Subsonic aircraft and ozone trends

Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO _x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO _x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO _x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.     

The effect of ozone photochemistry on atmospheric and surface temperature changes due to increased CO2, N2O,CH4 and volcanic aerosols in the atmosphere

Abstract

A coupled 1‐D radiative‐convective and photochemical diffusion model is used to study the influence of ozone photochemistry on changes in the vertical temperature structure and surface climate resulting from the doubling of atmospheric CO₂, N₂O, CH₄ and increased stratospheric aerosols owing to the El Chichón volcanic eruption. It is found when CO₂ alone is doubled, that the total ozone column increases by nearly 6% and the resulting increase in the solar heating contributes a smaller temperature decrease in the stratosphere (up to 4 K near the stratopause level). When the concentration of CO₂, N₂O and CH₄ are simultaneously doubled, the total ozone column amount increases by only 2.5% resulting in a reduced temperature recovery in the stratosphere. Additional results concerning the effect of the interaction of ozone photochemistry with the stratospheric aerosol cloud produced by the El Chichón eruption show that it leads to a reduction in stratospheric ozone, which in turn has the effect of increasing the cooling at the surface and above the cloud centre while causing a slight warming below in the lower stratosphere.     

Climatic changes associated with a global “2°C-stabilization” scenario simulated by the ECHAM5/MPI-OM coupled climate model

In this study, concentrations of the well-mixed greenhouse gases as well as the anthropogenic sulphate aerosol load and stratospheric ozone concentrations are prescribed to the ECHAM5/MPI-OM coupled climate model so that the simulated global warming does not exceed 2°C relative to pre-industrial times. The climatic changes associated with this so-called “2°C-stabilization” scenario are assessed in further detail, considering a variety of meteorological and oceanic variables. The climatic changes associated with such a relatively weak climate forcing supplement the recently published fourth assessment report by the IPCC in that such a stabilization scenario can only be achieved by mitigation initiatives. Also, the impact of the anthropogenic sulphate aerosol load and stratospheric ozone concentrations on the simulated climatic changes is investigated. For this particular climate model, the 2°C-stabilization scenario is characterized by the following atmospheric concentrations of the well-mixed greenhouse gases: 418 ppm (CO₂), 2,026 ppb (CH₄), and 331 ppb (N₂O), 786 ppt (CFC-11) and 486 ppt (CFC-12), respectively. These greenhouse gas concentrations correspond to those for 2020 according to the SRES A1B scenario. At the same time, the anthropogenic sulphate aerosol load and stratospheric ozone concentrations are changed to the level in 2100 (again, according to the SRES A1B scenario), with a global anthropogenic sulphur dioxide emission of 28 TgS/year leading to a global anthropogenic sulphate aerosol load of 0.23 TgS. The future changes in climate associated with the 2°C-stabilization scenario show many of the typical features of other climate change scenarios, including those associated with stronger climatic forcings. That are a pronounced warming, particularly at high latitudes accompanied by a marked reduction of the sea-ice cover, a substantial increase in precipitation in the tropics as well as at mid- and high latitudes in both hemispheres but a marked reduction in the subtropics, a significant strengthening of the meridional temperature gradient between the tropical upper troposphere and the lower stratosphere in the extratropics accompanied by a pronounced intensification of the westerly winds in the lower stratosphere, and a strengthening of the westerly winds in the Southern Hemisphere extratropics throughout the troposphere. The magnitudes of these changes, however, are somewhat weaker than for the scenarios associated with stronger global warming due to stronger climatic forcings, such as the SRES A1B scenario. Some of the climatic changes associated with the 2°C-stabilization are relatively strong with respect to the magnitude of the simulated global warming, i.e., the pronounced warming and sea-ice reduction in the Arctic region, the strengthening of the meridional temperature gradient at the northern high latitudes and the general increase in precipitation. Other climatic changes, i.e., the El Niño like warming pattern in the tropical Pacific Ocean and the corresponding changes in the distribution of precipitation in the tropics and in the Southern Oscillation, are not as markedly pronounced as for the scenarios with a stronger global warming. A higher anthropogenic sulphate aerosol load (for 2030 as compared to the level in 2100 according to the SRES A1B scenario) generally weakens the future changes in climate, particularly for precipitation. The most pronounced effects occur in the Northern Hemisphere and in the tropics, where also the main sources of anthropogenic sulphate aerosols are located.     

