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1.
We suggest a one-dimensional model of precipitation scavenging of soluble gaseous pollutants by non-evaporating and evaporating droplets that is valid for arbitrary initial vertical distribution of soluble trace gases in the atmosphere. It is shown that for low gradients of soluble trace gases in the atmosphere, scavenging of gaseous pollutants is governed by a linear wave equation that describes propagation of a wave in one direction. The derived equation is solved by the method of characteristics. Scavenging coefficient and the rates of precipitation scavenging are calculated for wet removal of sulfur dioxide (SO2) and ammonia (NH3) using measured initial distributions of trace gases. It is shown that scavenging coefficient for arbitrary initial vertical distribution of soluble trace gases in the atmosphere is non-stationary and height-dependent. In case of exponential initial distribution of soluble trace gases in the atmosphere, scavenging coefficient for non-evaporating droplets in the region between the ground and the position of a scavenging front is a product of rainfall rate, solubility parameter, and the growth constant in the formula for the initial profile of a soluble trace gas in the atmosphere. This expression yields the same estimate of scavenging coefficient for sulfur dioxide scavenging by rain as field estimates presented in McMahon and Denison (1979). It is demonstrated that the smaller the slope of the concentration profile the higher the value of a scavenging coefficient.  相似文献   

2.
Theoretical models that describe the uptake of trace gases by water drops falling at terminal velocity in air have been extended to include the effects of aqueous phase chemical processes that occur on time scales comparable with or greater than that over which the relevant physical scavenging processes operate. In particular, the case of reversible dervative formation by the absorbed species has been treated, and illustrated by application to the absorption of acetaldehyde under conditions prevailing in the atmosphere. In addition, the relative influences of aqueous phase chemistry and of convective-diffusion on the efficiency of the scavenging process have been explored more generally, using the revised models. A brief comparison of the factors controlling the uptake of sulfur dioxide, dichloromethane, and acetaldehyde is presented.  相似文献   

3.
Transport of trace gases within the gas phase to a cloud or a sulphate aerosol droplet proceeds by molecular diffusion at the gas-liquid interface. An accurate determination of the molecular diffusion coefficient has a direct bearing on estimates of trace gas uptake and scavenging. A literature search revealed that this parameter is often chosen rather arbitrarily and the choice of a particular value is constrained by the availability of experimental data which are usually available at one atmospheric pressure under laboratory conditions. Since the process of trace gas transport to droplets occur at heights much above the ground level, it is important to determine an accurate value of the diffusion coefficient at varying levels in the atmosphere. This was achieved theoretically by estimating diffusivities for some important trace gases under stratospheric conditions by a Lennard-Jones method. Molecular diffusivity of 22 trace gases (including ClONO2, HNO3, SO2 and H2O2 which may lead to heterogeneous reactions on various surfaces) have been estimated which can be used by modellers for improved scavenging estimates.  相似文献   

4.
A new approach is proposed to predict concentration fluctuations in the framework of one-particle Lagrangian stochastic models. The approach is innovative since it allows the computation of concentration fluctuations in dispersing plumes using a Lagrangian one-particle model with micromixing but with no need for the simulating of background particles. The extension of the model for the treatment of chemically reactive plumes is also accomplished and allows the computation of plume-related chemical reactions in a Lagrangian one-particle framework separately from the background chemical reactions, accounting for the effect of concentration fluctuations on chemical reactions in a general, albeit approximate, manner. These characteristics should make the proposed approach an ideal tool for plume-in-grid calculations in chemistry transport models. The results are compared to the wind-tunnel experiments of Fackrell and Robins (J Fluid Mech, 117:1–26, 1982) for plume dispersion in a neutral boundary layer and to the measurements of Legg et al. (Boundary-Layer Meteorol, 35:277–302, 1986) for line source dispersion in and above a model canopy. Preliminary reacting plume simulations are also shown comparing the model with the experimental results of Brown and Bilger (J Fluid Mech, 312:373–407, 1996; Atmos Environ, 32:611–628, 1998) to demonstrate the feasibility of computing chemical reactions in the proposed framework.  相似文献   

