平流层臭氧深度侵入对典型城区的影响过程分析

中纬度平流层臭氧深度侵入是造成对流层至近地面臭氧浓度突增的原因之一。筛选春夏季臭氧浓度升高时段的高分辨率大气再分析数据ERA5,以位涡值的下沉趋势分析了对流层顶折叠位置及变化过程;以AIRS数据反演了臭氧浓度、一氧化碳浓度和相对湿度的垂直廓线,并估计了其分布及相关性;以近地表污染物浓度变化、HYSPLIT模型后向轨迹分析结果证实了臭氧侵入气团的运移轨迹和局地效应;通过激光雷达监测结果观测臭氧垂直浓度分布,确定了臭氧浓度最大值所处高度,判定了受影响近地点的浓度升高时刻;以边界层高度变化、气象条件分析结果及当地与周边城市地面监测数据的逐小时变化情况等综合信息,进行了区域确认和近地面影响判定。通过以上数值综合分析,对城市地区受平流层臭氧深度侵入影响的过程和具体时间进行了详细再现,可为排除非人为排放因素导致的近地表臭氧浓度增加提供回溯分析,为臭氧污染防控决策提供依据。     

Airborne measurements of peroxy radicals using the PERCA technique

The Peroxy Radical Chemical Amplifier (PERCA) technique is a proven method for measurement of ambient levels of peroxy radicals at ground level, but there are no published instances of the technique being used on an aerial platform. Here we describe deployment of a PERCA on the former UK Meteorological Office C-130 Hercules research aircraft. The instrument uses the established method of chemical amplification and conversion of peroxy radicals to nitrogen dioxide (NO2) by doping the sample air-flow matrix with CO and NO, subsequently measuring the NO2 yield with an improved 'Luminox' LMA-3 NO2 detector. NO2 from the amplification chemistry is distinguished from other sources of NO2 reaching the detector by periodically injecting CO approximately 1 s downstream of the NO injection point (termination mode). Chain lengths (CL's) for the amplification chemistry were typically approximately 260 (ground level) to approximately 200 (7,000 m). This variation with altitude is less than the variation associated with the 'age' of the PFA inlet material where the amplification chemistry occurs; CL's of approximately 200 with old tubing to approximately 300 with new clean tubing were typical (ground level values). The CL determinations were made in-flight using an onboard calibration unit based on the 254 nm photolysis of 7.5 to 10 parts per billion (by volume, ppbv) of CH3I in air, producing CH3O2 in a quantitative manner. The noise-equivalent detection limit for peroxy radicals (HO2 + RO2) is 2 parts per trillion (by volume, pptv) at 3,650 m when the background ambient ozone levels are stable, based on a 5 min average of five 30 s amplification cycles and five 30 s termination cycles. This detection limit is a function of several factors but is most seriously degraded when there is large variability in the ambient ozone concentration. This paper describes the instrument design, considers its performance and proposes design improvements. It concludes that the performance of an airborne PERCA in the free troposphere can be superior to that of ground-based instruments when similar sampling frequencies are compared.     

京津冀地区一次浮尘过程的车载激光雷达走航观测

利用双波长三通道激光雷达与车载激光雷达,针对2018年3月28日京津冀区域的浮尘天气过程,分别进行了定点垂直观测与车载走航观测,对这次浮尘天气中沙尘的源地、沙尘气溶胶的时空分布、沙尘的传输路径与传输方式进行了综合分析。位于北京的激光雷达监测到28日凌晨开始,沙尘气溶胶与近地面污染物混合,受沙尘影响近地面污染物浓度迅速升高。北京到沧州的车载激光雷达走航观测结果显示,沙尘气溶胶先向南传输到京津冀南部区域,随后向西南方向传输,同时观测到京津冀区域上空1. 5 km左右存在沙尘传输带。结果表明,使用车载激光雷达走航观测,结合定点垂直激光雷达与其他地面监测数据,能可靠地观测到沙尘过程中颗粒物的时空变化特征。     