The Effect of Super Volcanic Eruptions on Ozone Depletion in a Chemistry–Climate Model

With the gradual yet unequivocal phasing out of ozone depleting substances(ODSs), the environmental crisis caused by the discovery of an ozone hole over the Antarctic has lessened in severity and a promising recovery of the ozone layer is predicted in this century. However, strong volcanic activity can also cause ozone depletion that might be severe enough to threaten the existence of life on Earth. In this study, a transport model and a coupled chemistry–climate model were used to simulate the impacts of super volcanoes on ozone depletion. The volcanic eruptions in the experiments were the 1991 Mount Pinatubo eruption and a 100 × Pinatubo size eruption. The results show that the percentage of global mean total column ozone depletion in the 2050 RCP8.5 100 × Pinatubo scenario is approximately 6% compared to two years before the eruption and 6.4% in tropics. An identical simulation, 100 × Pinatubo eruption only with natural source ODSs, produces an ozone depletion of 2.5% compared to two years before the eruption, and with 4.4% loss in the tropics. Based on the model results,the reduced ODSs and stratospheric cooling lighten the ozone depletion after super volcanic eruption.     

Aerosol and ozone changes as forcing for climate evolution between 1850 and 2100

Global aerosol and ozone distributions and their associated radiative forcings were simulated between 1850 and 2100 following a recent historical emission dataset and under the representative concentration pathways (RCP) for the future. These simulations were used in an Earth System Model to account for the changes in both radiatively and chemically active compounds, when simulating the climate evolution. The past negative stratospheric ozone trends result in a negative climate forcing culminating at ?0.15 W m^?2 in the 1990s. In the meantime, the tropospheric ozone burden increase generates a positive climate forcing peaking at 0.41 W m^?2. The future evolution of ozone strongly depends on the RCP scenario considered. In RCP4.5 and RCP6.0, the evolution of both stratospheric and tropospheric ozone generate relatively weak radiative forcing changes until 2060–2070 followed by a relative 30 % decrease in radiative forcing by 2100. In contrast, RCP8.5 and RCP2.6 model projections exhibit strongly different ozone radiative forcing trajectories. In the RCP2.6 scenario, both effects (stratospheric ozone, a negative forcing, and tropospheric ozone, a positive forcing) decline towards 1950s values while they both get stronger in the RCP8.5 scenario. Over the twentieth century, the evolution of the total aerosol burden is characterized by a strong increase after World War II until the middle of the 1980s followed by a stabilization during the last decade due to the strong decrease in sulfates in OECD countries since the 1970s. The cooling effects reach their maximal values in 1980, with ?0.34 and ?0.28 W m^?2 respectively for direct and indirect total radiative forcings. According to the RCP scenarios, the aerosol content, after peaking around 2010, is projected to decline strongly and monotonically during the twenty-first century for the RCP8.5, 4.5 and 2.6 scenarios. While for RCP6.0 the decline occurs later, after peaking around 2050. As a consequence the relative importance of the total cooling effect of aerosols becomes weaker throughout the twenty-first century compared with the positive forcing of greenhouse gases. Nevertheless, both surface ozone and aerosol content show very different regional features depending on the future scenario considered. Hence, in 2050, surface ozone changes vary between ?12 and +12 ppbv over Asia depending on the RCP projection, whereas the regional direct aerosol radiative forcing can locally exceed ?3 W m^?2.     

