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NASA NTRS1994

Contributions of a Tunable Diode Laser Instrument (ATLAS) to the Stratospheric Ozone Depletion Question

The Airborne Tunable Laser Absorption Spectrometer - ATLAS - was designed and built at the NASA Ames Research Center and operates on the NASA ER-2 high altitude research aircraft. ATLAS has taken part in a number of important polar and mid-latitude research campaigns, since 1987, focused on various aspects of stratospheric ozone chemistry and dynamics. The chief measurement carried out by the ATLAS second harmonic diode laser spectrometer is of the important atmospheric tracer N2O. Using N2O as an inert tracer we have been able to gain significant new information on polar vortex dynamics and on the correlations of several important long-lived tracers in the stratosphere. The correlation of N2O with NOy (total reactive nitrogen) has been shown to be linear for a great variety of unperturbed stratospheric conditions, and the breakdown of this correlation has been used to detect denitrification by PSCs in the polar vortex, especially in the Antarctic spring. Denitrification is an important step in the process of ozone hole formation in the austral spring. Correlations of N2O with CFCs and CH4 have led to improved estimates of atmospheric lifetimes of these important molecules. Finally the correlation of N2O with CO2, the latter now being measured with great precision by a new instrument on the ER-2, has led to a significant new tool for studying horizontal and vertical mixing in the lower stratosphere, a tool which is very useful in assessing the potential effects of high speed civil transport aircraft in the lower stratosphere. A new, light-weight version of ATLAS is currently being built for unmanned high altitude aircraft, specifically the new Perseus vehicle. We will give a brief description of this effort.

Loewenstein, Max↗

NASA NTRS2001

The Evolution of Stratospheric Data Assimilation Systems

The use of model-assimilated meteorological observations for stratospheric research has become routine since the late 1980's. The first stratospheric assimilation systems were straightforward extensions of systems developed for tropospheric weather forecasting. During the 1990's systems were developed that more directly addressed the specifics of stratospheric applications. These developments include better treatment of the satellite observations and improved models that better represent the residual circulation in the assimilated data sets. This talk will review the evolution of stratospheric data assimilation and its application, especially to problems of tracer transport. The new data assimilation currently under validation at NASA will be described in some detail, and results from the validation exercise will be presented. This data assimilation system sits at the foundation of a proposed stratospheric reanalysis that covers the era of the Upper Atmosphere Research Satellite (UARS).

Rood, Richard B.↗

NASA NTRS2001

What Controls the Arctic Lower Stratosphere Temperature?

The temperature of the Arctic lower stratosphere is critical for understanding polar ozone levels. As temperatures drop below about 195 K, polar stratospheric clouds form, which then convert HCl and ClONO2 into reactive forms that are catalysts for ozone loss reactions. Hence, the lower stratospheric temperature during the March period is a key parameter for understanding polar ozone losses. The temperature is basically understood to be a result of planetary waves which drive the polar temperature away from a cold "radiative equilibrium" state. This is demonstrated using NCEP/NCAR reanalysis calculations of the heat flux and the mean polar temperature. The temperature during the March period is fundamentally driven by the integrated impact of large scale waves moving from the troposphere to the stratosphere during the January through February period. We will further show that the recent cold years in the northern polar vortex are a result of this weakened wave driving of the stratosphere.

