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1.
Fifty flask air samples were taken during April 1986 from a NOAA WP-3D Orion aircraft which flew missions across a broad region of the Arctic as part of the second Arctic Gas and Aerosol Sampling Program (AGASP II). The samples were subsequently analyzed for both carbon dioxide (CO2) and methane (CH4). The samples were taken in well-defined layers of Arctic haze, in the background troposphere where no haze was detected, and from near the surface to the lower stratosphere. Vertical profiles were specifically measured in the vicinity of Barrow, Alaska to enable comparisons with routine surface measurements made at the NOAA/GMCC observatory. Elevated levels of both methane and carbon dioxide were found in haze layers. For samples taken in the background troposphere we found negative vertical gradients (lower concentrations aloft) for both gases. For the entire data set (including samples collected in the haze layers) we found a strong positive correlation between the methane and carbon dioxide concentrations, with a linear regression slope of 17.5 ppb CH4/ppm CO2, a standard error of 0.6, and a correlation coefficient (r2) of 0.95. This correlation between the two gases seen in the aircraft samples was corroborated by in situ surface measurements of these gases made at the Barrow observatory during March and April 1986. We also find a similar relationship between methane and carbon dioxide measured concurrenty for a short period in the moderately polluted urban atmosphere of Boulder, Colorado. We suggest that the strong correlation between methane and carbon dioxide concentrations reflects a common source region for both, with subsequent long-range transport of the polluted air to the Arctic.  相似文献   

2.
A series of 72 measurements of the acetaldehyde (CH3CHO) mixing ratio were made in the lower troposphere during TROPOZ II. These measurements are the first ever made of the background level of this trace gas in the free troposphere. The data show a vertical decrease of the CH3CHO mixing ratio with increasing altitude and indicate higher CH3CHO concentrations in the Northern Hemisphere — in general agreement with a model-derived average CH3CHO distribution. Deviations of the observed CH3CHO mixing ratios from the modelled mean distribution are correlated with similar deviations in the corresponding HCHO mixing ratios.  相似文献   

3.
Results of more than 800 new measurements of methane (CH4) concentrations in the Southern Hemisphere troposphere (34–41° S, 130–150° E) are reported. These were obtained between September 1980 and March 1983 from the surface at Cape Grim, Tasmania, through the middle (3.5–5.5 km) to the upper troposphere (7–10 km). The concentration of CH4 increased throughout the entire troposphere over the measurement period, adding further support to the view that CH4 concentrations are currently increasing on a global scale. For data averaged vertically through the troposphere the rate of increase found was 20 ppbv/yr or 1.3%/yr at December 1981. In the surface CH4 data a seasonal cycle with a peak to peak amplitude of approximately 28 ppbv is seen, with the minimum concentration occurring in March and the maximum in September–October. A cycle with the same phase as that seen at the surface, but with a significantly decreased amplitude, is apparent in the mid troposphere but no cycle is detected in the upper tropospheric data. The phase and amplitude of the cycle are qualitatively in agreement with the concept that the major sink for methane is oxidation by hydroxyl radicals. Also presented is evidence of a positive vertical gradient in methane, with a suggestion that the magnitude of this gradient has changed over the period of measurements.  相似文献   

4.
利用瓦里关大气本底站甲烷观测数据对美国Aqua卫星的AIRS观测结果进行对比分析,并分析研究了2003~2012年青藏高原对流层大气甲烷的时空分布特征,结果表明:1)AIRS观测结果与近地面观测资料变化趋势一致,存在显著的正相关关系,突变时间比较一致,可以用于青藏高原区域的甲烷浓度特征分析。2)青藏高原对流层甲烷浓度在空间分布上存在显著的西北—东南走向的低值带及其南北侧存在4个固定的高值中心,分别位于阿里、那曲、山南和玉树。3)青藏高原甲烷浓度呈现显著随高度而降低的趋势,年平均甲烷浓度分别为1.810ppm(1 ppm=10-6)、1.797 ppm和1.781 ppm。在对流层中层和中上层,甲烷浓度基本呈现低值带最低、南北侧均高的山谷型分布特征。在对流层层顶,以低值带为分界线,呈现明显的南高北低特征。4)青藏高原甲烷浓度随时间呈缓慢上升趋势,平均速度为0.0018 ppm/a,夏季上升最快,秋季上升最慢。5)青藏高原甲烷存在明显的单峰型季节变化特征,夏秋季高,冬春季低,与东部地区冬、夏双峰型特征不同,随着高度上升季节变化更为明显。  相似文献   