The Characteristics of Tropospheric Ozone Seasonality Observed from Ozone Soundings at Pohang, Korea

This paper presents the first analysis of vertical ozone sounding measurements over Pohang, Korea. The main focus is to analyze the seasonal variation of vertical ozone profiles and determine the mechanisms controlling ozone seasonality. The maxima ozone at the surface and in the free troposphere are observed in May and June, respectively. In comparison with the ozone seasonality at Oki (near sea level) and Happo (altitude of 1840 m) in Japan, which are located at the same latitude as of Pohang, we have found that the time of the ozone maximum at the Japanese sites is always a month earlier than at Pohang. Analysis of the wind flow at the surface shows that the wind shifts from westerly to southerly in May over Japan, but in June over Pohang. However, this wind shift above boundary layer occurs a month later. This wind shift results in significantly smaller amounts of ozone because the southerly wind brings clean wet tropical air. It has been suggested that the spring ozone maximum in the lower troposphere is due to polluted air transported from China. However, an enhanced ozone amount over the free troposphere in June appears to have a different origin. A tongue-like structure in the time-height cross-section of ozone concentrations, which starts from the stratosphere and extends to the middle troposphere, suggests that the ozone enhancement occurs due to a gradual migration of ozone from the stratosphere. The high frequency of dry air with elevated ozone concentrations in the upper troposphere in June suggests that the air is transported from the stratosphere. HYSPLIT trajectory analysis supports the hypothesis that enhanced ozone in the free troposphere is not likely due to transport from sources of anthropogenic activity.     

Two high-speed, portable GC systems designed for the measurement of non-methane hydrocarbons and PAN: results from the Jungfraujoch High Altitude Observatory

Near real-time measurements of light non-methane hydrocarbons (NMHCs) and peroxyacetyl nitrate (PAN) have been performed in the free troposphere using two fast gas chromatography (GC) instruments designed for use on aircraft. A GC-helium ionisation detector (HID) system measured 15 C(2)-C(5) hydrocarbons with 5 min time resolution and a dual channel GC-Electron Capture Detector (ECD) measured PAN with 90 s resolution. Both instruments had low parts per trillion by volume (pptV) detection limits and ran continuously at the remote Jungfraujoch (JFJ) research station in the Swiss Alps (46.55[degree]N, 7.98[degree]E), 3580 m above mean sea level (AMSL), during February/March 2003. Carbon monoxide, ozone, nitrogen oxide and nitrogen dioxide and all odd nitrogen species (NO(y)) were also measured continuously. Hydrocarbons and CO were strongly correlated in all air-masses whilst PAN exhibited both positive and negative correlations with respect to O(3), dependent on age and origin of the air-mass sampled. PAN was found to contribute [similar]20% to the NO(y) sampled on average. The experiment, as well as providing interesting datasets from this remote location, also demonstrated that when optimised, GC techniques have the potential to measure at a time resolution significantly greater than is traditionally considered, with high sensitivity and low uncertainty.     

京津冀一次空气重污染过程激光雷达走航观测分析

针对2016年国庆期间一次污染消散过程,开展了激光雷达定点与走航观测,并综合运用中国环境监测总站国家预报平台数值模型预报结果和国控站点PM_(2.5)监测数据,对污染团的移动和分布进行了分析。结果表明,雷达定点观测的消光系数突变,主要由北京西部累积污染团在夜间弱西北气流作用下的回流所引起。受此西北气流影响移出北京的污染气团在天津至沧州一带滞留。北京至保定沿线颗粒物污染消散现象,被雷达走航观测所捕捉。     

