displacements, respectively. Using the method of Pierce and Grant (1998) as applied by Thompson et al. (2007a, 2007b, 2010, 2011), amplitudes and frequencies in ozone laminae are compared among representative SHADOZ sites over Africa and the Pacific, Indian, and Atlantic oceans. GW signals maximize in the TTL and lower stratosphere. Depending on site and season, GW are identified in up to 90% of the soundings. GW are most prevalent over the Pacific and eastern Indian oceans, a distribution consistent with vertically propagating equatorial Kelvin waves. Ozone laminae from RW occur more often below the tropical tropopause and with lower frequency 20%). Gravity wave and Rossby wave indices (GWI, RWI) are formulated to facilitate analysis of interannual variability of wave signatures among sites. GWI is positively correlated with a standard ENSO (El Nino-Southern Oscillation) index over American Samoa (14degS, 171degW) and negatively correlated at Watukosek, Java (7.5degS, 114degE), Kuala Lumpur (3degN, 102degE), and Ascension Island (80degS, 15degW). Generally, the responses of GW and RW to ENSO are consistent with prior studies.

Thompson, Anne M.↗

Updated Trends of the Stratospheric Ozone Vertical Distribution in the 60°S-60°N Latitude Range Based on the LOTUS Regression Model

This study presents an updated evaluation of stratospheric ozone profile trends in the 60°S - 60°N latitude range over the 2000 - 2020 period using an updated version of the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) regression model that was used to evaluate such trends up to 2016 for the last WMO Ozone Assessment (2018). In addition to the derivation of detailed trends as a function of latitude and vertical coordinates, the regressions are performed with the data sets averaged over broad latitude bands, i.e., 60°S–35°S, 20°S–20°N and 35°N–60°N. The same methodology as in the last Assessment is applied to combine trends in these broad latitude bands in order to compare the results with the previous studies. Longitudinally resolved merged satellite records are also considered in order to provide a better comparison with trends retrieved from ground-based records, e.g., lidar, ozone sondes, Umkehr, microwave and Fourier Transform Infrared (FTIR) spectrometers at selected stations where long-term time series are available. The study includes a comparison with trends derived from the REF-C2 simulations of the Chemistry Climate Model Initiative (CCMI-1). This work confirms past results showing an ozone increase in the upper stratosphere, which is now significant in the three broad latitude bands. The increase is largest in the northern and southern hemisphere midlatitudes, with ~2.2%/decade at ~2.1 hPa, and ~2.1%/decade at ~3.2 hPa respectively, compared to ~1.6%/decade at ~2.6 hPa in the tropics. New trend signals have emerged from the records, such as a significant decrease of ozone in the tropics around 35 hPa and a non-significant increase of ozone in the southern midlatitudes at about 20 hPa. Non-significant negative ozone trends are derived in the lowermost stratosphere, with the most pronounced trends in the tropics. While a very good agreement is obtained between trends from merged satellite records and the CCMI-1 REF-C2 simulation in the upper stratosphere, observed negative trends in the lower stratosphere are not reproduced by models at southern and, in particular, at northern midlatitudes, where models report an ozone increase. However, the lower stratospheric trend uncertainties are quite large, for both measured and modelled trends. Finally, 2000-2020 stratospheric ozone trends derived from the ground-based and longitudinally resolved satellite records are in reasonable agreement over the European Alpine and tropical regions, while at the Lauder station in the southern hemisphere mid-latitudes they show some differences.

Stratospheric ozone trends↗

Improved Limb Atmospheric Spectrometer (ILAS) for polar stratospheric trace gas measurements

The Improved Limb Atmospheric Spectrometer (ILAS) is a grating spectrometer designed to measure vertical profiles of high latitude stratospheric constituents in a solar occultation mode. ILAS measurement gases are ozone (03), methane (CH4), nitrous oxide (N2O), nitric acid (HNO3), water vapor (H2O), nitrogen dioxide (NO2), and CFC-11 using an IR channel. Temperature, pressure, and aerosol are also measured using a visible channel. The IR channel consists of 44 detector elements which cover the spectral range 6.2 to 11.8 microns, and the visible channel is composed of 1024 pixels that cover 753 to 784 nm. ILAS will be installed on the Advanced Earth Observing Satellite (ADEOS) which will be launched in 1995. Instrument design data are outlined.