5.
The dynamics of a low-order coupled wind-driven ocean–atmosphere system is investigated with emphasis on its predictability properties. The low-order coupled deterministic system is composed of a baroclinic atmosphere for which 12 dominant dynamical modes are only retained (Charney and Straus in J Atmos Sci 37:1157–1176, 1980) and a wind-driven, quasi-geostrophic and reduced-gravity shallow ocean whose field is truncated to four dominant modes able to reproduce the large scale oceanic gyres (Pierini in J Phys Oceanogr 41:1585–1604, 2011). The two models are coupled through mechanical forcings only. The analysis of its dynamics reveals first that under aperiodic atmospheric forcings only dominant single gyres (clockwise or counterclockwise) appear, while for periodic atmospheric solutions the double gyres emerge. In the present model domain setting context, this feature is related to the level of truncation of the atmospheric fields, as indicated by a preliminary analysis of the impact of higher wavenumber (“synoptic” scale) modes on the development of oceanic gyres. In the latter case, double gyres appear in the presence of a chaotic atmosphere. Second the dynamical quantities characterizing the short-term predictability (Lyapunov exponents, Lyapunov dimension, Kolmogorov–Sinaï (KS) entropy) displays a complex dependence as a function of the key parameters of the system, namely the coupling strength and the external thermal forcing. In particular, the KS-entropy is increasing as a function of the coupling in most of the experiments, implying an increase of the rate of loss of information about the localization of the system on its attractor. Finally the dynamics of the error is explored and indicates, in particular, a rich variety of short term behaviors of the error in the atmosphere depending on the (relative) amplitude of the initial error affecting the ocean, from polynomial (at 2 + bt 3 + ct 4) up to exponential-like evolutions. These features are explained and analyzed in the light of the recent findings on error growth (Nicolis et al. in J Atmos Sci 66:766–778, 2009).  相似文献   

6.
With very few exceptions, just about all limited area models (LAMs) used in operational NWP and regional climate modeling use the Davies (Q J R Meteorol Soc 102:405–418, 1976) relaxation lateral boundary conditions (LBCs), even though they make no effort to respect the basic mathematics of the problem. While in the early stages of the primitive equation LAM development in the seventies numerous schemes have been proposed and tested, LAM communities have eventually for the most part settled on the relaxation LBCs with few questions asked. An exception is the Eta model used extensively at NCEP and several other centers, in which the Mesinger (Contrib Atmos Phys 50:200–210, 1977) LBCs are used, designed and based on knowledge available before the introduction of the relaxation scheme. They prescribe variables along the outermost row of grid points only; all of them at the inflow points and one less at the outflow points where the tangential velocity components are extrapolated from inside of the model domain. Additional schemes are in place to suppress separation of gravity-wave solutions on C-subgrids of the model’s E-grid. A recent paper of Veljovic et al. (Meteor Zeitschrift 19:237–246, 2010) included three 32-day forecasts done with both the Eta and the relaxation LBCs and the comparison of some of their verification results. Here we extend this experiment by three additional forecasts to arrive at an ensemble of six members run with both schemes, and present a more complete discussion of results. We in addition show results of one of these forecasts in which the linear change of relaxation coefficients was replaced by the change following the recommendation of Lehmann (Meteorol Atmos Phys 52:1–14, 1993). We feel that the results of our two verification schemes strongly suggest the advantage of the Eta over the conventional relaxation scheme, thereby raising doubts as to the justification for its use.  相似文献   

7.
We use recent advances in time series econometrics to estimate the relation among emissions of CO2 and CH4, the concentration of these gases, and global surface temperature. These models are estimated and specified to answer two questions; (1) does human activity affect global surface temperature and; (2) does global surface temperature affect the atmospheric concentration of carbon dioxide and/or methane. Regression results provide direct evidence for a statistically meaningful relation between radiative forcing and global surface temperature. A simple model based on these results indicates that greenhouse gases and anthropogenic sulfur emissions are largely responsible for the change in temperature over the last 130 years. The regression results also indicate that increases in surface temperature since 1870 have changed the flow of carbon dioxide to and from the atmosphere in a way that increases its atmospheric concentration. Finally, the regression results for methane hint that higher temperatures may increase its atmospheric concentration, but this effect is not estimated precisely.  相似文献   

