A global three-dimensional model of the tropospheric sulfur cycle

The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO₂ and SO₄ ^2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr^–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO₂, and SO₄ ^2– respectively.     

A global model of changing N2O emissions from natural and perturbed soils

A high resolution global model of the terrestrial biosphere is developed to estimate changes in nitrous oxide (N₂O) emissions from 1860–1990. The model is driven by four anthropogenic perturbations, including land use change and nitrogen inputs from fertilizer, livestock manure, and atmospheric deposition of fossil fuel NO _x . Global soil nitrogen mineralization, volatilization, and leaching fluxes are estimated by the model and converted to N₂O emissions based on broad assumptions about their associated N₂O yields. From 1860–1990, global N₂O emissions associated with soil nitrogen mineralization are estimated to have decreased slightly from 5.9 to 5.7 Tg N/yr, due mainly to land clearing, while N₂O emissions associated with volatilization and leaching of excess mineral nitrogen are estimated to have increased sharply from 0.45 to 3.3 Tg N/yr, due to all four anthropogenic perturbations. Taking into account the impact of each perturbation on soil nitrogen mineralization and on volatilization and leaching of excess mineral nitrogen, global 1990 N₂O emissions of 1.4, 0.7, 0.4 and 0.08 Tg N/yr are attributed to fertilizer, livestock manure, land clearing and atmospheric deposition of fossil fuel NO _x , respectively. Consideration of both the short and long-term fates of fertilizer nitrogen indicates that the N₂O/fertilizer-N yield may be 2% or more.C. NBM Definitions AET _mon (cm H₂O) = monthly actual evapotranspiration - AET _ann (cm H₂O) = annual actual evapotranspiration - age _h (years) = stand age of herbaceous biomass - age _w (years) = stand age of woody biomass - atmblc (gC/m²/month) = net flux of CO₂ from grid - biotoc (gC/g biomass) = 0.50 = convert g biomass to g C - beff _h = 0.8 = fraction of cleared herbaceous litter that is burned - beff _w = 0.4 = fraction of cleared woody litter that is burned - bfmin = 0.5 = fraction of burned N litter that is mineralized or converted to reactive gases which rapidly redeposit. Remainder assumed pyrodenitrified to N₂. + N₂O - bprob = probability that burned litter will be burned - burn _h (gC/m²/month) = herbaceous litter burned after land clearing - burn _w (gC/m²/month) = woody litter burned after land clearing - cbiomsh (gC/m²) = C herbaceous biomass pool - cbiomsw (gC/m²) = C woody biomass pool - clear (gC/m²/month) = woody litter C removed by land clearing - clearn (gN/m²/month) = woody litter N removed by land clearing - cldh (month^–1) = herbaceous litter decomposition coefficient - cldw (month^–1) = woody litter decomposition coefficient - clittrh (gC/m²) = C herbaceous litter pool - clittrw (gC/m²) = C woody litter pool - clph (month^–1) = herbaceous litter production coefficient - clpw (month^–1) = woody litter production coefficient - cnrath (gC/gN) = C/N ratio in herbaceous phytomass - cnrats (gC/gN) = C/N ratio in soil organic matter - cnratt (gC/gN) = average C/N ratio in total phytomass - cnratw (gC/gN) = C/N ratio in woody phytomass - crod (month^–1) = forest clearing coefficient - csocd (month^–1) = actual soil organic matter decompostion coefficient - decmult decomposition coefficient multiplier; natural =1.0; agricultural =1.0 (1.2 in sensitivity test) - fertmin (gN/m²/month) = inorganic fertilizer input - fleach fraction of excess inorganic N that is leached - fligh (g Lignin/ g C) = lignin fraction of herbaceous litter C - fligw (g Lignin/ g C) = 0.3 = lignin fraction of woody litter C - fln2o = .01–.02 = fraction of leached N emitted as N₂O - fnav = 0.95 = fraction of mineral N available to plants - fosdep (gN/m²/month) = wet and dry atmospheric deposition of fossil fuel NO _x - fresph = 0.5 = fraction of herbaceous litter decomposition