青藏高原大气甲烷浓度时空分布变化特征

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。     

Impacts of Global Emissions of CO, NOx, and CH4 on China Tropospheric Hydroxyl Free Radicals

Using the global chemistry and transport model MOZART,the simulated distributions of tropospheric hydroxyl free radicals(OH) over China and its sensitivities to global emissions of carbon monoxide(CO),nitrogen oxide(NO x),and methane(CH 4) were investigated in this study.Due to various distributions of OH sources and sinks,the concentrations of tropospheric OH in east China are much greater than in west China.The contribution of NO + perhydroxyl radical(HO 2) reaction to OH production in east China is more pronounced than that in west China,and because of the higher reaction activity of non-methane volatile organic compounds(NMVOCs),the contributions to OH loss by NMVOCs exceed those of CO and take the dominant position in summer.The results of the sensitivity runs show a significant increase of tropospheric OH in east China from 1990 to 2000,and the trend continues.The positive effect of double emissions of NO x on OH is partly offset by the contrary effect of increased CO and CH 4 emissions:the double emissions of NO x will cause an increase of OH of 18.1%-30.1%,while the increases of CO and CH 4 will cause a decrease of OH of 12.2%-20.8% and 0.3%-3.0%,respectively.In turn,the lifetimes of CH 4,CO,and NO x will increase by 0.3%-3.1% with regard to double emissions of CH 4,13.9%-26.3% to double emissions of CO and decrease by 15.3%-23.2% to double emissions of NO x.     

Measurements of tropospheric OH concentrations: A comparison of field data with model predictions

Using long path UV absorption spectroscopy we have measured OH concentrations close to the earth's surface. The OH values observed at two locations in Germany during 1980 through 1983 range from 0.7×10⁶ to 3.2×10⁶ cm^-3. Simultaneously we measured the concentrations of O₃, H₂O, NO, NO₂, CH₄, CO, and the light non methane hydrocarbons. We also determined the photolysis rates of O₃ and NO₂. This allows calculations of OH using a zero dimensional time depdendent model. The modelled OH concentrations significantly exceed the measured values for low NO _x concentrations. It is argued that additional, so far unidentified. HO _x loss reactions must be responsible for that discrepancy.     

NUMERICAL SIMULATION OF ATMOSPHERIC METHANE TRENDS OVER THE LAST 150 YEARS*

A global two-dimensional chemistry model is developed to study long-term trends of CH₄ since industrial revolution.The sources of CH₄,CO and NO_x 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.     

World-wide increase in tropospheric methane, 1978–1983

Tropospheric concentrations of methane in remote locations have averaged a yearly world-wide increase of 0.018±0.002 parts per million by volume (ppmv) during the period from January 1978 to December 1983. The concentrations in the north temperate zone are always greater than those in the south temperate zone by 7±1% because the major methane sources are all predominantly located in the northern hemisphere. The average world-wide tropospheric concentration of methane in dry air was 1.625 ppmv at the end of 1983, measured against an NBS standard certified as 0.97 ppmv (but with an accuracy of only ±1%). The world-wide concentration increases are described by a linear equation with a standard deviation of 0.003 ppmv for ten different collection periods during 1978–1983. The precision of measurement of the methane concentration in the atmospheric samples and in the standard was measured to be ±0.4% for each. Repetitive measurements of an air sample collected in November 1977 have shown the same concentration for six years with a standard deviation for these data of ±0.003 ppmv.The causes for the steady increase in methane concentration in the troposphere cannot be fixed with certainty from present data. Contributing causes can include increases in the source strengths from cattle and rice fields. The atmospheric concentrations of CO, CH₄ and HO are all closely coupled with one another, and increased concentrations of CO and/or CH₄ should cause reduced concentrations of HO, which in turn should lengthen the atmospheric lifetimes of CO and CH₄.Among other physical and chemical effects, a increase of 0.18 ppmv per decade should contribute a greenhouse warming of about 0.04°C per decade. Other secondary contributions to the greenhouse effect from increases in CH₄ may arise from methane-induced increases in stratospheric H₂O, in tropospheric O₃, and in numerous other trace species whose concentration is controlled by reaction with HO radicals.An increased CH₄ source strength may result from the effect of increasing atmospheric temperatures on the known aqueous biological CH₄ sources, such as swamps, and may be an added consequence of the greenhouse effect.     