8.
Gilles Bellon 《Climate Dynamics》2011,37(5-6):1081-1096
A simple coupled model is used in a zonally-symmetric configuration to investigate the effect of land?Catmosphere coupling on the Asian monsoon intraseasonal oscillation. The atmospheric model is a version of the Quasi-equilibrium Tropical Circulation Model with a prognostic atmospheric boundary layer, as well as two free-tropospheric modes in momentum, and one each in moisture and temperature. The land model is the simple one-layer model SLand. The complete nonlinear version and a linear version of the model are used to understand how land?Catmosphere interaction influences the northward-propagating intraseasonal oscillation that has been documented in the atmospheric model (Bellon and Sobel in J Geophys Res 113, 2008a, J Atmos Sci 65:470?C489, 2008b). Our results show that this interaction damps the intraseasonal variability in most cases. The small heat capacity of land surfaces is the main factor that intervenes directly in the dynamics of the intraseasonal oscillation and explains the damping of intraseasonal variability. But in a few peculiar cases, the small heat capacity of land can also cause a strong interaction between the intraseasonal oscillation and the mean state via the nonlinearity of precipitation, that enhances the monsoon intraseasonal variability. High land albedo indirectly influences the intraseasonal variability by setting the seasonal mean circulation to conditions unfavorable for the monsoon intraseasonal oscillation.  相似文献   

9.
Gary Yohe 《Climatic change》2010,99(1-2):295-302
Article 2 of the United Nations Framework Convention on Climate Change commits its parties to stabilizing greenhouse gas concentrations in the atmosphere at a level that “would prevent dangerous anthropogenic interference with the climate system.” Authors of the Third Assessment Report of the Intergovernmental Panel on Climate Change (IPCC 2001a, b) offered some insight into what negotiators might consider dangerous by highlighting five “reasons for concern” (RFC’s) and tracking concern against changes in global mean temperature; they illustrated their assessments in the now iconic “burning embers” diagram. The Fourth Assessment Report reaffirmed the value of plotting RFC’s against temperature change (IPCC 2007a, b), and Smith et al. (2009) produced an unpated embers visualization for the globe. This paper applies the same assessment and communication strategies to calibrate the comparable RFC’s for the United States. It adds “National Security Concern” as a sixth RFC because many now see changes in the intensity and/or frequency of extreme events around the world as “risk enhancers” that deserve attention at the highest levels of the US policy and research communities. The US embers portrayed here suggest that: (1) US policy-makers will not discover anything really “dangerous” over the near to medium term if they consider only economic impacts that are aggregated across the entire country but that (2) they could easily uncover “dangerous anthropogenic interference with the climate system” by focusing their attention on changes in the intensities, frequencies, and regional distributions of extreme weather events driven by climate change.  相似文献   

10.
The role of trace gases and aerosol particles in the control of sulfur and nitrogen levels in atmospheric precipitation is estimated on the basis of the enrichment factor in the precipitation of these elements relative to particulate matter in the air. By using air and precipitation chemistry data obtained at a Hungarian background air pollution station (K-puszta) it is found that the fraction of ammonium, nitrate and sulfate in precipitation, due to the removal of particulate matter is at least 59, 27 and 31%, respectively. The relationship between wet depositions and air concentrations of different species is determined statistically by applying daily data set. The regression equations obtained make the estimation of the sub-cloud scavenging ratios possible and they give some information on the magnitude of in-cloud scavenging processes. The results show that the in-cloud scavenging is a determining factor for precipitation sulfate, while it is relatively unimportant in the case of ammonium. The sub-cloud scavening of NO2 and SO2 is not too significant. However, for HNO3, and NH3 it is an effective process. The sub-cloud scavenging ratio of sulfur and nitrogen-containing particles varies around 0.25×106.  相似文献   

