Stratospheric methane concentration profiles measured during the Balloon Intercomparison Campaigns

Following the Balloon Intercomparison Campaigns carried out from the NSBF, Palestine, Texas, in the fall of 1982 (BIC1) and spring of 1983 (BIC2), three instruments have reported infrared measurements (one in emission and two in absorption) from which results on the concentration of methane between 20 and 40 km altitude have been deduced. While the absorption-retrieved concentration profiles are in excellent agreement, the results from the emission measurements are significantly lower. Recent methane profiles obtained by satellite and from Spacelab 1 are in satisfactory agreement with the absorption data reported here.     

Intercomparison of remote measurements of stratospheric NO and NO2

During the 1982 and 1983 Balloon Intercomparison Campaigns, the vertical profile of stratospheric NO₂ was measured remotely by nine instruments and that of NO by two. Total overhead columns were measured by two more instruments. Between 30 and 35km, where measurements overlapped, agreement between NO profiles was within ±30%, which is better than the accuracies claimed by the experimenters. Between 35 and 40km there was similarly good agreement between NO₂ profiles, but below 30km, differences of greater than a factor three were found. In the second Campaign, NO₂ values from most instruments agreed within their quoted errors, except that the Oxford radiometer gave much lower values; but the first Campaign and the column measurements show a more uniform spread of results.These differences below 30km could not be resolved, but new laboratory measurements are planned which should do so.     

Ozone measurements from the Balloon Intercomparison Campaign

Measurements of the Balloon Intercomparison Campaign (BIC), conducted during fall, 1982 (BIC-1) and summer, 1983 (BIC-2), are reported. Results of five remote and two in situ techniques agree (with a few exceptions) within 95% confidence level uncertainties and generally within 15% above 20 km. Weighted mean profiles, which best represent conditions during the capaign, are used as a comparison standard. Accuracies of experiments indicated by BIC generally confirm estimated uncertainites for ECC sondes, UV photometry, and microwave emission experiments, are somewhat better for far IR emission and IR absorption experiments, and are somewhat worse for IR emission and solar UV absorption experiments. The large collection of BIC measurements confirms a problem reported earlier with current theoretical modeling of ozone near 40 km where transport is negligible and the chemistry is believed to be simpler.     

Monitoring of the integrated column of hydrogen fluoride above the Jungfraujoch Station since 1977 — the HF/HCl column ratio

The amount of hydrogen fluoride (HF) above the International Scientific Station of the Jungfraujoch (Switzerland) has been monitored during the last 8 years. The results deduced spectro-scopically from solar IR absorption measurements near 2.48 m indicate a cumulative trend equivalent to (8.5±1)% increase per year, as well as short-term variability which appears to be strongly correlated with meridional circulation patterns during the February–April months. Based on intensified measurements made over the last three years, it is found that the integrated content of HF undergoes a seasonal change with a minimum occurring in the fall. The HF/HCl ratio derived from simultaneous HF and HCl measurements was found equal to 0.15 during the period 1977–79, and 0.24 for the 1983–85 timespan.     

Intercomparison of stratospheric water vapor profiles obtained during the Balloon Intercomparison Campaign

The Balloon Intercomparison Campaign (BIC) was set up to intercompare remote sensing measurements of a number of compounds other than water vapor; however, water vapor has strong absorption features throughout the infrared and mm wave regions of the spectrum. Therefore many of the investigators involved in BIC have absorption or emission features due to water vapor in the data they obtained during the balloon flights made under the campaign. These features have been used by the investigators to determine the stratospheric water vapor profiles which are compared in this paper. The profiles allow comparison of a wide range of remote sensing techniques involving both emission and absorption in the mid-infrared and emission techniques in the far infrared.     

The Balloon Intercomparison Campaigns an introduction and overview

The Balloon Intercomparison Campaigns of 1982 and 1983 compared balloon-borne sensors of HCl, HNO3, NO2, NO and O3, and measured many other stratospheric constituents. Most sensors were remote rather than in-situ. In the 1982 campaign, three large gondolas were successfully launched from Palestine, Texas on the same day; in the 1983 campaign, four gondolas were launched within 3 days. Accompanying papers describe the results of these successful intercomparisons.     