Stratospheric aerosol measurements in the Arctic winter of 1996/1997 with the M‐55 Geophysika high‐altitude research aircraft

In‐situ aerosol measurements were performed in the northern hemispheric stratosphere up to altitudes of 21 km between 13 November 1996 and 14 January 1997, inside and outside of the polar vortex during the Airborne Polar Experiment (APE) field campaign. These are measurements of particle size distributions with a laser optical particle counter of the FSSP‐300 type operated during 9 flights on the Russian M‐55 high‐altitude research aircraft Geophysika. For specific flights, the FSSP‐300 measurements are compared with balloon‐borne data (launched from Kiruna, Sweden). It was found that the stratospheric aerosol content reached levels well below the background concentrations measured by the NASA operated ER‐2 in 1988/89 in the northern hemisphere. During the APE campaign, no PSC particle formation was observed at flight altitudes although the temperatures were below the NAT condensation point during one flight. The measured correlations between ozone and aerosol give an indication of the subsidence inside the 1996/97 polar vortex. Despite the lower aerosol content in the winter 1996/97 compared to the 1989 background, the heterogeneous reactivity of the aerosol (as calculated from the measured data with additional model input) is comparable. This is due to the dependency of the reactive uptake coefficients on the atmospheric water vapor content. Under the described assumptions the reaction rates on the background aerosol are significantly smaller than for competing gas phase chlorine activation, as can be expected for stratospheric background conditions especially inside the polar vortex.     

Carbonyl Sulphide (OCS) Variability with Latitude in the Atmosphere

Abstract

Carbonyl sulphide (OCS) is an important precursor of sulphate aerosols and consequently a key species in stratospheric ozone depletion. The SPectromètre InfraRouge d'Absorption à Lasers Embarqués (SPIRALE) and shortwave infrared (SWIR) balloon-borne instruments have flown in the tropics and in the polar Arctic, and ground-based measurements have been performed by the Qualité de l'Air (QualAir) Fourier Transform Spectrometer in Paris. Partial and total columns and vertical profiles have been obtained to study OCS variability with altitude, latitude, and season. The annual total column variation in Paris reveals a seasonal variation with a maximum in April–June and a minimum in November–January. Total column measurements above Paris and from SWIR balloon-borne instrument are compared with several MkIV measurements, several Network for the Detection of Atmospheric Composition Change (NDACC) stations, aircraft, ship, and balloon measurements to highlight the OCS total column decrease from tropical to polar latitudes. OCS high-resolution in situ vertical profiles have been measured for the first time in the altitude range between 14 and 30?km at tropical and polar latitudes. OCS profiles are compared with Atmospheric Chemistry Experiment (ACE) satellite measurements and show good agreement. Using the correlation between OCS and N₂O from SPIRALE, the OCS stratospheric lifetime has been accurately determined. We find a stratospheric lifetime of 68?±?20 years at polar latitudes and 58?±?14 years at tropical latitudes leading to a global stratospheric sink of 49?±?14?Gg?S?y^?1.     

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.     

MANTRA ‐ A Balloon Mission to Study the Odd‐Nitrogen Budget of the Stratosphere

Abstract

The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) series of high‐altitude balloon flights is being undertaken to investigate changes in the concentrations of northern hemisphere mid‐latitude stratospheric ozone, and of nitrogen and chlorine compounds that play a role in ozone chemistry. Four campaigns have been carried out to date, all from Vanscoy, Saskatchewan, Canada (52°01'N, 107°02'W, 511.0 m). The first MANTRA mission took place in August 1998, with the balloon flight on 24 August 1998 being the first Canadian launch of a large high‐altitude balloon in about fifteen years. The balloon carried a payload of instruments to measure atmospheric composition, and made measurements from a float altitude of 32–38 km for one day. Three of these instruments had been flown on the Stratoprobe flights of the Atmospheric Environment Service (now the Meteorological Service of Canada) in the 1970s and early 1980s, providing a link to historical data predating the onset of mid‐latitude ozone loss.

The primary measurements obtained from the balloon‐borne instruments were vertical profiles of ozone, NO₂, HNO₃, HCl, CFC‐11, CFC‐12, N₂O, CH₄, temperature, and aerosol backscatter. Total column measurements of ozone, NO₂, SO₂, and aerosol optical depth were made by three ground‐based spectrometers deployed during the campaign. Regular ozonesonde and radiosonde launches were also conducted during the two weeks prior to the main launch in order to characterize the local atmospheric conditions (winds, pressure, temperature, humidity) in the vicinity of the primary balloon flight. The data have been compared with the Model for Evaluating oZONe Trends (MEZON) chemical transport model, the University of California at Irvine photochemical box model, and the Canadian Middle Atmosphere Model (CMAM) to test our current understanding of model photochemistry and mid‐latitude species correlations. This paper provides an overview of the MANTRA 1998 mission, and serves as an introduction to the accompanying papers in this issue of Atmosphere‐Ocean that describe specific aspects and results of this campaign.     