Tropospheric chemical composition measurements in Brazil during the dry season

Field measurement programs in Brazil during the dry seasons in August and September 1979 and 1980 have demonstrated the large importance of the continental tropics in global air chemistry. Many important trace gases are produced in large amounts over the continents. During the dry season, much biomass burning takes place, especially in the cerrado regions, leading to a substantial emission of air pollutants, such as CO, NO _x , N₂O, CH₄ and other hydrocarbons. Ozone concentrations are enhanced due to photochemical reactions. The large biogenic organic emissions from tropical forests play an important role in the photochemistry of the atmosphere and explain why CO is present in such high concentrations in the boundary layer of the tropical forest. Carbon monoxide production may represent more than 3% of the net primary productivity of the tropical forests. Ozone concentrations in the boundary layer of the tropical forests indicate strong removal processes. Due to atmospheric supply of NO _x by lightning, there is probably a large production of O₃ in the free troposphere over the Amazon tropical forests. This is transported to the marine-free troposphere and to the forest boundary layer.     

Variational data assimilation in the tropics using precipitation data part I: Column model

Summary This paper describes initial effort in the development of a four-dimensional variational data assimilation (4D-Var) in the tropics using precipitation data derived from remote sensing. The method of 4D-Var using precipitation data is formulated, and modifications to the parameterization schemes of moist processes to remove zeroth-order discontinuities are described. Variational data assimilation experiments are carried out using a column model to investigate the problems caused by discontinuities in parameterization schemes and assess the impact of assimilating precipitation data in the tropics.It is found that variational data assimilation with discontinuous parameterization schemes exhibits large fluctuations during the minimization process, slow convergence rates, and large analysis errors. The fluctuations become much more serious when precipitation data is assimilated. Precipitation data is very useful to estimate divergence in the tropics, provided that the temporal resolution of the data is sufficiently high. However, its impact on the analysis of temperature and moisture is not clear in the column model assimilation experiments, possibly due to the absence of horizontal advection.     

Formulation and Evaluation of IMS, an Interactive Three-Dimensional Tropospheric Chemical Transport Model 2. Model Chemistry and Comparison of Modelled CH4, CO, and O3 with Surface Measurements

In part two of this series of papers on the IMS model, we present the chemistry reaction mechanism usedand compare modelled CH₄, CO, and O₃ witha dataset of annual surface measurements. The modelled monthly and 24-hour mean tropospheric OH concentrationsrange between 5–22 × 10⁵ moleculescm^–3, indicating an annualaveraged OH concentration of about 10 × 10⁵ moleculescm^–3. This valueis close to the estimated 9.7 ± 0.6 × 10⁵ moleculescm^–3 calculated fromthe reaction of CH₃CCl₃ with OH radicals.Comparison with CH₄ generally shows good agreementbetween model and measurements, except for the site at Barrow where modelledwetland emission in the summer could be a factor 3 too high.For CO, the pronounced seasonality shown in the measurements is generally reproduced by the model; however, the modelled concentrations are lower thanthe measurements. This discrepancy may due to lower the CO emission,especially from biomass burning,used in the model compared with other studies.For O₃, good agreement between the model and measurements is seenat locations which are away from industrial regions. The maximum discrepancies between modelled results and measurementsat tropical and remote marine sites is about 5–10 ppbv,while the discrepancies canexceed 30 ppbv in the industrial regions.Comparisons in rural areas at European and American continental sites arehighly influenced by the local photochemicalproduction, which is difficult to model with a coarse global CTM.The very large variations of O₃ at these locations vary from about15–25 ppbv in Januaryto 55–65 ppbv in July–August. The observed annual O₃amplitude isabout 40 ppbv compared with about 20 ppbv in the model. An overall comparison of modelled O₃ with measurements shows thatthe O₃seasonal surface cycle is generally governed bythe relative importance of two key mechanisms that drivea springtime ozone maximum and asummertime ozone maximum.     

DRP-4DVar方法同化AIRS反演资料在一次江淮流域暴雨中的应用

利用经济省时的降维投影四维变分同化方法(DRP-4DVar),在2009年7月22～23日江淮流域的一次大暴雨过程中同化晴空条件下高光谱大气红外探测仪(AIRS)反演温度、湿度廓线,改进此次强降水过程的模拟。试验结果分析显示,同化AIRS反演的温度及湿度场后,基于四维变分同化系统的模式约束,能够改进湿度场、高度场、高低层散度场。从累积降水量偏差图及同化试验增量图可以看到,正降水量偏差对应于正湿度增量、负位势高度增量及低层负散度高层正散度增量,负降水量偏差则与之相反。同化试验较参照试验可更好地模拟出暴雨的天气形势、对暴雨的落区及强度有更好的反映。此外,从单次同化与连续同化的试验对比结果看出,连续同化试验结果较单次同化结果有进一步的改进,说明不断加入新的观测资料可以更好地模拟强降水过程。     

