Aircraft measurements of oxides of nitrogen along the eastern rim of the Asian continent: Winter observations

Aircraft observations of oxides of nitrogen (NO _y ), measured with a ferrous sulfate converter, over the sea surrounding the Japanese islands (30–43° N, 131–141° E) were carried out in the winter of 1983 and 1984 at altitudes mostly between 3 and 8 km. NO _y defined here is the sum of NO, NO₂, and other unstable oxides of nitrogen that are converted to NO by ferrous sulfate. The main observations were:

1. Over the Pacific Ocean between the latitudes of 30–35° N, the observed NO _y mixing ratio between 3 and 8 km was a fairly constant 200 pptv. The NO mixing ratio increased with altitude from 15 pptv at 3 km to 35 pptv at 7 km.
2. Over the Sea of Japan, tropospheric NO _y mesured between 1 and 6 km started increasing with latitude North of 35° N and reached about 1000 pptv at 40° N.
3. NO _y was measured in an air mass transported from the stratosphere near a tropopause fold region. When the ozone mixing ratio was between 80 and 140 ppbv, the NO _y mixing ratio was about 200 pptv.

     

Stratosphere-troposphere exchange and its specific features at extratropical latitudes

A review of the papers dealing with various aspects of stratosphere-troposphere exchange (STE) is presented. The development of STE concepts is described and quantitative estimates of STE obtained by different authors are given. Typical time scales and geographic features of STE are described. Special attention is given to the specific features of STE at extratropical latitudes where active vertical air transport is observed in both directions. The air ascent through the tropopause occurs there in the zones of warm conveyor belts, and the air descent takes place in the zones of stratospheric intrusions. Exchange processes in the key region including the upper troposphere and the lowermost stratosphere are described. The mechanisms of large-scale stratospheric intrusions in the systems of tropopause folds or cut-off lows are presented as well as the mechanisms of the mixing of the stratospheric air with the tropospheric one. Specific features of deep stratospheric intrusions are discussed which are based on the analysis of such indicators of stratospheric air as high concentrations of ozone and stratospheric radionuclide 7Be. Some aspects of stratosphere-troposphere energy exchange are considered.     

Deuterium, Oxygen-18, and Tritium as Tracers for Water Vapour Transport in the Lower Stratosphere and Tropopause Region

Simultaneous measurements of the three rare isotopes Deuterium (D), Tritium (T), and Oxygen-18 (18O) in water vapour were made for the first time in the vicinity of the northern hemisphere tropopause. In contrast to expectation, high D/H and 18O/16O ratios, but relatively low T/H ratios, were found within the lowermost stratosphere. Since water vapour in the low-latitude upper troposphere shows a similar isotopic signature, we conclude that in the mid-latitudes considerable amounts of tropospheric water vapour are injected into the lowermost stratosphere, probably resulting in a hydration of the lower stratosphere. In addition, T can serve as tracer for precipitation of water containing stratospheric aerosol particles, because the T/H ratio in stratospheric water vapour is orders of magnitude higher than in the upper troposphere. Thus, even a small contribution of water of stratospheric origin should be detectable in the tropopause region. In our measurements performed in the Arctic we did not find isotopic evidence for sedimentation of PSC particles down to the tropopause. This may be caused by the low spatial and temporal coverage of our observations; however, it may also be due to the much weaker wintertime dehydration of the Arctic vortex compared to the Antarctic.     

Constraints on 2-Way Transport across the Arctic Tropopause Based on O3, Stratospheric Tracer (SF6) Ages, and Water Vapor Isotope (D, T) Tracers