11.
Lifetimes, scavenging ratios, andbudgets describe the cycling of atmosphericconstituents and are often used in formulating airpollution control strategies. Most previous studiesof sulfur lifetimes, budgets, and scavenging ratioshave been based on limited observational data or datafrom highly simplified models. The Regional AcidDeposition Model (RADM2.61) shows some skill inpredicting atmospheric mixing ratios of acidicmaterials and other related trace constituents andacid deposition patterns in North America, and so,analysis of its established, theoretical, databaseserves as a counterpoint to previous studies of sulfurbudgets, lifetimes, and scavenging ratios. The annualbudget shows that the net transport (outflow minusinflow) of sulfur compounds out of eastern NorthAmerica is equal to the total deposition within thedomain. Of the total deposition, 63% is from wetdeposition and 37% is from dry deposition. Theannual average lifetime of sulfur dioxide (38 hours),estimated by the turnover time, is limited by aqueousconversion, while that for sulfate aerosols (54 hours)is limited by their removal in precipitation. Theannual average lifetime of sulfur in this domain isslightly more than three days. Episodic lifetimes andbudgets, based on particular synoptic situations, showlarge variations around the annual values. Episodicprecipitation scavenging ratios exhibit similarvariability and are used to offer explanations ofseveral potential biases found in the wet sulfurdeposition amounts as predicted by the EMEP sulfurtransport model and other published results.  相似文献   

12.
Laboratory experiments were carried out in the Mainz vertical wind tunnel to determine the retention of the trace gases ammonia and sulfur dioxide dissolved in supercooled cloud droplets during riming. The conditions during riming were similar to the ones in atmospheric mixed phase clouds: temperatures from ?18 °C to ?5 °C, liquid water contents between 1 and 1.5 g m?3, liquid drop radii between 10 and 20 μm, liquid phase concentrations from 1 to 22 mg/l. As collectors, floating ice particles and snow flakes with diameters between 6 mm and 1.5 cm were used. After riming the retention coefficients, i.e. the fractions of the species which remained in the ice phase after freezing were determined. Retention coefficients lying between 0.1 and 1.0 were measured depending on the solubility and dissociation of the trace gas, liquid phase concentration, ambient air temperature, and shape of rimed collector. This can be explained from the chemists’ point of view by the effective Henry’s law constant of the species and physically with the rate of latent heat removal from the rimed collector during freezing. Parameterizations derived from the different experimental cases describe the retention coefficients as a function of temperature. In general, an average retention of ammonia of 92?±?21 % was determined independently of liquid phase concentration while mean values for sulfur dioxide were 53?±?10 % at low liquid phase concentrations and 29?±?7 % at high liquid phase concentrations.  相似文献   

13.
Our previously described absorption model for the scavenging of trace gases by individual cloud and rain drops was applied to an ensemble of drops of given size distribution as found in typical atmospheric rainfalls. This study allowed: (1) determination of the redistribution which a pollution plume suffers as rain falls through it, and (2) determination of the amount of pollutant contained in. the fallen rain. For the present application it was assumed that the pollution plume consisted of SO2, only, and that its concentration varied vertically as a Gaussian distribution centered 200 m above the ground. Rain of various intensities and corresponding drop size distributions was allowed to pass through this pollution layer. The results of our study show that the average height and concentration of the plume decrease in proportion to the total amount of rain which had passed through the pollution layer. The fractional plume washout rate (in % per mm of rain) was found to be inversely proportional to the SO2 gas concentration, the plume height, and the plume thickness. By including the effects of oxidation inside the falling raindrops, it was noted that the removal of SO2 became enhanced by a factor of up to 10 times. For significant oxidation the rate with which SO2 was washed out was found to be inversely proportional to the rainfall rate. For the case of light drizzle (2 mm h-1) and large oxidation rate constants (100 s-1), as much as 40% of the sulfur load could be removed by 1 mm of rain. For the case of a heavier rainfall (25 mm h-1) composed of correspondingly larger drops, the washout rate varied between 2 and 10$ mm-1 over a wide range of oxidation rates.  相似文献   