臭氧数值预报模型综述

光化学大气质量模型在研究臭氧(O_3)污染以及O_3预报方面具有核心作用,是O_3污染防治决策者的有力工具。文章结合目前中国及国际区域尺度光化学大气质量预报模型的研究与应用,重点论述与O_3有关的大气化学过程在数值预报模型中的数学表达和计算方法,阐述大气物理与大气化学过程在主流大气质量数值预报模型中的实现方法及其优势和缺陷,介绍用于数值预报模型的大气物理过程和湍流参数化方案的最新进展。就当前O_3数值模拟的主要输入资料进行讨论,强调那些易被忽视但又显著影响模型预报能力和效果的诸多因素以及模型效果评估的重要性。结合O_3与复合型大气污染的关系,强调区域大气质量数值预报模型的发展趋势与方向以及在大气环境管理方面的意义和作用。     

Review of ozone and temperature lidar validations performed within the framework of the Network for the Detection of Stratospheric Change

The use of assimilation tools for satellite validation requires true estimates of the accuracy of the reference data. Since its inception, the Network for Detection of Stratospheric Change (NDSC) has provided systematic lidar measurements of ozone and temperature at several places around the world that are well adapted for satellite validations. Regular exercises have been organised to ensure the data quality at each individual site. These exercises can be separated into three categories: large scale intercomparisons using multiple instruments, including a mobile lidar; using satellite observations as a geographic transfer standards to compare measurements at different sites; and comparative investigations of the analysis software. NDSC is a research network, so each system has its own history, design, and analysis, and has participated differently in validation campaigns. There are still some technological differences that may explain different accuracies. However, the comparison campaigns performed over the last decade have always proved to be very helpful in improving the measurements. To date, more efforts have been devoted to characterising ozone measurements than to temperature observations. The synthesis of the published works shows that the network can potentially be considered as homogeneous within +/-2% between 20-35 km for ozone and +/-1 K between 35-60 km for temperature. Outside this altitude range, larger biases are reported and more efforts are required. In the lower stratosphere, Raman channels seem to improve comparisons but such capabilities were not systematically compared. At the top of the profiles, more investigations on analysis methodologies are still probably needed. SAGE II and GOMOS appear to be excellent tools for future ozone lidar validations but need to be better coordinated and take more advantage of assimilation tools. Also, temperature validations face major difficulties caused by atmospheric tides and therefore require intercomparisons with the mobile systems, at all sites.     

Ozone Destruction on Solid Particles

Ozone (O3) is an important constituent of the Earth atmosphere, either stratosphere, where it has a beneficial role to protect Earth's surface from harmful UV-B radiation, or troposphere where it is considered an air pollutant. We investigated the ozone destruction on solid particles of natural or anthropogenic origin as: silica-gel, pollen, coal fly ash, titanium dioxide with different specific surface (s) and sodium halides (NaCl, NaBr and NaI). The experiments were conducted in a fluidized bed reactor with elevated ambient concentrations of O3 (100 ppb) employed. The results indicate that the destruction of O3 depends upon: sample quantity (silica-gel with equal s), sample surface (TiO2 with different s) and chemical composition (coal fly ash comparative to wood ash). Interesting results were obtained with sodium halides: no effect on O3 concentrations was detected with NaCl, NaBr shows a certain destruction, while NaI removes completely O3 from the air stream. In the experiments with NaI doped NaCl, the destruction of O3 was dependent on NaI quantity.     

西太平洋台风“苏迪罗”对我国珠三角地区臭氧污染影响研究

通过资料分析和数值模拟开展了2015年8月1日—10日台风“苏迪罗”对珠三角地区臭氧（O₃）污染影响的机理研究。结果表明，2015年8月5—8日，在台风接近登陆点的过程中，台风外围天气导致了高温、高辐射和静小风等气象条件，促进了光化学反应的进行和污染物的局地积累。同时，高温、高辐射等气象条件加剧了植被源区生物源挥发性有机物（BVOCs）的排放。采用化学传输模式模拟发现，植被BVOCs对O₃污染的贡献最高可达24×10^-9。结合拉格朗日粒子扩散模式（LPDM）探索了影响珠三角地区的主导气团，发现珠三角城市地区和高BVOCs源区存在交互传输的现象。污染期间，高BVOCs源区的一次排放产物（BVOCs）和二次产物(O₃)经区域输送加剧了珠三角地区O₃的污染。此外，研究发现台风外围条件下珠三角内陆盛行的偏北风与海陆热力差异引起的海风在沿海地区辐合，造成污染物局地积累，加剧并延长了O₃污染。研究有利于加强对O₃污染机理的认识，进而更好地采取针对性措施，有助于减小O₃污染带来的危害。     