中国区域性极端降水事件及人口经济暴露度研究

This paper tests the idea of substituting the atmospheric observations with atmospheric reanalysis when setting up a coupled data assimilation system.The paper focuses on the quantification of the effects on the oceanic analysis resulted from this substitution and designs four different assimilation schemes for such a substitution.A coupled Lorenz96 system is constructed and an ensemble Kalman filter is adopted.The atmospheric reanalysis and oceanic observations are assimilated into the system and the analysis quality is compared to a benchmark experiment where both atmospheric and oceanic observations are assimilated.Four schemes are designed for assimilating the reanalysis and they differ in the generation of the perturbed observation ensemble and the representation of the error covariance matrix.The results show that when the reanalysis is assimilated directly as independent observations,the root-mean-square error increase of oceanic analysis relative to the benchmark is less than 16%in the perfect model framework;in the biased model case,the increase is less than 22%.This result is robust with sufficient ensemble size and reasonable atmospheric observation quality(e.g.,frequency,noisiness,and density).If the observation is overly noisy,infrequent,sparse,or the ensemble size is insufficiently small,the analysis deterioration caused by the substitution is less severe since the analysis quality of the benchmark also deteriorates significantly due to worse observations and undersampling.The results from different assimilation schemes highlight the importance of two factors:accurate representation of the error covariance of the reanalysis and the temporal coherence along each ensemble member,which are crucial for the analysis quality of the substitution experiment.     

Analysis of Air Quality in Eastern China and its Interaction with Other Regions of the World

In this study, we used satellite data (GOME and MOPITT) together with a global chemical-transport-model of atmosphere (MOZART-2) to characterize the chemical/aerosol composition over eastern China. We then estimated the effects of local emissions in China on the chemical budgets in other regions of the world. Likewise, we also investigated the effects of air pollution from other regions on the chemical budget over eastern China. The study shows that the column CO and NO _x concentrations are also high in eastern China. The high CO and NO _x concentrations produce modest levels of O₃ concentrations during summer (about 40 to 50 ppbv) and very low O₃ during winter (about 10 to 20 ppbv) in eastern China. The calculated NO₂ column is fairly consistent from the GOME measurement. The calculated CO column is underestimated from the MOPITT measurement. One of the reasons of the underestimation of the predicted CO is due to a fact that the CO emissions were taken without considering the rapid increase of emissions from 1990 to 2000. The calculated surface O₃ is consistent with the measured values, with strong seasonal variations. However, the measurement is very limited, and more measurements in eastern China will be needed. The column NO₂ has a very strong seasonal variation in eastern China, with the highest concentrations during winter and the lowest concentrations during summer. The cause of this seasonal variability is mainly due to the seasonal changes in the chemical loss of NO _x , which is very high in summer and very low during winter. The effects of the local emissions in China and long-range transport from other regions on the chemical distributions in eastern China are studied. The results show that NO _x concentrations in eastern China are mostly caused by the local emissions in China, especially during the winter. The CO concentration over eastern China is from both the local emissions (30% to 40%) and the transport from other regions. Likewise, the CO emissions in China have an important effect on the other regions of the world, but the effect is limited in the northern hemisphere. The local emissions in China also have an important effect on surface O₃ concentrations. During winter, the local emissions reduce the surface O₃ concentrations by 30 to 50%. During summer, the local emissions produce about 50 to 70% of the O₃ concentration in eastern China.     

Environmental process and convergence belt of atmospheric NO2 pollution in North China

Both surface environmental monitoring and satellite remote sensing show that North China is one of the regions that are heavily polluted by NO₂. Using the NO₂ monitoring data from 18 major cities in the region, the tropospheric NO₂ column density data from the Ozone Monitoring Instrument (OMI) on the Aura satellite, and the observations from the China Meteorological Administration network, this paper analyzes a regional NO₂ pollution event in February 2007 over North China, examines the convergence of the pollutant, and identies its correlation with the atmospheric background conditions. The results show that daily mean NO₂ concentrations derived from surface observations are consistent with the mean values of the OMI measurements, with their correlation coeficient reaching 0.81. The correlations of NO₂ concentration with general weather patterns and sequential changes of temperature structure from 925 hPa down to the surface indicate that the weather fronts, high pressure and low pressure systems in the atmosphere play a role in changing the temporal and spatial evolutions of NO₂ through removing, accumulating or converging of the pollutant, respectively. It is also found that the eastern Taihang Mountains is most heavily polluted by NO₂ in North China. Based on a model that correlates NO₂ column density with surface wind vector, the relation of the NO₂ concentrations in six major cities in North China to the surrounding wind field is analyzed. The results show that the maximum wind field is associated with the highest frequency of pollution events, and under certain large-scale atmospheric conditions together with the topographic effect, small- and meso-scale wind fields often act to transport and converge pollutants, and become a major factor in forming the heaviest NO₂ pollution event in North China. Analysis of the causes for the severe NO₂ pollution event in this study may shed light on understanding, forecasting, and mitigating occurrences of heavy NO₂ pollution.     