Yokota, Tatsuya↗

Feasibility Study For A Spaceborne Ozone/Aerosol Lidar System

Because ozone provides a shield against harmful ultraviolet radiation, determines the temperature profile in the stratosphere, plays important roles in tropospheric chemistry and climate, and is a health risk near the surface, changes in natural ozone layers at different altitudes and their global impact are being intensively researched. Global ozone coverage is currently provided by passive optical and microwave satellite sensors that cannot deliver high spatial resolution measurements and have particular limitations in the troposphere. Vertical profiling DIfferential Absorption Lidars (DIAL) have shown excellent range-resolved capabilities, but these systems have been large, inefficient, and have required continuous technical attention for long term operations. Recently, successful, autonomous DIAL measurements have been performed from a high-altitude aircraft (LASE - Lidar Atmospheric Sensing Experiment), and a space-qualified aerosol lidar system (LITE - Laser In-space Technology Experiment) has performed well on Shuttle. Based on the above successes, NASA and the Canadian Space Agency are jointly studying the feasibility of developing ORACLE (Ozone Research with Advanced Cooperative Lidar Experiments), an autonomously operated, compact DIAL instrument to be placed in orbit using a Pegasus class launch vehicle.

Campbell, Richard E.↗

Southern Hemispheric nitrous oxide measurements obtained during 1987 airborne Antarctic ozone experiment

The chemical lifetime of N2O is about 150 years, which makes it an excellent dynamical tracer of air motion on the time scale of the ozone depletion event. For these reasons it was chosen to help test whether dynamical theories of ozone loss over Antarctica were plausible, particularly the theory that upwelling ozone-poor air from the troposphere was replacing ozone-rich stratospheric air. The N2O measurements were made with the Airborne Tunable Laser Absorption Spectrometer (ATLAS) aboard the NASA ER-2 aircraft. The detection technique involves measuring the diffential absorption of the IR laser radiation as it is rapidly scanned over an N2O absorption feature. For the AAOE mission, the instrument was capable of making measurements with a 1 ppb sensitivity, 1 second response time, over an altitude range of 10 to 20 kilometers. The AAOE mission consisted of a series of 12 flights from Punta Arenas (53S) into the polar vortex (approximately 72S) at which time a vertical profile from 65 to 45 km and back was performed. Comparison of the observed profiles inside the vortex with N2O profiles obtained by balloon flights during the austral summer showed that an overall subsidence had occurred during the winter of about 5 to 6 km. Also, over the course of the mission (mid-August to late September), no trend in the N2O vertical profile, either upward or downward, was discernible, eliminating the possibility that upwelling was the cause of the observed ozone decrease.

Podolske, J. R.↗

Past Changes in the Vertical Distribution of Ozone Part 1: Measurement Techniques, Uncertainties and Availability

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given.

stratospheric ozone layer measurement↗

Mobile lidar system for measurement of water vapor mixing ratio and ozone number density

The Water Vapor Lidar was modified and extended to make differential absorption measurements of ozone. Water vapor measurements make use of a weak molecular scattering process known as Raman scattering. It is characterized by a shift in wavelength of the scattered beam of light relative to the incident one. Some of the energy of the incident photon is converted to vibrational or rotational energy within the molecule leaving the scattered photon shifted to a slightly longer wavelength. When performing water vapor measurements, profiles are acquired of water vapor mixing ratio from near the ground to beyond 7 km every 2 minutes. By forming a color composite image of the individual profiles, the spatial and temporal evolution of water vapor is visible with vertical resolution of 75 to 150m and temporal resolution of 2 minutes. The ozone lidar is intended for use as a cross calibration facility for other stationary ozone lidar systems. The ozone measurement employs the technique known as differential absorption. The backscattered laser radiation from two different wavelengths is measured. Successful measurements of 308 nm returns were made from 80 km with an averaging period of 6 hours. Using these data and a standard atmosphere density curve, an ozone number density profile was made which agrees very well with the standard ozone curve between 20 and 40 km.

Whiteman, D.↗

The Limb Infrared Monitor of the Stratosphere - Experiment description, performance, and results

An experiment and results, using a six-channel infrared radiometer aboard the Nimbus 7 spacecraft to sound the composition and structure of the middle atmosphere, are described. The measurement requirements are discussed, and critical instrument parameters are identified. Next, the instrument and its laboratory calibration are described. Temperature accuracy and precision are estimated to be 2 K and about 0.4 K respectively. Accuracy of the trace gas measurements is about 25 percent, comparable to the estimated accuracy of the in situ comparison data; their precision is about 0.25 ppmv for ozone and water vapor and 0.2 ppbv for nitric acid and nitrogen dioxide. Examples of the vertical profiles, maps, and cross sections of the data show previously unobserved variations with latitude, altitude, and time. The results demonstrate that infrared limb scanning is an extremely powerful method for sounding the middle atmosphere.