Intercomparison of NO column measurements during MAP/GLOBUS 1985

Column measurements of nitric oxide were made using several techniques during the MAP/GLOBUS campaign in France in September 1985. The data sets are nearly co-located and simultaneous, therefore allowing a valid intercomparison of the various measurement methods. The range of altitudes sampled differs from instrument to instrument. This complicates the comparison because the data sets are to some extent complementary. The NO distributions apparently vary significantly from day to day, and possibly over shorter timescales. Changes in dynamics may be responsible for these variations. The results from the instruments which measure in the infrared and the ultraviolet are self-consistent, and show good agreement with photochemical predictions. On 19 September, when the intercomparison was made, the profile measured by the in-situ chemiluminescent instrument differed significantly from the predicted profile, and the measured columns were generally higher.     

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.     

一次东移西南涡过程的平流层重力波特征研究

基于WRF模式对2011年6月16—19日一次东移西南涡过程的模拟,开展了西南涡激发平流层重力波的特征研究。东移西南涡可以分为发展、强盛和减弱3个阶段,每个阶段均伴随着强降雨天气,但由于降水位置和强度的不同,平流层重力波的分布和强度也不同。西南涡发展阶段,平流层重力波主要位于低涡的东侧,并向东北传播;西南涡强盛阶段,伴随对流降水的强度和范围明显增大,平流层重力波的振幅和范围也显著增大,且围绕西南涡的东侧和南侧呈现出半环状的重力波分布特征可分为两支,东侧波动波列表现为东北西南向分布,南侧的波列表现为东—西向分布;西南涡减弱阶段,重力波的振幅和范围均减小。波谱分析表明,重力波的纬向波数频率谱关于零频率呈非对称分布,且随着西南涡的增强,波谱在小尺度范围显著增大,即强对流更容易激发出小尺度的高频波;经向波数频率谱在波数较小谱段关于零频率基本呈对称分布,但在波数较大谱段,也呈非对称分布,这说明受平流层东风气流的影响,重力波主要向东传播。     

7个CMIP5模式的平流层、对流层温度趋势与SSU/MSU观测资料的对比

采用1979—2005年美国大气海洋局(NOAA)的卫星观测资料和IPCC第5次全球气候变化比较试验(CMIP5)的模式资料,对全球对流层和平流层近26 a的气温趋势进行了研究。结果表明,CMIP5模拟的全球平均大气温度趋势与观测结果较一致,能够再现平流层冷却和对流层增温等特点,但是在气温趋势的经纬度分布上,模式资料与观测资料间存在较大差异,同时模式间也存在明显的不一致。与观测资料相比,CMIP5模式资料低估了平流层在热带地区的降温速率,而且明显高估了对流层中部到平流层下层的南极区域的降温趋势。不同CMIP5模式间的最大标准方差出现在平流层的南北极区域,但是在对流层所有纬度上标准方差都保持着较小值。     

太阳准周期变化对北半球夏季平流层加热率的影响

采用1979—2013年6—8月欧洲中期数值预报中心ERA-Interim逐月再分析资料和2004—2010年6—8月美国国家大气和海洋管理局太阳光谱辐照度资料,利用北京气候中心大气辐射模式,计算了北半球平流层夏季臭氧加热率(Ozone Heating Rate,OHR)和净加热率(Net Heating Rate,NHR),分析了太阳准11 a变化中太阳活动强年与弱年纬向平均OHR(NHR)的差异,并讨论了差异形成的原因。结果表明:太阳活动强年比弱年的紫外辐射明显要强,导致OHR、NHR整层增强,且随高度增加而增加;臭氧浓度在平流层下层较小,在平流层上层较大,该变化导致OHR、NHR有类似的变化型,且稍向高处偏移;OHR、NHR在平流层上层的变化,由紫外辐射和臭氧共同作用,其他地区均为臭氧起主要作用。     

Nitrogen dioxide column content measurements made from an aircraft between 5° and 82°N

In the first two weeks of May 1981, the research jet of the German Aerospace Research Establishment (DFVLR) was charted to fly a meridional section between 5° and 82°N. A scanning filter photometer, developed at the Max Planck Institut für Aeronomie to measure column content values of atmospheric ozone and nitrogen dioxide, using ultra violet and visible absorption techniques, constituted part of the experimental payload for this campaign that was called SIMOC. The vertical NO₂ column content above the aircraft, flying at approximately 10 km, was found to decrease rapidly from 6.9×10¹⁵ molecules cm^-2 to 2.5×10¹⁵ molecules cm^-2 around 50°N and then to increase again north of 75°N. A sharp rise in the NO₂ content was observed south of the subtropical jet but this could possibly be due to the increased depth of the troposphere above the aircraft in these regions.     