5.
Measurements of carbon dioxide(CO2), methane(CH4), and carbon monoxide(CO) are of great importance in the Qinghai-Tibetan region, as it is the highest and largest plateau in the world affecting global weather and climate systems. In this study, for the first time, we present CO2, CH4, and CO column measurements carried out by a Bruker EM27/SUN Fourier-transform infrared spectrometer(FTIR) at Golmud(36.42°E, 94.91°N, 2808 m) in August 2021. The mean and...  相似文献   

6.
Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr3, CH2BrCl, CHBr2Cl, CHBrCl2, and CH2Br2) and CH3Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO x and NO x . Globally, the impact of bromine chemistry on tropospheric O3 is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O3 burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH3OOH, H2O2).  相似文献   

7.
A network of remote and in-situ sensors was deployed in a Paris suburb in order to evaluate the mesoscale evolution of the daily cycle of CO2 and related tracers in the atmospheric boundary layer (ABL) and its relation to ABL dynamics and nearby natural and anthropogenic sources and sinks. A 2-μm heterodyne Doppler differential absorption lidar, which combines measurements of, (1) structure of the atmosphere, (2) radial velocity, and (3) CO2 differential absorption was a particularly unique element of the observational array. We analyse the differences in the diurnal cycle of CO, CO2, lidar reflectivity (a proxy for aerosol content) and H2O using the lidar, airborne measurements in the free troposphere and ground-based measurements made at two sites located few kilometres apart. We demonstrate that vertical mixing dominates the early morning drawdown of CO and aerosol content trapped in the former nocturnal layer but not the H2O and CO2 mixing ratio variations. Surface fluxes, vertical mixing and advection all contribute to the ABL CO2 mixing ratio decrease during the morning transition, with the relative importance depending on the rate and timing of ABL rise. We also show evidence that when the ABL is stable, small-scale (0.1-km vertical and 1-km horizontal) gradients of CO2 and CO are large. The results illustrate the complexity of inferring surface fluxes of CO2 from atmospheric budgets in the stable boundary layer.  相似文献   

8.
利用搭载在美国Aqua卫星上的大气红外探测仪(AIRS)观测资料反演的全球甲烷(CH_4)产品和NCEP再分析资料,分析了2003~2014年青藏高原上空CH_4的时空变化特征,探讨了夏季CH_4高值变化与季风的关系。研究结果表明:就青藏高原整体而言,CH_4浓度随高度增加递减;对流层中高层CH_4含量季节变化较为明显,其平均浓度在7~9月处于高值,6月、10月次之,其余月份处于低值。2003~2014年CH_4含量呈逐年上升趋势,年增长率约为4.66ppb(10-9)。高原上空CH_4空间分布分析显示,高原北部CH_4浓度高于南部地区。夏季风期间,随着高原上的强对流输送和上空南亚高压的阻塞,对流层中高层CH_4浓度明显增加并不断积累,在8月底至9月初出现最大值。在分析季风指数的基础上发现,夏季季风影响下的强对流输送是高原对流层中高层CH_4高值形成的主要原因之一,对流层中高层CH_4浓度最大值出现时间较季风指数的峰值滞后约半至一个月,随着夏季风的撤退,CH_4浓度高值迅速降低。  相似文献   

9.
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.  相似文献   

10.
To investigate an alternative technique of providing background and transboundary transport inputs for ozone (O3) simulations on a regional scale, the EPA’s Community Multi-scale Air Quality (CMAQ) model was integrated with high spectral resolution data from the Tropospheric Emission Spectrometer (TES) aboard the NASA’s Aura satellite. This study presents a comprehensive model evaluation of O3 for the entire year of 2009 over the contiguous United States with a focus on the State of Texas using both ozonesonde and ground measurements. While improving model performance in the upper atmosphere, CMAQ’s initial and boundary conditions (IC/BC) derived from the original TES data do not improve model performance in the troposphere because the satellite data exaggerated concentration of tropospheric O3. With a 10-ppb deduction of O3 concentration from TES, the IC/BC derived from the adjusted TES improves model performance from ground level through the upper atmosphere. The mean bias of daily maximum 8-h average concentration of O3 (MDA8) from the ground monitored in Texas decreased from 7 ppb to 4 ppb. Model results also show small influences of O3 from the upper troposphere on the concentrations at the ground level. With a complete exclusion of stratospheric layers, changes of annual mean MDA8 of O3 concentrations at ground-level were smaller than 1.1 % in Dallas and Houston. In addition, limitations of satellite data are discussed and recommendations are provided regarding the future application of satellite data in regional O3 simulations.  相似文献   