ENSO in a hybrid coupled model. Part II: prediction with piggyback data assimilation

A hybrid coupled model (HCM) for the tropical Pacific ocean-atmosphere system is employed for ENSO prediction. The HCM consists of the Geophysical Fluid Dynamics Laboratory ocean general circulation model and an empirical atmospheric model. In hindcast experiments, a correlation skill competitive to other prediction models is obtained, so we use this system to examine the effects of several initialization schemes on ENSO prediction. Initialization with wind stress data and initialization with wind stress reconstructed from SST using the atmospheric model give comparable skill levels. In re-estimating the atmospheric model in order to prevent hindcast-period wind information from entering through empirical atmospheric model, we note some sensitivity to the estimation data set, but this is considered to have limited impact for ENSO prediction purposes. Examination of subsurface heat content anomalies in these cases and a case forced only by the difference between observed and reconstructed winds suggests that at the current level of prediction skill, the crucial wind components for initialization are those associated with the slow ENSO mode, rather than with atmospheric internal variability. A “piggyback” suboptimal data assimilation is tested in which the Climate Prediction Center data assimilation product from a related ocean model is used to correct the ocean initial thermal field. This yields improved skill, suggesting that not all ENSO prediction systems need to invest in costly data assimilation efforts, provided the prediction and assimilation models are sufficiently close. Received: 17 April 1998 / Accepted: 22 July 1999     

Methane,carbon monoxide and methylchloroform in the southern hemisphere

New observational data on CH₄, CO and CH₃CCl₃ in the southern hemisphere are reported. The data are analysed for long term trends and seasonal cycles. CH₃CCl₃ data are used to scale the OH fields incorporated in a two dimensional model, which in turn, is used to constrain the magnitude of a global CH₄ source function. The possible causes of observed seasonality of CH₃CCl₃, CH₄ and CO are identified, and several other aspects of observed CH₄ variability are discussed.Possible future research directions are also given.     

Assimilating Best Track Minimum Sea Level Pressure Data Together with Doppler Radar Data Using an Ensemble Kalman Filter for Hurricane Ike (2008) at a Cloud-Resolving Resolution

Extending an earlier study, the best track minimum sea level pressure (MSLP) data are assimilated for landfalling Hurricane Ike (2008) using an ensemble Kalman filter (EnKF), in addition to data from two coastal ground-based Doppler radars, at a 4-km grid spacing. Treated as a sea level pressure observation, the MSLP assimilation by the EnKF enhances the hurricane warm core structure and results in a stronger and deeper analyzed vortex than that in the GFS (Global Forecast System) analysis; it also improves the subsequent 18-h hurricane intensity and track forecasts. With a 2-h total assimilation window length, the assimilation of MSLP data interpolated to 10-min intervals results in more balanced analyses with smaller subsequent forecast error growth and better intensity and track forecasts than when the data are assimilated every 60 minutes. Radar data are always assimilated at 10-min intervals. For both intensity and track forecasts, assimilating MSLP only outperforms assimilating radar reflectivity (Z) only. For intensity forecast, assimilating MSLP at 10-min intervals outperforms radar radial wind (Vr) data (assimilated at 10-min intervals), but assimilating MSLP at 60-min intervals fails to beat Vr data. For track forecast, MSLP assimilation has a slightly (noticeably) larger positive impact than Vr(Z) data. When Vr or Z is combined with MSLP, both intensity and track forecasts are improved more than the assimilation of individual observation type. When the total assimilation window length is reduced to 1h or less, the assimilation of MSLP alone even at 10-min intervals produces poorer 18-h intensity forecasts than assimilating Vr only, indicating that many assimilation cycles are needed to establish balanced analyses when MSLP data alone are assimilated; this is due to the very limited pieces of information that MSLP data provide.     