On the nonlinear response of lower stratospheric ozone to NOx and ClOx perturbations for different CH4 sources

The impact of sulfate aerosol, ClOx and NOx perturbations for two different magnitudes of CH4 sources on lower stratospheric ozone is studied by using a heterogeneous chemical system that consists of 19 species belonging to 5 chemical families （oxygen, hydrogen, nitrogen, chlorine and carbon）. The results show that the present modeled photochemical system can present several different solutions, for instance, periodic states and multi-equilibrium states appearing in turn under certain parameter domains, through chlorine chemistry and nitrogen chemistry together with sulfate aerosol as well as the increasing magnitude of CH4 sources. The existence of catastrophic transitions could produce a dramatic reduction in the ozone concentration with the increase of external sources.     

平流层异常下传对2009年12月北半球大范围降雪过程的影响

2009年12月北半球中纬度出现大范围持续低温、暴风雪等天气。采用NCEP／NCAR再分析资料研究了平流层AO（Arctic Oscillation,北极涛动）异常信号下传的特征及其对本次极端气候事件的影响,并讨论了与平流层异常信号下传相关的行星波活动。结果表明：1）与此次极端气候事件相联系的负位相A0异常11月首先发生在平流层,维持将近1个月后于12月初开始下传,并且迅速传至地面。12月整个对流层的位势高度及温度在极区附近出现强的正异常,而中纬度地区则为负异常。2）平流层AO异常信号下传后,地面出现有利于低温降雪过程的环流异常。12月上旬,亚洲大陆东部及北美大陆西部出现异常偏北风,造成了俄罗斯、北美西部大面积负的温度异常;12月中下旬,欧洲大陆盛行偏西北气流,同时蒙古高压增强,欧亚大陆北部包括中国北方出现大片负的温度异常。3）在此次极端气候事件之前,北半球高纬度地区有异常强的行星波上传至平流层,导致平流层出现负位相的AO异常,并维持了一个月;随后,上传到平流层的行星波减弱,同时平流层负位相的AO异常迅速传至地面,导致了有利于低温降雪的环流异常。     

Intercomparison of instruments for measurements of the atmospheric turbulence characteristics

In this paper, intercomparison testings of the Wind Master sonic anemometer manufactured by Gill Instruments Ltd. (U.K.) and two sonic anemometers manufactured by the Taifun Scientific Industrial Association (Obninsk, Russia), ATsAT-3M are described. Data of measurements of the standard deviations and spectrum characteristics of the vertical and horizontal wind speed components, heat and friction fluxes are presented. Dispersion of the measurements and degree of their coherence are characterized by the regression equation coefficients (a and b) and the cross-correlation coefficients. The coherence plot shows compliance of the measurements data throughout the entire frequency range.     

Atmospheric chemistry of hydrogen fluoride

Although a large volume of monitoring and computer simulation data exist for global coverage of HF, study of HF in the troposphere is still limited to industry whose primary interest is the safety and risk assessment of HF release because it is a toxic gas. There is very limited information on atmospheric chemistry, emission sources, and the behavior of HF in the environment. We provide a comprehensive review on the atmospheric chemistry of HF, modeling the reactions and transport of HF in the atmosphere, the removal processes in the vertical layer immediately adjacent to the surface (up to approximately 500 m) and recommend research needed to improve our understanding of atmospheric chemistry of HF in the troposphere. The atmospheric chemistry, emissions, and surface boundary layer transport of hydrogen fluoride (HF) are summarized. Although HF is known to be chemically reactive and highly soluble, both factors affect transport and removal in the atmosphere, the chemistry can be ignored when the HF concentration is at a sufficiently low level (e.g., 10 ppmv). At a low concentration, the capability for HF to react in the atmosphere is diminished and therefore the species can be mathematically treated as inert during the transport. At a sufficiently high concentration of HF (e.g., kg/s release rate and thousands of ppm), however, HF can go through a series of rigorous chemical reactions including polymerization, depolymerization, and reaction with water to form molecular complex. As such, the HF species cannot be considered as inert because the reactions could intimately influence the plume’s thermodynamic properties affecting the changes in plume temperature and density. The atmospheric residence time of HF was found to be less than four (4) days, and deposition (i.e., atmosphere to surface transport) is the dominant mechanism that controls the removal of HF and its oligomers from the atmosphere. The literature data on HF dry deposition velocity was relatively high compared to many commonly found atmospheric species such as ozone, sulfur dioxide, nitrogen oxides, etc. The global average of wet deposition velocity of HF was found to be zero based on one literature source. Uptake of HF by rain drops is limited by the acidity of the rain drops, and atmospheric particulate matter contributes negligibly to HF uptake. Finally, given that the reactivity of HF at a high release rate and elevated mole concentration cannot be ignored, it is important to incorporate the reaction chemistry in the near-field dispersion close to the proximity of the release source, and to incorporate the deposition mechanism in the far-field dispersion away from the release source. In other words, a hybrid computational scheme may be needed to address transport and atmospheric chemistry of HF in a range of applications. The model uncertainty will be limited by the precision of boundary layer parameterization and ability to accurately model the atmospheric turbulence.     