11.
利用探空站数据对北京和张家口冬奥赛场周边地区的地基微波辐射计和FY 4A大气垂直探测仪资料进行验证分析。选取2020年全年FY 4A大气垂直探测仪资料以及2020年12月至2021年3月期间对冬奥赛事有重要影响的寒潮前后、雾霾和沙尘暴这3种不同天气现象下探测得到的气温廓线数据进行个例分析。结果表明:在晴空条件下,地基微波辐射计和FY 4A大气垂直探测仪探测大气垂直气温的精度较高,平均相关系数达到0.97,低层大气(500 hPa以下)较高层大气探测结果的一致性较好;大气污染对探测精度产生一定影响,其中PM2.5产生的影响较小,PM10的提高对FY 4A大气垂直探测仪的探测产生较大影响,尤其是发生沙尘暴时,星载探测仪无法对低层大气进行探测。经过对比和验证,卫星探测作为补充探测手段,可以与地基微波辐射计互相补充,尤其是在空间覆盖和时间分辨率上具备一定优势,但在有云和沙尘暴的天气条件下无法对低层大气开展探测;地基微波辐射计可以对一个地点的大气垂直参数开展不间断的探测,与探空站数据的一致性较高。卫星探测和地基微波辐射计均可以为冬奥赛事提供高时间分辨率的探测数据,为数值天气预报提供有力的数据支撑。  相似文献   

12.
Dibromomethane (CH2Br2), a natural stratospheric ozone depleting substance, is mostly emitted from the ocean, but the relative importance of coastal (or macroalgae) and open ocean emissions is unknown. We made long-term high-frequency measurements of CH2Br2 concentrations at two remote coastal sites in Japan, on the subtropical Hateruma Island (poor in macroalgae) and at Cape Ochiishi (rich in macroalgae). CH2Br2 concentrations at Hateruma showed prominent seasonal variation, being lower in summer (around 0.94 ppt) than in winter (around 1.23 ppt). In contrast, CH2Br2 concentrations at Ochiishi were highly variable, often exceeding 2 ppt in the summer but with minimum baseline concentrations close to those from Hateruma; in the winter the concentrations were almost constant at about 1.3 ppt. Analysis of the data suggested that (1) emissions from macroalgae were not likely to extend offshore, but instead were localized near the shore, (2) strong macroalgal emissions of CH2Br2 were almost limited to the summer, but it was not reflected in the seasonality of the baseline concentrations of CH2Br2 in the atmosphere, and therefore (3) macroalgal or coastal emissions of CH2Br2 in the temperate zone might have a rather limited contribution to the global CH2Br2 sources. These findings are especially important for the understanding of the tropospheric and stratospheric bromine budget.  相似文献   

13.
In order to investigate the different thermodynamic mechanisms between rapid intensifying (RI) and rapid weakening (RW) tropical cyclones (TCs), the thermodynamic structures of two sets of composite TCs are analyzed based on the complete-form vertical vorticity tendency equation and the NCEP/NCAR reanalysis data. Each composite is composed of five TCs, whose intensities change rapidly over the coastal waters of China. The results show that the maximum apparent heating source Q 1 exists in both the upper and lower troposphere near the RI TC center, and Q 1 gets stronger at the lower level during the TC intensification period. But for the RW TC, the maximum Q 1 exists at the middle level near the TC center, and Q 1 gets weaker while the TC weakens. The maximum apparent moisture sink Q 2 lies in the mid troposphere. Q 2 becomes stronger and its peak-value height rises while TC intensifies, and vice versa. The increase of diabatic heating with height near the TC center in the mid-upper troposphere and the increase of vertical inhomogeneous heating near the TC center in the lower troposphere are both favorable to the TCs’ rapid intensification; otherwise, the intensity of the TC decreases rapidly.  相似文献   