Newman, Paul A.↗

NASA NTRS2002

Homogenous Surface Nucleation of Solid Polar Stratospheric Cloud Particles

A general surface nucleation rate theory is presented for the homogeneous freezing of crystalline germs on the surfaces of aqueous particles. While nucleation rates in a standard classical homogeneous freezing rate theory scale with volume, the rates in a surface-based theory scale with surface area. The theory is used to convert volume-based information on laboratory freezing rates (in units of cu cm, seconds) of nitric acid trihydrate (NAT) and nitric acid dihydrate (NAD) aerosols into surface-based values (in units of sq cm, seconds). We show that a surface-based model is capable of reproducing measured nucleation rates of NAT and NAD aerosols from concentrated aqueous HNO3 solutions in the temperature range of 165 to 205 K. Laboratory measured nucleation rates are used to derive free energies for NAT and NAD germ formation in the stratosphere. NAD germ free energies range from about 23 to 26 kcal mole, allowing for fast and efficient homogeneous NAD particle production in the stratosphere. However, NAT germ formation energies are large (greater than 26 kcal mole) enough to prevent efficient NAT particle production in the stratosphere. We show that the atmospheric NAD particle production rates based on the surface rate theory are roughly 2 orders of magnitude larger than those obtained from a standard volume-based rate theory. Atmospheric volume and surface production of NAD particles will nearly cease in the stratosphere when denitrification in the air exceeds 40 and 78%, respectively. We show that a surface-based (volume-based) homogeneous freezing rate theory gives particle production rates, which are (not) consistent with both laboratory and atmospheric data on the nucleation of solid polar stratospheric cloud particles.

Tabazadeh, A.↗

NASA NTRS2002

Sensitivity of Lower Stratospheric Assimilated Ozone on Error Covariance Modeling and Data Selection

Assimilated ozone is produced at the NASA/Goddard Data Assimilation Office by blending ozone retrieved from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument and the Earth Probe Total Ozone Mapping Spectrometer (EP TOMS) measurements into an off-line transport model. The current system tends to overestimate the amount of lower stratospheric ozone. This is a region where ozone plays a key role in the forcing of climate. A biased ozone field in this region will adversely impact calculations of the stratosphere-troposphere exchange and, when used as a first guess in retrievals, the values determined from satellite observations. Since these are all important applications of assimilated ozone products, effort is being directed towards reducing this bias. The SBUV ozone data have a coarse vertical resolution with increased uncertainty below the ozone maximum, and TOMS provides only total ozone columns. Thus, the assimilated ozone in the lower stratosphere, and its vertical distribution in particular, are only weakly constrained by the incoming SBUV and TOMS data. Consequently, the assimilated ozone distribution should be sensitive to changes in inputs to the statistical analysis scheme. Accordingly, the sensitivity of the assimilated lower stratospheric ozone fields to changes in the TOMS error-covariance modeling and the SBUV data selection has been investigated. The use of a spatially correlated TOMS error covariance model led to improvements in the product. However, withholding the SBUV/2 data for the layer between 63 and 126 hPa typically degraded the product, a result which vindicates the use of this layer ozone product, despite its known errors. These efforts to improve the lower stratospheric distribution will be extended to include a more advanced forecast error covariance model, and by assimilating ozone products from new instruments on Envisat and EOS Aura.

Stajner, Ivanka↗

NASA NTRS2002

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.↗

NASA NTRS2003

On the Eastward Travelling Wavenumber Two in the Northern Stratosphere

Disturbances in the middle atmosphere are often interpreted in the framework of waves superimposed on a zonal-mean flow. This paper presents an analysis of travelling waves in the northern hemisphere stratosphere, concentrating on planetary wavenumber two (W2). Space-time spectral analysis reveals the existence of a substantial eastward-travelling planetary W2 at high latitudes in winter. While a similar feature is well documented in the southern hemisphere stratosphere, where it is observed in most winters, this northern hemisphere counterpart is less common and has not been examined in detail. A climatology of occurrence of the wave is given for the northern stratospheric winter. It is denoted as the quasi-16-day eastward travelling W2, because of its dominant periodicity, which ranges from about one to three weeks. Although the wave has some similarities with the southern hemispheric wave, there is much larger interannual and intraseasonal variability in the northern hemisphere. will emphasize the variations in the spatial and temporal structure of this wave, as isolated in meteorological analyses of radiosonde and satellite data. The possible role of these travelling waves in preconditioning the stratosphere as a precursor to sudden stratospheric warmings in both hemispheres will be discussed.