Measurements of stratospheric chlorine monoxide (ClO) from groudbased FTIR observations

Infrared absorption features due to ClO in the lower stratosphere have been identified from groundbased solar absorption spectra taken from Aberdeen, U.K. (57° N, 2° W) on 20 January 1995. A vertical column abundance of 3.42 (±0.47)×10¹⁵ molec cm^-2 has been derived from 13 independent absorption features in the P and R branches of the (0–1) vibration-rotation band of ³⁵ClO, spanning the spectral region 817–855 cm^-1. The observed absorption features are consistent with very high levels of ClO (approximately 2.6 parts per billion by volume (ppbv)) in the altitude range 16–22 km. A comparison of this profile with a 3D chemical transport model profile indicates the observation was made inside the polar vortex and shows good qualitative agreement but the model underestimates the concentrations of ClO. Simultaneous measurements of other species were made including HCl, HF and ClONO₂. These columns yield a value for HCl+ClONO₂+ClO of 7.02±0.65×10¹⁵ molec cm^-2. This is lower than the total inorganic chlorine (ClO _y ) column of 10.7±1.6×10¹⁵ molec cm^-2 estimated from mean measured (HCl+ClONO₂)/HF ratios together with in-vortex HF measurements. The discrepancy is probably due to significant amounts of the ClO dimer (Cl₂O₂) in the lower part of the stratosphere. The measurements of highly elevated levels of ClO are used to estimate O₃ loss rates at the 400, 475 and 550 K levels making assumptions about the probable distribution of ClO and Cl₂O₂. These are compared with loss rates derived from ozone sonde data.     

Altitude profile and sunset decay measurements of stratospheric nitric oxide

In July 1974 an NO/O₃ chemiluminescent instrument was used to obtain measurements of NO in the stratosphere during two balloon flights launched from Churchill (59°N, 95°W). On the first flight, an altitude profile was obtained in which the NO volume mixing ratio was observed to increase from 0.3 to 2.7 ppbv between 19 and 29.5 km. On the second flight, the mixing ratio was observed to increase from 0.25 to 2.7 ppbv between 19 and 29 km and to remain almost constant at about 2.7 ppbv from 29 to 34.5 km. On this flight, the sunset decay of NO was also obtained while the payload was at a constant float altitude of 34.5 km. These decay measurements are compared satisfactorily with the results obtained from a time dependent stratospheric model.     

Balloon Intercomparison Campaigns: Results of remote sensing measurements of HCl

All of the techniques used to measure stratospheric HCl during the two BIC campaigns involved high resolution infrared spectroscopy. The balloon-borne instruments included five different spectrometers, three operating in the solar absorption mode and two in emission (at distinctly different wavelengths). Ground-based and aircraft correlative measurements were made close to the balloon locations, again by near-infrared spectroscopy.Within this set of results, comparisons between different techniques (absorption vs emission) viewing the same airmass (i.e., on the same gondola) were possible, as were comparisons between the same technique used on different gondolas spaced closely in time and location. The final results yield a mean profile of concentration of HC1 between 18 and 40 km altitude; an envelope of ±15% centered on this profile encompasses all of the results within one standard deviation of their individual mean values. The absolute accuracy of the final profile is estimated to be no worse than 10%. It is concluded also that the measurement techniques for HCl have reached a level of performance where a precision of 10% to 15% can be confidently expected.