that goes to CO₂ respiration - fresps = 0.51 + .068 ^* sand = fraction of soil organic matter decomposition that goes to CO₂ respiration - frespw = 0.3 ^* (^* see comments in Section 2.3 under decomposition) = fraction of woody litter decomposition that goes to CO₂ respiration - fsoil = ratio of NPP measured on given FAO soil type to NPF_miami - fstruct = 0.15 + 0.018 ^* ligton = fraction of herbaceous litter going to structural/woody pool - fvn2o = .05–.10 = fraction of excess volatilized mineral N emitted as N₂O - fvol = .02 = fraction of gross mineralization flux and excess mineral N volatilized - fyield ratio of total agricultural NPP in a given country in 1980 to total NPP_miami of all displaced natural grids in that country - gimmob _h (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of herbaceous litter - gimmob _s (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of soil organic matter - gimmob _w (gN/m²/month) = gross immobilization of inorganic N into microbial biomass due to decomposition of woody litter - graze (gC/m²/month) = C herbaceous biomass grazed by livestock - grazen (gN/m²/month) = N herbaceous biomass grazed by livestock - growth _h (gC/m²/month) = herbaceous litter incorporated into microbial biomass - growth _w (gC/m²/month) = woody litter incorporated into microbial biomass - gromin _h (gN/m²/month) = gross N mineralization due to decomposition and burning of herbaceous litter - gromin _s (gN/m²/month) = gross N mineralization due to decomposition of soil organic matter - gromin _w (gN/m²/month) = gross N mineralization due to decomposition and burning of woody litter - herb herbaceous fraction by weight of total biomass - leach (gN/m²/month) = leaching (& volatilization) losses of excess inorganic N - ligton (g lignin-C/gN) = lignin/N ratio in fresh herbaceous litter - LP _h (gC/m²/month)= C herbaceous litter production - LP (gC/m²/month) = C woody litter production - LPN _h (gN/m²/month) = N herbaceous litter production - LPN _W (gN/m²/month) = N woody litter production - manco2 (gC/m²/month) = grazed C respired by livestock - manlit (gC/m²/month) = C manure input (feces + urine) - n2oint (gN/m²/month) = intercept of N₂O flux vs gromin regression - n2oleach (gN/m²/month) = N₂O flux associated with leaching and volatilization of excess inorganic N - n2onat (gN/m²/month) = natural N₂O flux from soils - n2oslope slope of N₂O flux vs gromin regression - nbiomsh (gN/m²) = N herbaceous biomass pool - nbiomsw (gN/m²) = N woody biomass pool - nfix (gN/m²/month) = N₂ fixation + natural atmospheric deposition - nlittrh (gN/m²) = N herbaceous litter pool - nlittrw (gN/m²) = N woody litter pool - nmanlit (gN/m²/month) = organic N manure input (feces) - nmanmin (gN/m²/month) = inorganic N manure input (urine) - nmin (gN/m²) = inorganic N pool - NPP _acth (gC/m²/month)= actual herbaceous net primary productivity - NPP _actw (gC/m²/month) = actual woody net primary productivity - nvol (gN/m²/month) = volatilization losses from inorganic N pool - plntnav (gN/m²/month)= mineral N available to plants - plntup _h (gN/m²/month) = inorganic N incorporated into herbaceous biomass - plntup _w (gN/m²/month) = inorganic N incorporated into woody biomass - precip _ann (mm) = mean annual precipitation - precip _mon (mm) = mean monthly precipitation - pyroden _h (gN/m²/month) = burned herbaceous litter N that is pyrodenitrified to N₂ - pyroden _w (gN/m²/month) = burned woody litter N that is pyrodenitrified to N₂ - recyc fraction of N that is retranslocated before senescence - resp _h (gC/m²/month) = herbaceous litter CO₂ respiration - resp _s (gC/m²/month) = soil organic carbon CO₂ respiration - resp _w (gC/m²/month) = woody litter CO₂ respiration - sand sand fraction of soil - satrat ratio of maximum NPP to N-limited NPP - soiloc (gC/m²) = soil organic C pool - soilon (gN/m²) = soil organic N pool - temp _ann (°C) = mean annual temperature - temp _mon (°C) = mean monthly temperature Now at the NOAA Aeronomy Laboratory, Boulder, Colorado.     