Based upon airborne trace gas and isotope observations in the winter months 1991/1992 to1994/1995, transport pathways across the mid-latitude and Arctic tropopause areinvestigated. A powerful set of contrasting transport tracers are examined, such asdeuterated water vapor (HDO) which is shown to trace the passage of water vapor from thetroposphere into the lowermost stratosphere (LS), or the `SF₆ age' defined as theresidence time of an air parcel within the stratosphere since its entry at thetropopause. Cross-tropopause transport in both directions was found near mid-latitudecyclones (at baroclinic flanks of troughs in the polar front), in which about 80% of thestratosphere-to-troposphere flux proceeded along potential temperature ()surfaces of 300 ± 10 K. As these isentropes are the lowest which reach into the LS(in winter), a mixing zone just above the Arctic tropopause (at least 1.5 km thick) isformed. Here, upwelling tropospheric air is mixed with downwelling LS air which isaffected by air from higher altitudes, the surf-zone and the polar vortex. The observedelevated D/H isotope ratio of water vapor within the mixing zone can be explained byinjection of subtropical water vapor that is transported to the tropopause by the warmconveyor belt associated with mid-latitude cyclones. Downward vertical transport ofArctic LS air, which may be influenced by ouflowing chemically disturbed polar vortexair, into the Arctic troposphere was found to be small.     

Measurements of atmospheric dimethyl sulfide and carbon disulfide in the western Atlantic boundary layer

Shipboard measurements of atmospheric dimethyl sulfide were made during two transects along the east coast of the United States and at several stations in the Gulf of Maine. Limited measurements of carbon disulfide and hydrogen sulfide are also reported. The mean DMS mixing ratio was 29 pptv (=25, n=84, median 19 pptv) during the Atlantic transects, and 101 pptv (=67, n=77, median 79 pptv) in the Gulf of Maine. Distinct diurnal variations were found in the DMS data from the transects. The meteorology of the study area appears to control day-to-day differences in the magnitude of these diurnal variations, although rapid daytime oxidation is suggested in some cases. Diurnal variations were also evident in near-shore stations in the Gulf of Maine due to nocturnal boundary-layer inversion. Diurnal variation was not evident at other sites in the Gulf due to large scale changes in the atmospheric circulation pattern, which effectively masked any effects due to oxidation processes. Model simulations confirm that the DMS levels and diurnal variation found during the transects are not consistent with atmospheric oxidation processes alone. Atmospheric CS₂ and H₂S mixing ratios were less than 3 pptv during the transects, except for a single period of higher CS₂ mixing ratios (reaching 11 pptv) during advection of continental air. Calculations of the flux of oceanic sulfur to the eastern United States show that the contribution of natural sulfur to the North American sulfur budget is small compared to anthropogenic sources.     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.     

The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30° north latitude

The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS)-Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH₃Cl, ClONO₂, CCl₄, CCl₂F₂, CCl₃F, CHClF₂, CF₄, COF₂, and SF₆ near 30° north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH₃CCl₃ and C₂F₃Cl₃ below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30° N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58±0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15±0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.     

Chemistry–Climate Interactions of Stratospheric and Mesospheric Ozone in EMAC Long-Term Simulations with Different Boundary Conditions for CO2, CH4, N2O,and ODS

Abstract

To evaluate future climate change in the middle atmosphere and the chemistry–climate interaction of stratospheric ozone, we performed a long-term simulation from 1960 to 2050 with boundary conditions from the Intergovernmental Panel on Climate Change A1B greenhouse gas scenario and the World Meteorological Organization Ab halogen scenario using the chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). In addition to this standard simulation we performed five sensitivity simulations from 2000 to 2050 using the rerun files of the simulation mentioned above. For these sensitivity simulations we used the same model setup as in the standard simulation but changed the boundary conditions for carbon dioxide (CO₂), methane (CH₄), nitrous oxide (N₂O), and ozone-depleting substances (ODS). In the first sensitivity simulation we fixed the mixing ratios of CO₂, CH₄, and N₂O in the boundary conditions to the amounts for 2000. In each of the four other sensitivity simulations we fixed the boundary conditions of only one of CO₂, CH₄, N₂O, or ODS to the year 2000.

In our model simulations the future evolution of greenhouse gases leads to significant cooling in the stratosphere and mesosphere. Increasing CO₂ mixing ratios make the largest contributions to this radiative cooling, followed by increasing stratospheric CH₄, which also forms additional H₂O in the upper stratosphere and mesosphere. Increasing N₂O mixing ratios makes the smallest contributions to the cooling. The simulated ozone recovery leads to warming of the middle atmosphere.