Gille, J. C.↗

Western US Tropospheric Ozone: An Assessment of Vertical and Seasonal Variations over California and Nevada

In the rural western US free-tropospheric O3 has risen in recent years as a result of rising Asian emissions, deep stratospheric intrusions and more frequent wildfires. This increasing O3 trend combined with the high surface elevation of much of the western US, which aids mixing between boundary layer and free-troposphere, pose challenges in attaining the more stringent O3 National Ambient Air Quality Standard (NAAQS) at many western US rural surface sites. As such, the ability to identify various sources and transport mechanisms that contribute towards surface O3 is increasingly important. This paper analyzes vertical profiles of O3 from the Alpha Jet Atmospheric eXperiment (AJAX) over California and Nevada, ozonesondes from Trinidad Head, CA and tropospheric ozone profiles from the differential absorption lidar (DIAL) at the JPL Table Mountain Facility, CA. Surface O3 from the US EPA Clean air Status and Trends Network (CASNET) are used to discuss surface trends. GEOS-Chem determines the trends in regional O3 and assess the contributions of various sources on surface O3. And Realtime Air Quality Modeling System (RAQMS) is used to forecast and interpret free-tropospheric observations. Specifically we will address the following questions: What are the effects of the lowered NAAQS? Do we observe elevated O3 during 2012 at surface sites reported in previous studies? And if so, what are the causes? How variable is free-tropospheric O3 over California and Nevada? How frequently do we observe high O3 lamina in the free troposphere and what are the surface impacts?

tropospheric↗

Quasi-biennial oscillations of ozone and diabatic circulation in the equatorial stratosphere

The quasi-biennial oscillation (QBO) in ozone in the equatorial stratosphere is obtained by analyzing the Stratospheric Aerosol and Gas Experiment (SAGE) data from 1984 to 1989. The phase of the ozone QBO in the lower stratosphere is found to precede the zonal wind QBO by several months as opposed to the theoretically expected in-phase relationship between the two. A mechanistic model is developed to explore possible reasons for this disagreement. The model is capable of simulating the actual time evolution of the ozone QBO by introducing the observed zonal wind profile as input. The modeled results confirm the conventional view that the ozone QBO is generated by the vertical ozone advection that is driven to maintain the temperature structure against radiative damping. However, a series of experiments emphasizes the importance of the feedback of the ozone QBO to the diabatic heating through the absorption of solar radiation. Due to this effect, the phase of the ozone QBO shifts up to a quarter cycle ahead and approaches that of the temperature QBO. Because of this inphase relationship, the feedback of the ozone QBO to the diabatic heating acts to compensate for the radiative damping of the temperature structure, thus reducing the magnitude of the induced diabatic circulation. Because the reduction of the magnitude of the vertical motion facilitates downward transport of easterly momentum by the mean flow, this feedback process can help to resolve the insufficiency of the easterly momentum in driving the dynamical QBO in general circulation models (GCMs). It should be emphasized that more sophisticated models that allow for full interaction between the chemical species and radiative and dynamical processes should be developed to improve our understanding of both dynamical and ozone QBOs.

Hasebe, Fumio↗

Constraining Remote Oxidation Capacity with ATom Observations

The global oxidation capacity, defined as the tropospheric mean concentration of the hydroxyl radical (OH), controls the lifetime of reactive trace gases in the atmosphere such as methane and carbon monoxide (CO). Models tend to underestimate the methane lifetime and CO concentrations throughout the troposphere, which is consistent with excessive OH. Approximately half the oxidation of methane and non-methane volatile organic compounds (VOCs) is thought to occur over the oceans where oxidant chemistry has received little validation due to a lack of observational constraints. We use observations from the first two deployments of the NASA ATom aircraft campaign during July–August 2016 and January–February 2017 to evaluate the oxidation capacity over the remote oceans and its representation in the GEOS-Chem chemical transport model. The model successfully simulates the magnitude and vertical profile of remote OH within the measurement uncertainties. Comparisons against the drivers of OH production (water vapor, ozone, and NOy concentrations, ozone photolysis frequencies) also show minimal bias with the exception of wintertime NOy, for which a model overestimate may indicate insufficient wet scavenging and/or missing loss on seasalt aerosol but large uncertainties remain that require further studies of NOy partitioning and removal in the troposphere. During the ATom-1 deployment, OH reactivity (OHR) below 3 km is significantly enhanced, and this is not captured by the sum of its measured components (cOHRobs) or by the model (cOHRmod). This enhancement could suggest missing reactive VOCs but cannot be explained by new estimates of ocean VOC sources and additional modeled reactivity in this region would be difficult to reconcile with the full suite of ATom measurement constraints. The model generally reproduces the magnitude and seasonality of cOHRobs but underestimates the contribution of oxygenated VOC, mainly acetaldehyde, which is severely underestimated throughout the troposphere despite its calculated lifetime of less than a day. Missing model acetaldehyde in previous studies was attributed to measurement uncertainties that have been largely resolved. Observations of peroxyacetic acid (PAA) provide new support for remote levels of acetaldehyde. The underestimate in modeled acetaldehyde and PAA is present throughout the year in both hemispheres and peaks during Northern Hemisphere summer. The addition of ocean VOC sources in the model increases annual surface cOHRmod by 10 % and improves model-measurement agreement for acetaldehyde particularly in winter but cannot resolve the model summertime bias. Doing so would require a 100 Tg yr−1 source of a long-lived unknown precursor throughout the year with significant additional emissions in the Northern Hemisphere summer. Improving the model bias for remote acetaldehyde and PAA is unlikely to fully resolve previously reported model global biases in OH and methane lifetime, suggesting that future work should examine the sources and sinks of OH over land.