14.
利用星载微波临边遥感探测结果,对2006年6月28~29日江淮地区的一次强对流天气过程中对流层上部一氧化碳 (CO) 、臭氧 (O3) 、水汽 (H2O) 和冰水含量 (IWC) 的分布特点进行了研究.强对流天气过程前后的对比分析表明,CO混合比增大,在200 hPa处增加了0.12 ppm (1 ppm=10-6);O3混合比减小,在70 hPa处减少了0.30 ppm;H2O混合比在250 hPa处增加了400 ppm;IWC在强降水发生之前有大幅增长,在200 hPa处最大含量可达0.03 g/m3.CO和O3含量与垂直运动速度两者的相关变化表明,对流垂直输送作用可能是造成对流层上层和平流层低层大气成分变化的机制之一.而H2O和IWC含量的增加主要局限于对流层顶以下,这表明对流层上部水物质的质量和形态是由垂直输送作用和对流系统内部的微物理过程共同决定的.  相似文献   

15.
Abstract

Arctic haze has been attributed to industrial pollution released at mid‐latitudes. Our current understanding has been pieced together from routine meteorological data, ground‐based air chemistry observations and limited aircraft measurements. This study investigates the relationship between synoptic boundary‐layer meteorology and the composition of the near‐surface atmosphere during the polar sunrise at Alert, N.W.T. A secondary objective is to characterize the influence of local activity on the atmospheric composition at a site for a new baseline monitoring station and at a location where aerosol chemistry and grab‐flask samples for CO2 have been made for many years. Detailed measurements of the vertical distribution of aerosols were obtained from an upward‐looking lidar to complement the ground‐based measurements. Meteorological profiles of the near‐surface boundary layer were obtained from both free‐flying and tethered balloons. Near‐surface measurements were made of aerosol physical and chemical properties, O3, NO2, NO/NOx, Peroxyacetylnitrate (PAN) and hydrocarbons.

The study period was characterized by prolonged periods with strong surface inversions, which were broken up occasionally by intrusions of cold air into the warmer air aloft. Lidar observations showed that ice crystals often accompanied aerosols and were responsible for reducing visibility below 30–40 km. There was a strong correlation between aerosol mass in the diameter size range 0.15 to 1.5 μm and total SO4 = . PAN found at concentrations of about 200 ppt(v) was the main carrier of atmospheric nitrogen. Aerosol trace elements were divisible into anthropogenic soil, mixed soil/anthropogenic sea salt and halogens. Vertical transport in the surface boundary layer, as regulated by the strength of the surface radiation inversion, may play an important role in influencing the chemical composition of the air at the ground. The location of the new baseline monitoring laboratory was found to be generally windier and warmer than the lower altitude weather station, and the influence of local activity was found to be minimal.  相似文献   

16.
The paper presents a coupled chemical-radiative one-dimensional model which is used to assess the steady-state and time-dependent composition and temperature changes in relation to the release in the atmosphere of chemicals such as CO2, N2O, CH4, NO x and chlorofluorocarbons.The model indicates that a doubling in CO2 leads to an increase in temperature of 12.7 K near the stratopause and to an increase in total ozone of 3.3% with a local enhancement of 17% at 40 km altitude. Additional release of N2O leads to an ozone reduction in the middle stratosphere. The reduction in the ozone column is predicted to be equal to 8.8% when the amount of N2O is doubled. The chemical effect of CH4 on ozone is particularly important in the troposphere. A doubling in the mixing ratio of this gas enhances the O3 concentration by 11% at 5 km. The predicted increase of the ozone column is equal to 1.4%. A constant emission of CFCl3 (230 kT/yr) and CF2Cl2 (300 kT/yr) leads to a steady-state reduction in the ozone column of 1.9% compared to the present-day situation. The effect of some uncertainties in the chemical scheme as well as the impact of a high chlorine perturbation are briefly discussed.Finally the results of a time dependent calculation assuming a realistic scenario for the emission of chemical species are presented and analyzed.  相似文献   

17.
Peroxyacetyl nitrate (PAN,CH3C(O)O2NO2) has been measured inthe polluted boundary layer and free troposphere by thermal conversion tonitrogen dioxide (NO2) followed by detection of thedecomposition product with a Scintrex LMA-3 NO2-luminolinstrument. Following laboratory tests of the efficiency of PAN conversionand investigations of possible interferences, the technique was evaluated atthe West Beckham TOR (Tropospheric Ozone Research) Station near the northNorfolk coast in Eastern England between September 1989 and August 1990. PANmeasured by the new technique was reasonably well correlated with PANrecorded using electron capture gas chromatography (EC/GC). PAN was alsowell correlated with ozone (O3) in the summer months. Springand autumn episodes of simultaneously high concentrations of PAN andO3 were examined in conjunction with air parcelback-trajectories and synoptic- and local-scale meteorology in a study ofthe sources of photooxidants on the east coast of England. Spring-timemeasurements of PAN made in the free troposphere in a light aircraft ataltitudes up to 3.1 km showed the presence of 0.54 and 0.26 ppbv PAN inpolar maritime and mid-latitude oceanic air masses, respectively. Thetechnique is particularly suited to airborne applications because potentialinterferences are minimised and the frequency of measurements is higher thangenerally achieved with EC/GC methods.  相似文献   