In the EMAC model the future development of ozone is influenced by several factors. 1) Cooler temperatures lead to an increase in ozone in the upper stratosphere. The strongest contribution to this ozone production is cooling due to increasing CO₂ mixing ratios, followed by increasing CH₄. 2) Decreasing ODS mixing ratios lead to ozone recovery, but the contribution to the total ozone increase in the upper stratosphere is only slightly higher than the contribution of the cooling by greenhouse gases. In the polar lower stratosphere a decrease in ODS is mainly responsible for ozone recovery. 3) Higher NO_x and HO_x mixing ratios due to increased N₂O and CH₄ lead to intensified ozone destruction, primarily in the middle and upper stratosphere, from additional NO_x; in the mesosphere the intensified ozone destruction is caused by additional HO_x. In comparison to the increase in ozone due to decreasing ODS, ozone destruction caused by increased NO_x is of similar importance in some regions, especially in the middle stratosphere. 4) In the stratosphere the enhancement of the Brewer-Dobson circulation leads to a change in ozone transport. In the polar stratosphere increased downwelling leads to additional ozone in the future, especially at high northern latitudes. The dynamical impact on ozone development is higher at some altitudes in the polar stratosphere than the ozone increase due to cooler temperatures. In the tropical lower stratosphere increased residual vertical upward transport leads to a decrease in ozone.     

Short-Term Variability of Atmospheric DMS and Its Oxidation Products at Amsterdam Island during Summer Time

A one-month experiment was performed at Amsterdam Island in January 1998, to investigate the factors controlling the short-term variations of atmospheric dimethylsulfide (DMS) and its oxidation products in the mid-latitudes remote marine atmosphere. High mixing ratios of DMS, sulfur dioxide (SO₂) and dimethylsulfoxide (DMSO) have been observed during this experiment, with mean concentrations of 395 parts per trillion by volume (pptv) (standard deviation, = 285, n = 500), 114 pptv ( = 125, n = 12) and 3 pptv ( = 1.2, n = 167), respectively. Wind speed and direction were identified as the major factors controlling atmospheric DMS levels. Changes in air temperature/air masses origin were found to strongly influence the dimethylsulfoxide (DMSO)/DMS and SO₂/DMS molar ratios, in line with recent laboratory data. Methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO₄ ^2–) mean concentrations in aerosols during this experiment were 12.2± 6.5 pptv (1, n=47) and 59 ± 33 pptv (1, n=47), respectively. Evidence of vertical entrainment was reported following frontal passages, with injection of moisture-poor, ozone-rich air. High MSA/ nss-SO₄ ^2– molar ratios (mean 0.44) were calculated during these events. Finally following frontal passages, few spots in condensation nuclei (CN) concentration were also observed.     

In Situ Trace Gas and Particle Measurements in the Summer Lower Stratosphere during STREAM II: Implications for O3 Production

In situ aircraft measurements of O₃, CO,HNO₃, and aerosol particles are presented,performed over the North Sea region in the summerlower stratosphere during the STREAM II campaign(Stratosphere Troposphere Experiments by AircraftMeasurements) in July 1994. Occasionally, high COconcentrations of 200-300 pbbv were measured in thelowermost stratosphere, together with relatively highHNO₃ concentrations up to 1.6 ppbv. The particlenumber concentration (at standard pressure andtemperature) between 0.018-1 m decreased acrossthe tropopause, from >1000 cm^-3 in the uppertroposphere to <500 cm^-3 in the lowermoststratosphere. Since the CO sources are found in thetroposphere, the elevated CO mixing ratios areattributed to mixing of polluted tropospheric air intothe lowermost extratropical stratosphere. Further wehave used a chemical model to illustrate that nitrogenoxide reservoir species (mainly HNO₃) determinethe availability of NO_x (=NO + NO₂) andtherefore largely control the total net O₃production in the lower kilometers of thestratosphere. Model simulations, applying additionalNO_x perturbations from aircraft, show that theO₃ production efficiency of NO_x is smallerthan previously assumed, under conditions withrelatively high HNO₃ mixing ratios, as observedduring STREAM II. The model simulations furthersuggest a relatively high O₃ productionefficiency from CO oxidation, as a result of therelatively high ambient HNO₃ and NO_xconcentrations, implying that upward transport of COrich air enhances O₃ production in the lowermoststratosphere. Analysis of the measurements and themodel calculations suggest that the lowermoststratosphere is a transition region in which thechemistry deviates from both the upper troposphere andlower stratosphere.     