14.
The Arrhenius expressions and the data plotted in Figure 2 of Rodriguez et al. 2008 give rate coefficients of approximately 2?×?10-8 cm3 molecule-1 s-1 at 255 K. Such values are approximately two orders of magnitude larger than expected from simple collision theory (Finlayson-Pitts and Pitts 1986). The rate coefficients reported at sub-ambient temperatures are substantially greater than the gas kinetic limit and are not physically plausible. The rate coefficients reported by Rodriguez et al. imply a long range attraction between the reactants which is not reasonable for reaction of neutral species such as chlorine atoms and unsaturated alcohols. We also note that the pre-exponential A factors (10-23-10-20) and activation energies (?15 kcal mol-1) are not physically plausible. We conclude that there are large systematic errors in the study by Rodriguez et al. (Atmos Chem 59:187–197, 2008).  相似文献   

15.
对流层臭氧的数值模拟试验   总被引：2，自引：0，他引：2       下载免费PDF全文
建立一个一维大气化学模式、利用该模式模拟O3等微量气体的日变化和O3的一些敏感性试验。结果表明:CH4和CO的增加会使O3增加，水汽增加将使O3减少；温度升高使自由大气中O3减少，而使边界层中O3增加；太阳辐射的加强使自由大气中的O3减少，边界层中O3增加。最后，研究了边界层结构对大气微量气体分布的影响。结果表明，模拟低层大气微量气体的变化需要考虑边界层结构的影响。  相似文献   

16.
We present further steps in our analysis of the early anthropogenic hypothesis (Ruddiman, Clim Change 61:261–293, 2003) that increased levels of greenhouse gases in the current interglacial, compared to lower levels in previous interglacials, were initiated by early agricultural activities, and that these increases caused a warming of climate long before the industrial era (～1750). These steps include updating observations of greenhouse gas and climate trends from earlier interglacials, reviewing recent estimates of greenhouse gas emissions from early agriculture, and describing a simulation by a climate model with a dynamic ocean forced by the low levels of greenhouse gases typical of previous interglacials in order to gauge the magnitude of the climate change for an inferred (natural) low greenhouse gas level relative to a high present day level. We conduct two time slice (equilibrium) simulations using present day orbital forcing and two levels of greenhouse gas forcing: the estimated low (natural) levels of previous interglacials, and the high levels of the present (control). By comparing the former to the latter, we estimate how much colder the climate would be without the combined greenhouse gas forcing of the early agriculture era (inferred from differences between this interglacial and previous interglacials) and the industrial era (the period since ～1750). With the low greenhouse gas levels, the global average surface temperature is 2.7 K lower than present day—ranging from ～2 K lower in the tropics to 4–8 K lower in polar regions. These changes are large, and larger than those reported in a pre-industrial (～1750) simulation with this model, because the imposed low greenhouse gas levels (CH4 = 450 ppb, CO2 = 240 ppm) are lower than both pre-industrial (CH4 = 760 ppb, CO2 = 280 ppm) and modern control (CH4 = 1,714 ppb, CO2 = 355 ppm) values. The area of year-round snowcover is larger, as found in our previous simulations and some other modeling studies, indicating that a state of incipient glaciation would exist given the current configuration of earth’s orbit (reduced insolation in northern hemisphere summer) and the imposed low levels of greenhouse gases. We include comparisons of these snowcover maps with known locations of earlier glacial inception and with locations of twentieth century glaciers and ice caps. In two earlier studies, we used climate models consisting of atmosphere, land surface, and a shallow mixed-layer ocean (Ruddiman et al., Quat Sci Rev 25:1–10, 2005; Vavrus et al., Quat Sci Rev 27:1410–1425, 2008). Here, we replaced the mixed-layer ocean with a complete dynamic ocean. While the simulated climate of the atmosphere and the surface with this improved model configuration is similar to our earlier results (Vavrus et al., Quat Sci Rev 27:1410–1425, 2008), the added information from the full dynamical ocean is of particular interest. The global and vertically-averaged ocean temperature is 1.25 K lower, the area of sea ice is larger, and there is less upwelling in the Southern Ocean. From these results, we infer that natural ocean feedbacks could have amplified the greenhouse gas changes initiated by early agriculture and possibly account for an additional increment of CO2 increase beyond that attributed directly to early agricultural, as proposed by Ruddiman (Rev Geophys 45:RG4001, 2007). However, a full test of the early anthropogenic hypothesis will require additional observations and simulations with models that include ocean and land carbon cycles and other refinements elaborated herein.  相似文献   