Near UV absorption spectra and photolysis products of difunctional organic nitrates: Possible importance as NO x reservoirs

Difunctional organic nitrates are important products of the atmospheric reaction of NO₃ radicals with unsaturated hydrocarbons about which relatively little is known. In a continuation of the investigation of the atmospheric chemistry of such compounds, the UV absorption spectra of the following organic dinitrates and keto nitrates have been quantitively measured in the gas phase at 298±2 K and atmospheric pressure: 1,2-propandiol dinitrate, CH₃CH(ONO₂)CH₂(ONO₂); 1,2-butandiol dinitrate, CH₃CH₂CH(ONO₂)CH₂(ONO₂); 2,3-butandiol dinitrate, CH₃CH(ONO₂)CH(ONO₂)CH₃;cis 1,4-dinitrooxy-2-butene, CH₂(ONO₂)CH=CHCH₂(ONO₂); 3,4-dinitrooxy-1-butene, CH₂(ONO₂CH(ONO₂)CH=CH₂; -nitrooxy acetone, CH₃COCH₂(ONO₂); 1-nitrooxy-2-butanone, CH₃CH₂COCH₂(ONO₂); 3-nitrooxy-2-butanone, CH₃CH(ONO₂)COCH₃.Although the UV spectra of the nitrates are all very similar in shape those of the keto nitrates are red-shifted compared to the dinitrates and in the spectral range of atmospheric interest (>290 nm) their absorption cross-sections are approximately a factor of 5 higher. The cross-sections of the dinitrates are a factor of 2 higher than those reported in the literature for the corresponding alkyl mononitrates.The UV absorption cross-sections of the difunctional nitrates were used in combination with solar actinic flux data to estimate photolysis frequencies and consequently atmospheric lifetimes for these compounds. The results indicate that for the saturated difunctional nitrates studied in this work photolysis will generally be somewhat some important than reaction with OH radicals as an atmospheric removal process. However, for unsaturated nitrates loss due to reaction with OH will dominate over photolysis as an atmospheric sink.Preliminary FT-IR analyses of the photolysis products of -nitrooxy acetone, 3-nitrooxy-2-butanone and 2,3-butandiol dinitrate using both mercury and fluorescent lamps indicate that NO₂ is released in the primary step. The further reactions of the radicals thus produced result in the formation of CO, aldehydes and PAN. The possible significance of the results for difunctional organic nitrate as reservoirs for reactive odd nitrogen NO _y in the atmosphere, especially during the night, is briefly discussed.     

Modeling the concentration of pollutants using the WRF-ARW atmospheric model and CHIMERE chemistry transport model

Described is a system for analyzing and forecasting the air quality in the central regions of Russia, During the operation of the system, the detailed meteorological information provided by the WRF-ARW model is used by the CHIMERE chemistry transport model for simulating the processes of transport, chemical transformation, and deposition of atmospheric minor constituents. Considered is the quality of retrieved and forecasted (with the lead time up to three days) concentrations of O₃, NO₂, NO, CO, and PM₁₀. The presented verification scores of pollutant concentrations demonstrate a relative success of the system. Demonstrated is a need in improving the data on the emissions of the air pollutants used for simulations. A procedure for the statistical correction of computed concentrations is described and verification scores of its results are given.     

Effect of HITRAN Database Improvement on Retrievals of Atmospheric Carbon Dioxide from Reflected Sunlight Spectra in the 1.61-μm Spectral Window

A large number of experimental and theoretical investigations of carbon dioxide (CO2) spectra have been conducted since the most recent update of the High-Resolution Transmission Molecular Absorption (...     

Estimates of indirect global warming potentials for CH4, CO and NOX

Emissions may affect climate indirectly through chemical interactions in the atmosphere, but quantifications of such effects are difficult and uncertain due to incomplete knowledge and inadequate methods. A preliminary assessment of the climatic impact of changes in tropospheric O₃ and CH₄ in response to various emissions is given. For a 10% increase in the CH₄ emissions the relative increase in concentration has been estimated to be 37% larger. The radiative forcing from enhanced levels of tropospheric O₃ is estimated to 37% of the forcing from changes in CH₄. Inclusion of indirect effects approximately doubles the climatic impact of CH₄ emissions. Emissions of NO_x increase tropospheric O₃, while the levels of CH₄ are reduced. For emissions of NO_x from aircraft, the positive effects via O₃ changes are significantly larger than the negative through changes in CH₄. For NO_x emitted from surface sources, the effects through changes in O₃ and CH₄ are estimated to be of similar magnitude and large uncertainty is connected to the sign of the net effect. Emissions of CO have positive indirect effects on climate through enhanced levels of tropospheric o₃ and increased lifetime of CH₄. These results form the basis for estimates of global warming potentials for sustained step increases in emissions.