Pawson, Steven↗

NASA NTRS2003

Ultraviolet Radiation and Stratospheric Ozone

Ultraviolet radiation from the sun produces ozone in the stratosphere and it participates in the destruction of ozone. Absorption of solar ultraviolet radiation by ozone is the primary heating mechanism leading to the maximum in temperature at the stratopause. Variations of solar ultraviolet radiation on both the 27-day solar rotation period and the 11-year solar cycle affect ozone by several mechanisms. The temperature and ozone in the upper stratosphere respond to solar uv variations as a coupled system. An increase in uv leads to an increase in the production of ozone through the photolysis of molecular oxygen. An increase in uv leads to an increase in temperature through the heating by ozone photolysis. The increase in temperature leads to a partially-offsetting decrease in ozone through temperature-dependent reaction rate coefficients. The ozone variation modulates the heating by ozone photolysis. The increase in ozone at solar maximum enhances the uv heating. The processes are understood and supported by long-term data sets. Variation in the upper stratospheric temperatures will lead to a change in the behavior of waves propagating upward from the troposphere. Changes in the pattern of wave dissipation will lead to acceleration or deceleration of the mean flow and changes in the residual or transport circulation. This mechanism could lead to the propagation of the solar cycle uv variation from the upper stratosphere downward to the lower stratosphere. This process is not well-understood and has been the subject of an increasing number of model studies. I will review the data analyses for solar cycle and their comparison to model results.

Stolarski, R.↗

NASA NTRS2004

Quasi-Liquid Layer Formation on Ice under Stratospheric Conditions

Characterization of the interaction of hydrogen chloride (HCl) with ice is essential to understanding at a molecular level the processes responsible for ozone depletion involving polar stratospheric cloud (PSC) particles. To explain the catalytic role PSC particle surfaces play during chlorine activation, we proposed previously that HCl induces the formation of a disordered region on the ice surface, a quasi-liquid layer (QLL), at stratospheric conditions. The QLL is known to exist in pure ice crystals at temperatures near the melting point, but its existence at stratospheric temperatures (-85 C to -70 C) had not been reported yet. We studied the interaction of HCl with ice under stratospheric conditions using the complementary approach of a) ellipsometry to directly monitor the ice surface, using chemical ionization mass spectrometry (CIMS) to monitor the gas phase species present in the ellipsometry experiments, and b) flow-tube experiments with CIMS detection. Here we show that trace amounts of HCl induce QLL formation at stratospheric temperatures, and that the QLL enhances the chlorine-activation reaction of HCl with chlorine nitrate (ClONO2), and also enhances acetic acid (CH3COOH) adsorption.

McNeill, V. Faye↗

NASA NTRS2005

Attribution of Recovery in Lower-Stratospheric Ozone

Multiple satellite and ground-based observations provide consistent evidence that the thickness of Earth's protective ozone layer has stopped declining since 1997, close to the time of peak stratospheric halogen loading. Regression analyses with Effective Equivalent Stratospheric Chlorine (EESC) in conjunction with further analyses using more sophisticated photochemical model calculations constrained by satellite data demonstrate that the cessation of ozone depletion between 18-25 km altitude is consistent with a leveling off of stratospheric abundances of chlorine and bromine, due to the Montreal Protocol and its amendments. However, ozone increases in the lowest part of the stratosphere, from the tropopause to 18 km, account for about half of the improvement in total column ozone during the past 9 years at northern hemisphere mid-latitudes. The increase in ozone for altitudes below 18 km is most likely driven by changes in transport, rather than driven by declining chlorine and bromine. Even with this evidence that the Montreal Protocol and its amendments are having the desired, positive effect on ozone above 18 km, total column ozone is recovering faster than expected due to the apparent transport driven changes at lower altitudes. Accurate prediction of future levels of stratospheric ozone will require comprehensive understanding of the factors that drive temporal changes at various altitudes, and partitioning of the recent transport-driven increases between natural variability and changes in atmospheric structure perhaps related to anthropogenic climate change.