17.
Sulfur emissions to the atmosphere from natural sourees   总被引：1，自引：0，他引：1  
Emissions of sulfur gases from both natural and anthropogenic sources strongly influence the chemistry of the atmosphere. To assess the relative importance of these sources we have combined the measurements of sulfur gases and fluxes during the past decade to create a global emission inventory. The inventory, which is divided into 12 latitude belts, takes into account the seasonal dependence of sulfur emissions from biogenic sources. The total emissions of sulfur gases from natural sources are approximately 0.79 Tmol S/a. These emissions are 16% of the total sulfur emissions in the Northern Hemisphere and 58% in the Southern Hemisphere. The inventory clearly shows the impact of anthropogenic sulfur emissions in the region between 35° and 50°N.  相似文献   

18.
Little is known about in-canopy processes that may alter forest–atmosphere exchanges of trace gases and aerosols. To improve our understanding of in-canopy mixing, we use large-eddy simulation to study the effect of scalar source/sink distributions on scalar concentration moments, fluxes, and correlation coefficients within and above an ideal forest canopy. Scalars are emitted from: (1) the ground, (2) the canopy, and (3) both the ground and the canopy; a scalar is also deposited onto the canopy. All scalar concentration moments, fluxes, and correlation coefficients are affected by the source location/distribution, as is the scalar segregation intensity. We conclude that vertical source/sink distribution has a profound impact on scalar concentration profiles, fluxes, correlation coefficient, and scalar segregation.  相似文献   

19.
One of the crucial problems in study on the middle atmosphere is to determine theconcentration and distribution of some trace gases.In this aspect,sounding methods with highspectral resolution have been developed by many scientists.Some major trace gases and theirspectral characteristics,space-borne limb method for determination of trace gases in the middleatmosphere are introduced,requirements for used methods and instruments,development andchallenge encountered by sounding of trace gases with high spectral resolution are discussed in thispaper.  相似文献   

20.
不同降水强度对PM2.5的清除作用及影响因素   总被引：1，自引：0，他引：1       下载免费PDF全文
云和降水过程是大气污染物的重要清除途径,但由于降水过程和大气污染颗粒物本身的复杂性,目前降水过程对大气污染物的清除机制及影响因素有待深入研究。该文利用2014年3月—2016年7月在北京地区连续观测的PM2.5和降水数据,研究了不同降水强度对PM2.5的清除率,以及雨滴谱、风速和降水持续时间对PM2.5清除率的影响。研究表明:降水强度越大,对PM2.5清除效率越高。小雨、中雨和大雨对PM2.5清除率平均值分别为5.1%,38.5%和50.6%。小雨不但对PM2.5的清除率最低,而且对PM2.5的清除效果也存在很大差异,约50%的小雨个例中PM2.5质量浓度出现减小情况,而另外50%的小雨个例中,PM2.5质量浓度出现增加情况。在持续时间长或地面风速增大的情况下,小雨也表现出较高的清除率。在中雨和大雨情况下,PM2.5质量浓度均出现明显减小情况。但降水持续时间和风速对中雨和大雨的清除率影响较小,这是由于中雨和大雨一般在较短时间内即可清除大部分PM2.5,因此,对降水的持续时间和风速大小不敏感。  相似文献   

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