18.
Ground-based FTIR measurements have been performed in the Arctic summer in July 1993 and June 1994 at 79° N to study the zenith column densities of several trace gases in the undisturbed Arctic summer atmosphere. Zenith column densities of H2O, N2O, HNO3, NO2, NO, ClONO2, ClO, HCl, HF, COF2, OCS, SF6, HCN, CH4, C2H6, C2H2, CO, O3, CFC-12, CFC-22, and CO2 were retrieved by line-by-line calculations. The results are compared with winter and springtime observations measured at the same site, with column densities obtained in the Antarctic summer atmosphere, and with measurements at midlatitudes. For HCl the spectra give lower total zenith columns than expected, but the ratio HF/HCl agrees well with midlatitude literature data. Measurements of ClONO2 give low total columns in agreement with observations at midlatitudes. In the undisturbed atmosphere HCl was found to be in excess of ClONO2. The total columns of HNO3, N2O and the sum of NO and NO2 agree with summer observations in Antarctica. Results for the tropospheric trace gas C2H6 are higher by 250% when compared with Antarctic observations. Contrary to N2O and CH4 the seasonal cycle of C2H6 and C2H2 give much higher total columns in winter/spring compared to the summer observations. This is assigned to transport of polluted airmasses from mid-latitudes into the Arctic.  相似文献   

19.
Series of high-resolution infrared solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, between 06/1986 and 11/1992, and at Kitt Peak National Observatory, Tucson, Arizona (U.S.A.), from 12/1980 to 04/1992, have been analyzed to provide a comprehensive ensemble of vertical column abundances of CHCIF2 (HCFC-22; Freon-22) above the European and the North American continents. The columns were derived from nonlinear least-squares curve fittings between synthetic spectra and the observations containing the unresolved 2v 6 Q-branch absorption of CHCIF2 at 829.05 cm–1. The changes versus time observed in these columns were modeled assuming both an exponential and a linear increase with time. The exponential rates of increase at one-sigma uncertainties were found equal to (7.0±0.35)%/yr for the Junfraujoch data and (7.0±0.23)%/yr for the Kitt Peak data. The exponential trend of 7.0%/yr found at both stations widely separated in location can be considered as representative of the global increase of the CHCIF2 burden in the Earth's atmosphere during the period 1980 to 1992. When assuming two realistic vertical volume mixing ratio profiles for CHCIF2 in the troposphere, one quasi constant and the other decreasing by about 13% from the ground to the tropopause, the concentrations for mid-1990 were found to lie between 97 and 111 pptv (parts per trillion by volume) at the 3.58 km altitude of the Jungfraujoch and between 97 and 103 pptv at Kitt Peak, 2.09 km above sea level. Corresponding values derived from calculations using a high vertical resolution-2D model and recently compiled HCFC-22 releases to the atmosphere, were equal to 107 and 105 pptv, respectively, in excellent agreement with the measurements. The model calculated lifetime of CHCIF2 was found equal to 15.6 years. The present results are compared critically with similar data found in the literature. On average, the concentrations found here are lower by 15–20% than those derived from in situ investigations; this difference cannot be explained by the absolute uncertainty of ±11% assigned presently to the infrared remote measurements.  相似文献   

20.
A global two-dimensional chemistry model is developed to study long-term trends of CH4 since industrial revolution.The sources of CH4,CO and NOx are parameterized as functions of latitude and time.With two long-term emission scenarios,long-term trends of CH4 are simulated.The results have a good agreement with observation from ice cores.The modeled CH4 increased from 760 ppbv in 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OH decreased from 7.17×105 cm-3 in 1840 to 5.79×105 cm-3 in 1991.The increase of atmospheric CH4 can be explained by the increase of emission of CH4 and build-up because of decrease of OH radicals that remove CH4 from the atmosphere.The model is also used to simulate the distribution of CH4.Comparisons between the model results and observations show that the model can simulate both latitudinal distribution and seasonal variation of CH4 well.  相似文献   

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