Yang, Eun-Su↗

NASA NTRS2006

Attribution of Recovery in Lower-stratospheric Ozone

Yang, Eun-Su↗

NASA NTRS2008

Stratospheric Ozone in the Post-CFC Era

Vertical and latitudinal changes in the stratospheric ozone in the post-chlorofluorocarbon (CFC) era are investigated using simulations of the recent past and the 21st century with a coupled chemistry-climate model. Model results reveal that, in the 2060s when the stratospheric halogen loading is projected to return to its 1980 values, the extratropical column ozone is significantly higher than that in 1975-1984, but the tropical column ozone does not recover to 1980 values. Upper and lower stratospheric ozone changes in the post- CFC era have very different patterns. Above 15 hPa ozone increases almost latitudinally uniformly by 6 Dobson Unit (DU), whereas below 15 hPa ozone decreases in the tropics by 8 DU and increases in the extratropics by up to 16 DU. The upper stratospheric ozone increase is a photochemical response to greenhouse gas induced strong cooling, and the lower stratospheric ozone changes are consistent with enhanced mean advective transport due to a stronger Brewer-Dobson circulation. The model results suggest that the strengthening of the Brewer-Dobson circulation plays a crucial role in ozone recovery and ozone distributions in the post-CFC era.

Li, Feng↗

NASA NTRS2009

Mechanisms and Feedbacks Causing Changes in Upper Stratospheric Ozone in the 21st Century

Stratospheric ozone is expected to increase during the 21st century as the abundance of halogenated ozone-depleting substances decrease to 1960 values. However, climate change will likely alter this "recovery" of stratospheric ozone by changing stratospheric temperatures, circulation, and abundance of reactive chemical species. Here we quantity the contribution of different mechanisms to changes in upper stratospheric ozone from 1960 to 2100 in the Goddard Earth Observing System Chemistry-Climate Model (GEOS CCM), using multiple linear regression analysis applied to simulations using either Alb or A2 greenhouse gas (GHG) scenarios. In both these scenarios upper stratospheric ozone has a secular increase over the 21st century. For the simulation using the Alb GHG scenario, this increase is determined by the decrease in halogen amounts and the greenhouse gas induced cooling, with roughly equal contributions from each mechanism. There is a larger cooling in the simulation using the A2 GHG scenario, but also enhanced loss from higher NOy and HOx concentrations, which nearly offsets the increase due to cooler temperatures. The resulting ozone evolutions are similar in the A2 and Alb simulations. The response of ozone due to feedbacks from temperature and HOx changes, related to changing halogen concentrations, are also quantified using simulations with fixed halogen concentrations.

Oman, Luke↗

NASA NTRS2010

Quantifying Uncertainty in Projections of Stratospheric Ozone Over the 21st Century

Future stratospheric ozone concentrations will be determined both by changes in the concentration of ozone depleting substances (ODSs) and by changes in stratospheric and tropospheric climate, including those caused by changes in anthropogenic greenhouse gases (GHGs). Since future economic development pathways and resultant emissions of GHGs are uncertain, anthropogenic climate change could be a significant source of uncertainty for future projections of stratospheric ozone. In this pilot study, using an ensemble of opportunity of chemistry-climate model (CCM) simulations, the contribution of scenario uncertainty from different plausible emissions pathways for 10 ODSs and GHGs to future ozone projections is quantified relative to the contribution from model uncertainty and internal variability of the chemistry-climate system. For both the global, annual mean ozone concentration and for ozone in specific geographical regions, differences between CCMs are the dominant source of uncertainty for the first two-thirds of the 21 st century, up-to and after the time when ozone concentrations 15 return to 1980 values. In the last third of the 21st century, dependent upon the set of greenhouse gas scenarios used, scenario uncertainty can be the dominant contributor. This result suggests that investment in chemistry-climate modelling is likely to continue to refine projections of stratospheric ozone and estimates of the return of stratospheric ozone concentrations to pre-1980 levels.