GRAPES全球模式云方案的诊断研究

在对GRAPES全球预报系统(GRAPES_GFS)云预报性能进行诊断评估的基础上,对凝结(华)和蒸发等物理过程及对流卷出对云的影响过程进行改进和优化,旨在提高GRAPES_GFS云量及其特征量和降水的预报精度.通过研究GRAPES全球模式、欧洲中期天气预报中心(ECMWF)和美国环境预报中心(NCEP)全球模式中3种...     

Evaluation of alkene degradation in the detailed tropospheric chemistry mechanism, MCM v3, using environmental chamber data

The representation of alkene degradation in version 3 of the Master Chemical Mechanism (MCM v3) has been evaluated, using environmental chamber data on the photo-oxidation of ethene, propene, 1-butene and 1-hexene in the presence of NO_x, from up to five chambers at the Statewide Air Pollution Research Center (SAPRC) at the University of California. As part of this evaluation, it was necessary to include a representation of the reactions of the alkenes with O(³P), which are significant under chamber conditions but generally insignificant under atmospheric conditions. The simulations for the ethene and propene systems, in particular, were found to be sensitive to the branching ratios assigned to molecular and free radical forming pathways of the O(³P) reactions, with the extent of radical formation required for proper fitting of the model to the chamber data being substantially lower than the reported consensus. With this constraint, the MCM v3 mechanisms for ethene and propene generally performed well. The sensitivity of the simulations to the parameters applied to a series of other radical sources and sink reactions (radical formation from the alkene ozonolysis reactions and product carbonyl photolysis; radical removal from the reaction of OH with NO₂ and β-hydroxynitrate formation) were also considered, and the implications of these results are discussed. Evaluation of the MCM v3 1-butene and 1-hexene degradation mechanisms, using a more limited dataset from only one chamber, was found to be inconclusive. The results of sensitivity studies demonstrate that it is impossible to reconcile the simulated and observed formation of ozone in these systems for ranges of parameter values which can currently be justified on the basis of the literature. As a result of this work, gaps and uncertainties in the kinetic, mechanistic and chamber database are identified and discussed, in relation to both tropospheric chemistry and chemistry important under chamber conditions which may compromise the evaluation procedure, and recommendations are made for future experimental studies. Throughout the study, the performance of the MCM v3 chemistry was also simultaneously compared with that of the corresponding chemistry in the SAPRC-99 mechanism, which was developed and optimized in conjunction with the chamber datasets.     

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.     

4D tomographic reconstruction of the tropospheric wet refractivity using the concept of virtual reference station,case study: northwest of Iran

Iran enjoys a variety of climatological conditions. Moreover, numerical weather prediction (NWP) models are not assimilated with the meteorological data in Iran, the country suffering from poor spatial and temporal resolution of radiosonde measurements. These facts make modeling of troposphere impossible using the measurements and NWP. On the other hand, the global positioning system (GPS) has been emerged as a valuable tool for modeling and remote sensing of Earth’s atmosphere. This research is the first attempt to address the tropospheric wet refractivity modeling by GPS measurements in Iran. Changes of topography in the study area are taken into account. As a leading work, virtual reference stations (VRS) are used to fix the rank deficiency of the problem. The model space resolution matrix is used to achieve the optimum spatial resolution of the tomographic model and the optimum number of VRS stations. The accuracy of the developed model (KNTU1) is investigated by deploying radiosonde measurements.     

A numerical study of tropospheric ozone in the springtime in East Asia

The Models-3 Community Multi-scale Air Quality modeling system (CMAQ)coupled with the Regional Atmospheric Modeling System (RAMS)is applied to East Asia to study the transport and photochemical transformation of tropospheric ozone in March 1998．The calculated mixing ratios of ozone and carbon monoxide are compared with ground 1evel observations at three remote sites in Japan and it is found that the model reproduces the observed features very well．Examination of several high episodes of ozone and carbon monoxide indicates that these elevated levels are found in association with continental outflow,demonstrating the critical role of the rapid transport of carbon monoxide and other ozone precursors from the continental boundary layer．In comparison with available ozonesonde data,it is found that the model-calculated ozone concentrations are generally in good agreement with the measurements,and the stratospheric contribution to surface ozone mixing ratios is quite limited．     