北半球两大地形下游冬季环流的动力分析——Ⅱ.行星波的垂直传播

线性、定常、多层半球谱模式模拟结果表明,在东亚纬向气流下,青藏高原能在平流层激发出强大的1波扰动,脊槽分别位于太平洋和大西洋上空。在北美纬向气流下,落基山在平流层激发的1波很弱。观测资料计算指出,对流层行星1波很难通过北美对流层顶上传,但却能自由穿过东亚高纬度地区的对流层顶向平流层传播。北美地形所激发的波动在上传过程中均折向低纬传播。青藏高原所激发的行星1波和2波在上传过程中有分支:折向低纬的一支主要局限在对流层中;折向高纬的一支进入平流层。模拟和分析证明,这些差异是北半球两大地形不同的动力作用的结果。     

Surface NO and NO2 mixing ratios measured between 30° N and 30° S in the Atlantic region

Surface NO and NO₂ mixing ratios were measured aboard the research vessel Polarstern during the mission ANT VII/1 from 24 September to 5 October 1988. The measurements were taken along the meridian at 30° W in the Atlantic region covering latitudes between 30° N and 30° S. The average mixing ratios were about 12 pptv NO/30 pptv NO₂ in the Northern Hemisphere and about 7 pptv NO/22 pptv NO₂ in the Southern. Elevated mixing ratios of 20 pptv NO/70 pptv NO₂ were found at 12° N (probably due to air masses originating from the surface of West Africa) and in the region of the ITCZ between 8° N and 5° N. Because of probable contamination by the ship, the measured mixing ratios mostly represent upper limits.     

ANALYSES OF THE DYNAMIC EFFECTS ON WINTER CIRCULATION OF THE TWO MAIN MOUNTAINS IN THE NORTHERN HEMISPHERE——Ⅱ.VERTICAL PROPAGATION OF PLANETARY WAVES

A linear,hemispheric and stationary spectral model with multilayers in the vertical was employed to simulate thevertical propagation of waves triggered by mountains.Results show that,in cooperation with the East Asia zonal meanflow,Tibetan Plateau can excite a strong wavenumber 1 perturbation in the stratosphere with its ridge and trough lo-cated over the Pacific and Atlantic Oceans respectively.On the other hand,the stratospheric wavenumber 1 perturbationcaused by the mechanical forcing of the Rocky Mountains in cooperation with the North America zonal mean flow isvery weak.Calculations from observational data of the vertical profile of critical wavenumber for vertically propagatingwaves imply that the tropospheric wavenumber 1 perturbation can hardly penetrate the North America tropopause up-wards,whereas it can freely propagate through the East Asia tropopause into the stratosphere.Two-dimensional E-Pcross-sections obtained from both observational data and simulated results also demonstrate that waves excited by theRocky Mountains are refracted towards low latitudes in the troposphere during their upward propagation:whereas,inaddition to the above mentioned equatorward leaning branch,the wavenumber 1 and 2 planetary waves excited by theTibetan Plateau possess another branch which is refracted to high latitudes during upward propagation and penetratesthe tropopause into the stratosphere.It is therefore concluded that the difference in the horizontal and vertical wavepropagations in the two hemispheres is a result of the different dynamical forcing induced by the two main mountains inthe Northern Hemisphere.     

Is there a stratospheric radiative feedback in global warming simulations?