Charlton-Perez, A. J.↗

NASA NTRS2010

Response of the Antarctic Stratosphere to Two Types of El Nino Events

This study is the first to identify a robust El Nino/Southern Oscillation (ENSO) signal in the Antarctic stratosphere. El Nino events are classified as either conventional "cold tongue" events (positive SST anomalies in the Nino 3 region) or "warm pool" events (positive SST anomalies in the Nino 4 region). The ERA-40, NCEP and MERRA meteorological reanalyses are used to show that the Southern Hemisphere stratosphere responds differently to these two types of El Nino events. Consistent with previous studies, "cold tongue" events do not impact temperatures in the Antarctic stratosphere. During "warm pool" El Nino events, the poleward extension and increased strength of the South Pacific Convergence Zone (SPCZ) favor an enhancement of planetary wave activity during the SON season. On average, these conditions lead to higher polar stratospheric temperatures and a weakening of the Antarctic polar jet in November and December, as compared with neutral ENSO years. The phase of the quasi-biennial oscillation (QBO) modulates the stratospheric response to "warm pool" El Nino events: the strongest planetary wave driving events are coincident with the easterly phase of the QBO.

Hurwitz, M. M.↗

NASA NTRS2010

QBO Influence on Polar Stratospheric Variability in the GEOS Chemistry-Climate Model

The quasi-biennial oscillation modulates the strength of both the Arctic and Antarctic stratospheric vortices. Model and observational studies have found that the phase and characteristics of the quasi-biennial oscillation (QBO) contribute to the high degree of variability in the Arctic stratosphere in winter. While the Antarctic stratosphere is less variable, recent work has shown that Southern Hemisphere planetary wave driving increases in response to "warm pool" El Nino events that are coincident with the easterly phase of the QBO. These events hasten the breakup of the Antarctic polar vortex. The Goddard Earth Observing System (GEOS) chemistry-climate model (CCM) is now capable of generating a realistic QBO, due a new parameterization of gravity wave drag. In this presentation, we will use this new model capability to assess the influence of the QBO on polar stratospheric variability. Using simulations of the recent past, we will compare the modeled relationship between QBO phase and mid-winter vortex strength with the observed Holton-Tan relation, in both hemispheres. We will use simulations of the 21 St century to estimate future trends in the relationship between QBO phase and vortex strength. In addition, we will evaluate the combined influence of the QBO and El Nino/Southern Oscillation (ENSO) on the timing of the breakup of the polar stratospheric vortices in the GEOS CCM. We will compare the influence of these two natural phenomena with trends in the vortex breakup associated with ozone recovery and increasing greenhouse gas concentrations.

Hurwitz, M. M.↗

NASA NTRS2009

Stratospheric Ozone in the Post-CFC Era

Vertical and latitudinal changes in the stratospheric ozone in the post-chlorofluorocarbon (CFC) era are investigated using simulations of the recent past and the 21st century with a coupled chemistry-climate model. Model results reveal that, in the 2060s when the stratospheric halogen loading is projected to return to its 1980 values, the extratropical column ozone is significantly higher than that in 1975-1984, but the tropical column ozone does not recover to 1980 values. Upper and lower stratospheric ozone changes in the post-CFC era have very different patterns. Above 15 hPa ozone increases almost latitudinally uniformly by 6 Dobson Unit (DU), whereas below 15 hPa ozone decreases in the tropics by 8 DU and increases in the extratropics by up to 16 DU. The upper stratospheric ozone increase is a photochemical response to greenhouse gas induced strong cooling, and the lower stratospheric ozone changes are consistent with enhanced mean advective transport due to a stronger Brewer-Dobson circulation. The model results suggest that the strengthening of the Brewer-Dobson circulation plays a crucial role in ozone recovery and ozone distributions in the post-CFC era.

Li, F.↗

NASA NTRS2011

Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange

We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of approximately 60 ppbv and NOx of approximately 25 pptv throughout spring and summer with CO decreases from approximately 145 ppbv in spring to approximately 100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140-160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (approximately 800 pptv in spring and approximately 1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of approximately 120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

Liang, Q.↗