Geoengineering climate by stratospheric sulfur injections: Earth system vulnerability to technological failure

We use a coupled climate–carbon cycle model of intermediate complexity to investigate scenarios of stratospheric sulfur injections as a measure to compensate for CO₂-induced global warming. The baseline scenario includes the burning of 5,000 GtC of fossil fuels. A full compensation of CO₂-induced warming requires a load of about 13 MtS in the stratosphere at the peak of atmospheric CO₂ concentration. Keeping global warming below 2°C reduces this load to 9 MtS. Compensation of CO₂ forcing by stratospheric aerosols leads to a global reduction in precipitation, warmer winters in the high northern latitudes and cooler summers over northern hemisphere landmasses. The average surface ocean pH decreases by 0.7, reducing the calcifying ability of marine organisms. Because of the millennial persistence of the fossil fuel CO₂ in the atmosphere, high levels of stratospheric aerosol loading would have to continue for thousands of years until CO₂ was removed from the atmosphere. A termination of stratospheric aerosol loading results in abrupt global warming of up to 5°C within several decades, a vulnerability of the Earth system to technological failure.     

Modeling the sudden decrease in CH4 growth rate in 1992

A two-dimensional global chemistry model is developed to study the distribution and long-term trends of methane. The model contains 34 species and 104 chemical and photochemical reactions. Using the model, the long-term trends of CH₄, CO and OH in atmosphere are simulated, comparison between the model and observations shows that the simulation is successful. Experiments are done to investigate the causes of dramatic decrease in the growth rate of CH₄ in 1992 such as OH increase due to stratospheric ozone depletion, decrease of temperature in the troposphere due to Mount Pinatubo eruption and descendent of CH₄ sources fluxes. A new explanation is proposed and verified by this model that the decrease of CO emission plays an important role for the abnormal growth rate of CH₄ in 1992. We find that the decreases of CH₄ and CO emissions are the main reasons for the sudden decrease of growth rate of CH₄ in 1992, which account for 73% and 27% respectively.     

Heterogeneous Chemistry and the O3 Budget in the Lower Mid-Latitude Stratosphere

A photochemical box model including a detailed heterogeneous chemistrymodule has been used to analyze in detail the effects of temperature andaerosol surface area on odd oxygen production/depletion in the lowerstratosphere at 30° S. Results show that for background aerosolloading, the hydrolysis of BrONO₂ and N₂O₅are most important atall temperatures studied except when the temperature falls below about205 K, when ClONO₂ hydrolysis becomes most important. Thisprocessing leads to removal of active nitrogen to form nitric acid andenhancement of HO_x, BrO_x, ClO_x levels. Detailed O₃ budgets asa function of temperature are presented showing how ozone loss andproduction terms vary with changes in stratospheric sulfate aerosol loadingfor the individual families. For (most) aerosol loading levels, thelargest ozone losses occurred at warmer temperatures due to the strongtemperature dependence of the NO_x ozone-destroying reactions. Theexception to this occurred for the conditions representative of volcanicloading, which showed a strong increase in ozone destruction due toincreases in destruction from the ClO_x and HO_x families.The ozoneproduction term k[NO][HO₂] did not show a strong dependence oneithertemperature or aerosol loading, due to the offsetting effect of reducedNO_xand increased HO_x concentrations.     

平流层臭氧非线性响应的机理研究

完善了王革丽和杨培才(2007)建立的平流层下部臭氧异相光化学反应箱式模式,在原有模式基础上加入溴族,研究了平流层下部臭氧对硫酸气溶胶表面积浓度与氯化物、溴化物以及氮氧化物的排放强度变化的非线性响应,理解平流层臭氧对人类活动的依赖性.结果表明,当氯化物排放强度偏离当前水平时,气溶胶可以通过与溴化物、氯化物、氮氧化物之间的相互作用,干预光化系统的非线性行为,改变系统在参数空间中的拓扑结构.     