Assessment of ozone effects on local rice cultivar by portable ozone fumigation system in Hanoi, Vietnam

This study examined the effects of troposphere ozone (O3) on rice by developing a portable ozone fumigation system and applied to the field in Hanoi, Vietnam. The system was nearly identical to the open top chamber but designed to easily and cheaply assess the O3 sensitivity of local agricultural crops in the actual field. The rice (Oryza sativa L.) was exposed to ozone during the flowering stage at peri-urban experimental site of Hanoi. The fumigation protocols covered five different levels, namely; non-filtered air (ambient) as the control treatment, 32, 62, 85 and 113 ppb in 7-h mean. It was found that observed impacts corresponded well to similar open-top chamber studies in other Asian countries. The methodology and the system left a large room for improvement and called for very careful interpretation and pre-conditions (e.g. low ambient O3 concentration). However, the portable O3 exposure in the field might open a door to the less developed countries to implement the phytotoxic risk assessment of the local agricultural species.     

Global and Regional Distribution of Carbon Monoxide from MOPITT: Seasonal Distribution at 700 hPa

The Measurement of Pollution in the Troposphere (MOPITT) instrument is an eight-channel gas correlation radiometer, which was launched on the Earth Observing System (EOS) Terra satellite in 1999. Carbon monoxide (CO) is one of the important trace gases because its concentration in the troposphere directly influences the concentrations of tropospheric hydroxyl (OH), which controls the lifetimes of tropospheric trace gases. CO traces the transport of global and regional pollutants from industrial activities and large scale biomass burning. The global and regional distributions of CO were analyzed using the MOPITT data for East Asia, which were compared with the ozone distributions. In general, seasonal CO variations are characterized by a peak in the spring, which decrease in the summer. This work also revealed that the seasonal cycles for CO are at a maximum in the spring and a minimum in the summer, with average concentrations ranging from 118 to 170 ppbv. The monthly average for CO shows a similar profile to that for O3. This fact clearly indicates that the high concentration of CO in the spring is possibly due to one of two causes: the photochemical production of CO in the troposphere, or the transport of the CO into East Asia. The seasonal cycles for CO and O3 in East Asia are extensively influenced by the seasonal exchanges of different air mass types due to the Asian monsoon. The continental air masses contain high concentrations of O3 and CO, due to the higher continental background concentrations, and sometimes to the contribution from regional pollution. In summer this transport pattern is reversed, where the Pacific marine air masses that prevail over Korea bring low concentrations of CO and O3, which tend to give the apparent summer minimums.     

Pool of Dust Particles over the Asian Continent: Balloon-borne Optical Particle Counter and Ground-based Lidar Measurements at Dunhuang, China

Measurements of aerosols were made in 2001 and 2002 at Dunhuang (40 degrees 00'N, 94 degrees 30'E), China to understand the nature of atmospheric particles over the desert areas in the Asian continent. Balloon-borne measurements with an optical particle counter suggested that particle size and concentration had noticeable peaks in super micron size range not only in the boundary mixing layer but also in the free troposphere. Super-micron particle concentration largely decreased in the mid tropopause (from 5 to 10 km; above sea level, a.s.l.). Lidar measurements made during August 2002 at Dunhuang suggested the possibility that mixing of dust particles occurred from near the ground to about 6 km even under calm weather conditions, and a large depolarization ratio of particulate matter was found in the aerosol layer. The top of the aerosol layer was found at heights of nearly 6 km (a.s.l.). It is strongly suggested that nonspherical dust particles (Kosa particles) frequently diffused in the free atmosphere over the Taklamakan desert through small-scale turbulences and are possible sources of dust particles of weak Kosa events that have been identified in the free troposphere not only in spring but also in summer over Japanese archipelago. Electron microscopic experiments of the particles collected in the free troposphere confirmed that coarse and nonspherical particles observed by the mineral particle were major components of coarse mode (diameter larger than 1 microm) below about 5 km over Dunhuang, China.     