The radiative impacts of the stratosphere in global warming simulations are investigated using abrupt CO₂ quadrupling experiments of the Coupled Model Inter-comparison Project phase 5 (CMIP5), with a focus on stratospheric temperature and water vapor. It is found that the stratospheric temperature change has a robust bullhorn-like zonal-mean pattern due to a strengthening of the stratospheric overturning circulation. This temperature change modifies the zonal mean top-of-the-atmosphere energy balance, but the compensation of the regional effects leads to an insignificant global-mean radiative feedback (?0.02 ± 0.04 W m^?2 K^?1). The stratospheric water vapor concentration generally increases, which leads to a weak positive global-mean radiative feedback (0.02 ± 0.01 W m^?2 K^?1). The stratospheric moistening is related to mixing of elevated upper-tropospheric humidity, and, to a lesser extent, to change in tropical tropopause temperature. Our results indicate that the strength of the stratospheric water vapor feedback is noticeably larger in high-top models than in low-top ones. The results here indicate that although its radiative impact as a forcing adjustment is significant, the stratosphere makes a minor contribution to the overall climate feedback in CMIP5 models.     

On the Temporal and Spatial Structure of Troposphere-to- Stratosphere Transport in the Lowermost Stratosphere over the Asian Monsoon Region during Boreal Summer

This study produced a novel characterization of the troposphere-to-stratosphere transport(TST) over the Asian monsoon region during boreal summer,using a comprehensive analysis of 60-day backward trajectories initialized in the stratosphere.The trajectory datasets were derived from the high-resolution Lagrangian particle dispersion model(FLEXPART) simulation driven by the wind fields acquired from the National Center for Environmental Prediction(NCEP).The results indicate that the distribution of residence time(tTST) of tropopause-crossing trajectories in the lowermost stratosphere represents a horizontal signature of the Asian summer monsoon.Vertically,the distribution of tTST can be roughly separated into two layers:a consistent lower layer with tTST <5 days forming a narrow band,corresponding to a layer～3 km thick following the location of the tropopause,and an upper layer at a larger distance from the local tropopause.The maximum residence time was～20 days,especially within the Asian high anticyclone consistent with its confinement effects.In general,the overall geographical distribution of dehydration points was not coincident with the location of tropopause crossing.TST trajectories,which were initialized in the stratosphere,underwent their Lagrangian cold points mostly in the tropics and subtropics 1-4 days after the TST event;they were characterized by a wide range of temperature differences,with a mean value of 3-12 K.The vertical extent of the influence of tropospheric intrusion on the Asian monsoon region in the stratosphere exhibited a peak at～16.5-18.5 km,and the uppermost height was～21 km.     

ANALYSES OF THE DYNAMIC EFFECTS ON WINTER CIRCULATION OF THE TWO MAIN MOUNTAINS IN THE NORTHERN HEMISPHERE--Ⅱ.VERTICAL PROPAGATION OF PLANETARY WAVES

A linear,hemispheric and stationary spectral model with multilayers in the vertical was employed to simulate the vertical propagation of waves triggered by mountains.Results show that,in cooperation with the East Asia zonal mean flow,Tibetan Plateau can excite a strong wavenumber 1 perturbation in the stratosphere with its ridge and trough located over the Pacific and Atlantic Oceans respectively.On the other hand,the stratospheric wavenumber 1 perturbation caused by the mechanical forcing of the Rocky Mountains in cooperation with the North America zonal mean flow is very weak.Calculations from observational data of the vertical profile of critical wavenumber for vertically propagating waves imply that the tropospheric wavenumber 1 perturbation can hardly penetrate the North America tropopause upwards,whereas it can freely propagate through the East Asia tropopause into the stratosphere.Two-dimensional E-Pcross-sections obtained from both observational data and simulated results also demonstrate that waves excited by the Rocky Mountains are refracted towards low latitudes in the troposphere during their upward propagation:whereas,in addition to the above mentioned equatorward leaning branch,the wavenumber 1 and 2 planetary waves excited by the Tibetan Plateau possess another branch which is refracted to high latitudes during upward propagation and penetrates the tropopause into the stratosphere.It is therefore concluded that the difference in the horizontal and vertical wave propagations in the two hemispheres is a result of the different dynamical forcing induced by the two main mountains in the Northern Hemisphere.     