Tropospheric ozone and oxides of nitrogen over the north-western Pacific in summer

In summer, atmospheric ozone was measured from an aircraft platform simultaneously with nitric oxide (NO), oxides of nitrogen (NO _y ), and water vapor over the Pacific Ocean in east Asia from 34° N to 19° N along the longitude of 138±3°E. NO _y was measured with the aid of a ferrous sulfate converter. The altitude covered was from 0.5 to 5 km. A good correlation in the smoothed meridional distributions between ozone and NO _y was seen. In particular, north of 25° N, ozone and NO _y mixing ratios were considerably higher than those observed in tropical marine air south of 25° N. NO _y and O₃ reached a minimum of 50 pptv and 4 ppbv respectively in the boundary layer at a latitude of 20° N. The NO concentration between 2 and 5 km at the same latitude was 30 pptv. The profiles of ozone and water vapor mixing ratios were highly anti-correlated between 25° N and 20° N. In contrast, it was much poorer at the latitude of 33° N, suggesting a net photochemical production of ozone there.     

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.     

The vertical sulfur dioxide distribution at the tropopause level

In 1978–1980 nine aircraft flights to an altitude of up to 15 km were made over western Europe. Sulfur dioxide was measured with a sensitive chemiluminescence method consisting of separate sampling and analysis stages and application of a wet chemical filter procedure (detection limit: 8 pptv SO₂).The measurements performed in the upper troposphere and lower stratosphere lead to some unexpected results: (a) the meteorological conditions at the tropopause level have an important influence on the observed SO₂ mixing ratio; (b) between the 500 mb and the actual tropopause level the SO₂ mixing ratio is found to be <100 pptv, and weak vertical gradients of SO₂ suggest only a small flux of tropospheric SO₂ into the stratosphere; (c) increasing SO₂ mixing ratios within the first kilometers of the stratosphere give strong support to a stratospheric source of SO₂.In the light of improved one-dimensional models considering the vertical distribution of stratospheric sulfur compounds (Crutzen, 1981; Turco et al. 1981) it can be shown that the oxidation of organic sulfur compounds (e.g., OCS, CS₂) seems to be a stratospheric source of SO₂. Furthermore, the flux calculations based on the SO₂ mixing ratios measured at the tropopause level indicate that the contribution of tropospheric (man-made) SO₂ to the stratospheric aerosol layer is of only minor importance.     

A reassessment of stratospheric ozone: Credibility of the threat

A recent review of ozone observations and model predictions designed to determine the credibility of current stratospheric models, arrived at the following conclusions. Aside from prompt variations at altitudes above 30 km, observed variations in stratospheric ozone cannot be explained by the process of catalytic destruction; i.e. past variations in the ozone layer have been controlled by processes not included in current models. Past episodic stratospheric injections of oxides of nitrogen and chlorine have not induced changes in total ozone identifiable in the observational data. Species concentrations from different models differ greatly; by up to two orders of magnitude in some features. Even models with highly unlikely chemical reaction rates compute species concentration profiles currently considered to be in reasonable agreement with available observations. Observations of stratospheric species, particularly nitrous oxide and nitric acid, suggest that the natural stratospheric source of odd nitrogen has been underestimated by most models by 2- to 5-fold. These apparent disparities between observations and theory suggest flaws or omissions in our understanding of stratospheric ozone and a need for caution in accepting the predictions of current stratospheric models.A slightly amended but unupdated version of an invited paper presented at the Environmental Health Sciences Symposium: SST Pollution and Skin Cancer at the 50th Anniversary Congress of the Pan American Medical Association, Hollywood, Florida, October 25–29, 1976. Editor's Note: This paper, while containing an unsual number of personal opinions - which are, commendably, stated as such - does focus on an important controversy. Thus, it is published in the interest of stimulating further debate on the subject.     