Determination of O3, NO2, SO2, CO and PM10 measured in Belgrade urban area

O(3), NO(2), SO(2), CO and PM(10) concentrations, simultaneously determined for the first time in Belgrade urban area in the autumnal period of 2005, are presented. The obtained results display similar behaviour of SO(2), NO(2), CO, PM(10) opposite from that of O(3). The weekend effect was also investigated showing diminution of average daily concentrations of SO(2), NO(2), PM(10) and CO for 72, 40, 37 and 42% respectively, and increase of the average daily concentration of O(3) for 56%. Influence of meteorological conditions on observed concentration levels was studied, too. The observed influence of wind speed on the O(3) nightly concentration levels was analyzed pointing to the phenomena of O(3) transport during episodic measurements. To make an identification of possible pollution sources and analyse the influence of meteorological parameters on pollution levels, air back trajectories for high level concentrations episodes were calculated and analysed. A multivariate receptor modelling (Principal Component Analysis, Cluster Analysis) has been applied to a set of data in order to determine the contribution of different sources. It was found that the main principal components, extracted from the air pollution data, were related to gasoline combustion, oil combustion and ozone transport.     

Characteristics of surface ozone at an urban site of Xi'an in Northwest China

Surface ozone concentrations in Xi'an, China were monitored from March 23, 2008 to January 12, 2009 using the Model ML/EC9810 ozone analyzer. The daily average O(3) ranged from <1 ppb to 64.2 ppbv with an annual average of 16.0 ppbv. The seasonal average of O(3) in summer (32.5 ppbv) was more than 10 times higher than that in winter (3.0 ppbv). A significant positive correlation was found between ozone concentration and ambient temperature, indicating that the intensity of solar radiation was one of the several major factors controlling surface ozone production. Using the NOAA HYSPLIT 4 trajectory model, the three longest O(3) pollution episodes were found to be associated with the high biogenic volatile organic carbon (BVOC) emissions from the vegetation of Qinling Mountains. No significant weekday and weekend difference in O(3) levels was detected due to the non-significant change in NO(x) emissions. O(3) depletion by NO emission directly emitted from vehicles, low oxygenated VOC concentrations, and low-level solar radiation caused by high aerosol loading all contributed to the low levels of O(3) found in Xi'an compared to other cities and rural areas.     

宜宾地区气溶胶垂直结构地基空基联合监测分析

利用Cloud-Aerosol LIDAR with Orthogonal Polarization （CALIOP）正交极化云-气溶胶星载激光雷达Level1B资料和LGJ-01型号气溶胶地基激光雷达资料对宜宾地区2016年12月—2017年2月无污染时期、少云轻度污染时期和多云重度污染时期气溶胶的衰减后向散射系数和退偏振比光学参数的垂直分布进行对比分析研究。结果表明：少云轻度污染时期，CALIOP数据监测到海拔高度为0.2~1.0 km范围内气溶胶颗粒集中分布，LGJ-01数据监测到厚度约为0.2 km的近地面气溶胶层，2个激光雷达监测结果基本一致；重度污染时期，LGJ-01地基激光雷达能够较好地探测近地面气溶胶层，CALIOP星载激光雷达能够较好地探测到高空云层，若将两者结合，则能实现不同天气状况下的综合探测，以期较全面客观地为研究气溶胶垂直结构提供观测及科研数据。     