Travis, Katherine R.↗

Spatial-frequency response of the Limb Infrared Monitor of the Stratosphere /LIMS/ radiometer

The Limb Infrared Monitor of the Stratosphere (LIMS), an experiment on the Nimbus-7 satellite, is designed to scan the earth's limb vertically and measure spectral emission profiles of trace atmospheric gases believed to be important in processes controlling the stratospheric ozone distribution. Experiment objectives are reviewed and several analyses and measurements are described which were performed to determine the adequacy of the system for satisfying these objectives. Adequate spatial-frequency response for all the spectral channels is required to provide, through inversion of the measured limb-radiance profiles, important information about the temperature, structure, and composition of the atmosphere. From the LIMS design-model data, the MTF was calculated for the optical system, the detector field mask, the electronics, and the overall system, for each channel. The signal output performance of the instrument was predicted from the system MTF data model input radiance data for each channel. MTF measurements made on the flight sensor confirmed the analytical results. The predictions indicate that the instrument can satisfy the basic measurement objectives of the experiment.

Wilson, R. G.↗

Absorption in Extended Inhomogeneous Clouds

The launch of several different sensors, including CloudSat, into the A-train constellation of satellites allows us for the first time to compute absorption that can occur in realistic vertically inhomogeneous clouds including multiple cloud decks. CloudSat data show that these situations are common. Therefore, understanding vertically inhomogeneous clouds is important from both climate and satellite atmospheric composition remote sensing perspectives. Satellite passive sensors that operate from the near IR to the UV often rely on radiative cloud pressures derived from absorption in oxygen bands (A, B, gamma, or O2-O2 bands) or from rotational-Raman scattering in order to retrieve information about atmospheric trace gases. The radiative cloud pressure is distinct from the physical cloud top derived from thermal infrared measurements. Therefore, the combination of information from different passive sensors yields some information about the cloud vertical profile. When either or both the clouds or atmospheric absorbers (trace gases and aerosols) are vertically inhomogeneous, the use of an effective cloud pressure derived from these approaches may lead to errors. Here, we focus on several scenarios (deep convective clouds and distinct two layer clouds) based on realistic cloud optical depth vertical profiles derived from the CloudSatfMODIS combination. We focus on implications for trace-gas column amount retrievals (specifically ozone and NO2) and derived surface UV irradiance from the Ozone Monitoring Instrument (OMI) on the Atrain Aura platform.

Joiner, Joanna↗

Tropospheric Ozone Source Attribution in Southern California during Summer 2014 Based on Lidar Measurements and Model Simulations

In the past decades, significant efforts have been made to increase tropospheric ozone long-term monitoring. A large number of ground-based, airborne and space-borne instruments are currently providing valuable data to contribute to better understand tropospheric ozone budget and variability. Nonetheless, most of these instruments provide in-situ surface and column-integrated data, whereas vertically resolved measurements are still scarce. Besides ozonesondes and aircraft, lidar measurements have proven to be valuable tropospheric ozone profilers. Using the measurements from the tropospheric ozone differential absorption lidar (DIAL) located at the JPL Table Mountain Facility, California, and the GEOS-Chem and GEOS-5 model outputs, the impact of the North American monsoon on tropospheric ozone during summer 2014 is investigated. The influence of the Monsoon lightning-induced NOx will be evaluated against other sources (e.g. local anthropogenic emissions and the stratosphere) using also complementary data such as backward-trajectories analysis, coincident water vapor lidar measurements, and surface ozone in-situ measurements.

Lidar↗