Concentration of trace gases in the lower troposphere,simultaneously recorded at neighboring mountain stations Part II: Ozone

Summary Long-term ozone recordings at different altitude levels, conducted in remote areas, can make a valuable contribution to an understanding of the background level of ozone, its periodical variations and possible long-term trends.The measuring stations (three high mountain stations between 740 and nearly 3000 m a.s.l. with small horizontal distance) are described together with recording and calibration procedures. Information is provided on the time history of all recordings since 1978, considering not only the annual means but also the monthly and 10-day means as a function of height. An analysis is presented of the annual variations which differ considerably in the respective height levels and—in three-dimensional diagrams—the correlation between daily and annual variation is shown as a function of height. Then follows a careful parameterization: analysis of the frequency distribution of the ozone concentration, correlation with relative humidity, relative sunshine duration, and temperature. It can be seen that the correlations are very different and partly inverse, depending on the altitude level.Many ozone profiles obtained between valley level and nearly 3000 m a.s.l. (cable car O₃ radiosonde) give a picture of the typical ozone profile for different meteorological situations and for the case of stratospheric intrusions of ozone into the troposphere. The stratospheric contribution of ozone to the tropospheric ozone budget is discussed.Since obviously a very high photochemical production rate can be established for ozone in the lowest layer above ground (correlation of O₃ with the daily variation of the sunshine duration) it was examined if this O₃ variation might be caused only by horizontal transport of ozone from remote areas with high anthropogenic activity by the daily quasiperiodical currents near the ground. But this is not the case.The correlation between ozone concentration, other trace gases such as nitrogen-oxygen compounds and hydrocarbons is shown.With 29 Figures     

华南地区春季平流层入侵对对流层低层臭氧影响的模拟研究

利用中尺度大气化学模式WRF/Chem对2013年3月6日华南地区一次平流层入侵事件及其对对流层低层臭氧的影响进行模拟研究。通过加入UBC（Upper Boundary Condition）上边界处理方案,弥补WRF/Chem模式未考虑平流层臭氧化学反应的不足。结合臭氧探空廓线资料、地面O₃、CO、NO_x、相对湿度、温度和风速等观测资料以及再分析资料对模拟结果进行定量评估,结果表明模式能较为真实地模拟本次平流层入侵过程。模拟分析进一步揭示:（1）副热带高空急流是本次平流层入侵的主要原因。当华南地区处在副热带急流入口区左侧下沉区域时,平流层入侵将富含臭氧的干燥空气输送到对流层中低层。（2）本次平流层入侵对对流层低层臭氧收支有重要影响,导致香港地区近地层臭氧体积混合比浓度明显上升,如塔门站夜间臭氧浓度升高21.3 ppb（1 ppb=1×10-9）。地面气象场和化学物种的分析进一步确认了平流层入侵的贡献。（3）采用动力学对流层顶高度时零维箱式模型和Wei公式计算得到的平流层入侵通量相当,分别为-1.42×10-3 kg m-2 s-1和-1.59×10-3 kg m-2 s-1,这一结果与前人研究相吻合,且与采用热力学对流层顶高度计算所得到的结果具有可比性。     

Radiative forcing from surface NO x emissions: spatial and seasonal variations

The global three-dimensional Lagrangian chemistry-transport model STOCHEM has been used to follow changes in the tropospheric distributions of methane CH₄ and ozone O₃ following the emission of pulses of the oxides of nitrogen NO _x . Month-long emission pulses of NO _x produce deficits in CH₄ mixing ratios that bring about negative radiative forcing (climate cooling) and decay away with e-folding times of 10–15 years. They also produce short-term excesses in O₃ mixing ratios that bring about positive radiative forcing (climate warming) that decay over several months to produce deficits, with their attendant negative radiative forcing (climate cooling) that decays away in step with the CH₄ deficits. Total time-integrated net radiative forcing is markedly influenced by cancellation between the negative CH₄ and long-term O₃ contributions and the positive short-term O₃ contribution to leave a small negative residual. Consequently, total net radiative forcing from NO _x emission pulses and the global warming potentials derived from them, show a strong dependence on the magnitudes, locations and seasons of the emissions. These dependences are illustrated using the Asian continent as an example and demonstrate that there is no simple robust relationship between continental-scale NO _x emissions and globally-integrated radiative forcing. We find that the magnitude of the time-integrated radiative forcing from NO _x -driven CH₄ depletion tends to approach and outweigh that from ozone enhancement, leaving net time-integrated radiative forcings and global warming potentials negative (climate cooling) in contrast to the situation for aircraft NO _x (climate warming). Control of man-made surface NO _x emissions alone may lead to positive radiative forcing (climate warming).