Aircraft measurements and model simulations of stratospheric ozone and N2O: implications for chemistry and transport processes in the models

Airborne measurements of stratospheric ozone and N₂O from the SCIAMACHY (Scanning Imaging Absorption Spectrometer) Validation and Utilization Experiment (SCIA-VALUE) are presented. The campaign was conducted in September 2002 and February–March 2003. The Airborne Submillimeter Radiometer (ASUR) observed stratospheric constituents like O₃ and N₂O, among others, spanning a latitude from 5°S to 80°N during the survey. The tropical ozone source regions show high ozone volume mixing ratios (VMRs) of around 11 ppmv at 33 km altitude, and the altitude of the maximum VMR increases from the tropics to the Arctic. The N₂O VMRs show the largest value of 325 ppbv in the lower stratosphere, indicating their tropospheric origin, and they decrease with increasing altitude and latitude due to photolysis. The sub-tropical and polar mixing barriers are well represented in the N₂O measurements. The most striking seasonal difference found in the measurements is the large polar descent in February–March. The observed features are interpreted with the help of SLIMCAT and Bremen Chemical Transport Model (CTMB) simulations. The SLIMCAT simulations are in good agreement with the measured O₃ and N₂O values, where the differences are within 1 ppmv for O₃ and 15 ppbv for N₂O. However, the CTMB simulations underestimate the tropical middle stratospheric O₃ (1–1.5 ppmv) and the tropical lower stratospheric N₂O (15–30 ppbv) measurements. A detailed analysis with various measurements and model simulations suggests that the biases in the CTMB simulations are related to its parameterised chemistry schemes.     

On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

We present a theory for the formation of frozen aerosol particles in the Antarctic stratosphere, the coldest region of the Earth's stratosphere. The theory is applied specifically to the formation of polar stratospheric clouds. We suggest that the condensed ices are composed primarily of nitric acid and water with small admixtures of other compounds such as H₂SO₄ and HCl in solid solution. Our assumed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinctions observed in the winter polar stratosphere. Physical chemistry and thermodynamic considerations suggest that at temperatures between about 200 and 185 K, stratospheric particulates are composed primarily of frozen nitric acid solutions with a composition near that of the trihydrate. Available data suggest the particles are amorphous solid solutions and not in the crystalline hydrate form. At lower temperatures (i.e., below the forst point of pure water) cirrus-like ice clouds can form.     

Further evidences of deep convective vertical transport of water vapor through the tropopause

A few years ago, we identified a deep convective transport mechanism, of water vapor through the tropopause, namely, storm top gravity wave breaking, such that tropospheric water substance can be injected into the lower stratosphere via this pathway. The main evidence presented previously was taken from the lower resolution AVHRR images of the storm anvil top cirrus plumes obtained by polar orbiting satellites. Recent observations have provided further supporting evidence for this important cross-tropopause transport mechanism. There are now many higher resolution satellite images, mainly from MODIS instrument, that show more definitely the existence of these plumes, many of which would probably be unseen by lower resolution images.Furthermore, a thunderstorm movie taken in Denver (USA) area during STEPS2000 field campaign and another thunderstorm movie taken by a building top webcam in Zurich also demonstrate that the jumping cirrus phenomenon, first identified by T. Fujita in 1980s, may be quite common in active thunderstorm cells, quite contrary to previous belief that it is rare. We have used a cloud model to demonstrate that the jumping cirrus is exactly the gravity wave breaking phenomenon that transports water vapor through the tropopause.These additional evidences provide increasing support that deep convection contributes substantially to the troposphere-to-stratosphere transport of water substance. This corroborates well with recent studies of the stratospheric HDO/H₂O ratio which is much highly than it would be if the transport is via slow ascent. The only explanation that can be used to interpret this observation at present is that water substance is transported through the tropopause via rapid vertical motion, i.e., deep convection.