臭氧综合指数与臭氧潜势指数的构建与应用

随着社会经济的快速发展,我国臭氧污染日益严重,因此,研发出能定量评估气象条件对臭氧污染影响程度的诊断指数,成为提高和改善气象服务质量的重要任务之一。利用中国大陆地区2018年温度、总云量、风速、风向、相对湿度等气象场数据与臭氧浓度数据,研究臭氧污染敏感气象条件,统计各气象因子分布在不同数值区间时发生臭氧污染事件的相对频率(即分指数),按照分指数最大值和最小值的差值大小进行排序,筛选出10个与臭氧污染密切相关的气象因子,将10个气象因子的分指数进行累加,即得出臭氧综合指数。随后,对各地构建臭氧综合指数时采用的气象要素进行统计,得到出现频率最高的3个气象要素,并参考这些气象要素构建了臭氧潜势指数。分别以臭氧潜势指数和臭氧综合指数对北京市2019年臭氧日最大浓度建立拟合预报模型,结果表明:两类指数的拟合预报值与实测值有着相似的变化趋势;利用臭氧综合指数计算得到的预报值与实测值的相关系数为0.76,优于利用臭氧潜势指数计算得到的预报值与实测值的相关系数(0.64)。     

Differences between weekend and weekday ozone levels over rural and urban sites in Southern Italy

Air quality data from a network of 11 monitoring stations in the Apulia region of southern Italy during the summer of 2005 reveal a high frequency of ozone law limit violations. Since ozone is a secondary pollutant, air quality control strategies aimed at reducing ozone concentration are not immediate. Herein, we analyse weekly changes in concentration levels of ozone (O(3)), nitrogen oxides (NO(x)), carbon monoxide (CO), and volatile organic compounds (VOCs), and evaluate how the differences in primary emissions cause changes in the production of ozone. The comparison between weekend and weekday levels of O(3) and its precursors are direct evidence for the existence of the "ozone weekend effect." This effect was observed at all stations with a considerable variation in the overall ozone magnitude, including both traffic stations and non-traffic stations. Data from VOC measurements at traffic stations primarily indicated elevated levels of benzene, toluene, and xylenes (BTX); all of these substances showed an overall decrease over the weekend. A single station indicated levels of non-methane hydrocarbon (NMHC) and PM10, both of which did not demonstrate any weekly cycle. Analysis of weekly and diurnal cycles of O(3), NO(x), CO, NMHC, and PM10 indicates that higher weekend ozone levels result from a reduction in the emission of nitrogen oxides on weekends in VOC-sensitive regimes. This indicates that a reduction in VOC and NO(x) levels would be more effective than NO(x) reduction alone. Our results underscore the need for improved and more efficient VOC measurements.     

An observational case study of ozone and precursors inflow to South East England during an anticyclone

Summertime photochemical air pollution episodes within the United Kingdom have been proposed via modelling studies to be strongly influenced by regional scale inflow of air from the continental European boundary layer. We present a vertically resolved case study using measurements made from the NERC/Met Office BAe 146 research aircraft on 18th August 2005 over the South East of England and the North Sea during a weak anticyclone centred over Northern Europe. The vertical distribution of ozone, CO, NO(x), peroxyacetyl nitrate (PAN) and a wide range of both nonmethane hydrocarbons (NMHC) and oxygenated volatile organic compounds (OVOCs) were determined between 500 ft (approximately 152 m) and 7000 ft (approximately 2134 m) over the East Anglia coastline and 50 km inland. In excess of 80 ppbV ozone was observed within inflowing boundary layer air over the North Sea coast in a broad N-S sloping feature around 60 km wide. The inflowing feature of European origin was also observed further inland within the boundary layer albeit with lower, more variable, ozone mixing ratios. The increased variability in ozone over land was a product of titration by fresh surface emissions of NO via rapid upward transport in thermals, a hypothesis supported by the observed vertical wind speed component. Fast boundary layer mixing over land was further illustrated by a uniform distribution in reactive alkenes. A comparison between aircraft and surface O(3) UK AUN (Automatic Urban Network) measurements showed good agreement with the inland site, Sibton, but marked differences with the coastal monitoring site at Weybourne, potentially due to gradients established by ocean deposition in stably stratified marine air.