Impact of cloud dynamics on tropospheric chemistry: Advances in modeling the interactions between microphysical and chemical processes

A chemical module describing the tropospheric photochemistry of ozone precursors in both gaseous and aqueous phases for a remote continental atmosphere has been developed within the framework of a two-dimensional cloud model. Dynamical, microphysical and chemical processes are fully interacting in order to study the influence of clouds on ozone chemistry and to quantify the relative importance of the different processes on the budget and evolution of 12 chemical species. Whereas the concentrations of highly soluble species are strongly affected by evaporation and sedimentation, less soluble species are affected primarily by accretion. The model reproduces previously observed chemical phenomena such as the enrichment of formic acid at the top of the cloud.     

Effects of tropical deforestation on global and regional atmospheric chemistry

A major portion of tropospheric photochemistry occurs in the tropics. Deforestation, colonization, and development of tropical rain forest areas could provoke significant changes in emissions of radiatively and photochemically active trace gases. A brief review of studies on trace-gas emissions in pristine and disturbed tropical habitats is followed by an effort to model regional tropospheric chemistry under undisturbed and polluted conditions. Model results suggest that changing emissions could stimulate photochemistry leading to enhanced ozone production and greater mineral acidity in rainfall in colonized agricultural regions. Model results agree with measurements made during the NASA ABLE missions. Under agricultural/pastoral development scenarios, tropical rain forest regions could export greater levels of N₂O, CH₄, CO, and photochemical precursors of NO _y and O₃ to the global atmosphere with implications for climatic warming.     

A three-dimensional model of the global ammonia cycle

Using a three-dimensional (3-D) transport model of the troposphere, we calculated the global distributions of ammonia (NH₃) and ammonium (NH ₄ ⁺ ), taking into account removal of NH₃ on acidic aerosols, in liquid water clouds and by reaction with OH. Our estimated global 10°×10° NH₃ emission inventory of 45 Tg N-NH₃ yr^– provides a reasonable agreement between calculated wet NH ₄ ⁺ deposition and measurements and of measured and modeled NH ₄ ⁺ in aerosols, although in Africa and Asia especially discrepancies exist.NH₃ emissions from natural continental ecosystems were calculated applying a canopy compensation point and oceanic NH₃ emissions were related to those of DMS (dimethylsulfide). In many regions of the earth, the pH found in rain and cloud water can be attributed to acidity derived from NO, SO₂ and DMS emissions and alkalinity from NH₃. In the remote lower troposphere, sulfate aerosols are calculated to be almost neutralized to ammonium sulfate (NH₄)₂SO₄, whereas in the middle and upper troposphere, according to our calculations, the aerosol should be more acidic, as a result of the oxidation of DMS and SO₂ throughout the troposphere and removal of NH₃ on acidic aerosols at lower heights. Although the removal of NH₃ by reaction with the OH radical is relatively slow, the intermediate NH₂ radical can provide a substantial annual N₂O source of 0.9 _–0.4 ^+0.9 Tg, thus contributing byca. 5% to estimated global N₂O production. The oxidation by OH of NH₃ from anthropogenic sources accounts for 10% of the estimated total anthropogenic sources of N₂O. This source was not accounted for in previous studies, and is mainly located in the tropics, which have high NH₃ and OH concentrations. Biomass burning plumes, containing high NO _x and NH₃ concentrations provide favourable conditions for gas phase N₂O production. This source is probably underestimated in this model study, due to the coarse resolution of the 3-D model, and the rather low biomass burning NH₃ and NO _x emissions adopted. The estimate depends heavily on poorly known concentrations of NH₃ (and NO _x ) in the tropics, and uncertainties in the rate constants of the reactions NH₂ + NO₂ N₂O + H₂O (R4), and NH₂ + O₃ NH₂O + O₂ (R7).     

A study on large-scale nudging effects in regional climate model simulation

The large-scale nudging effects on the East Asian summer monsoon (EASM) are examined using the National Centers for Environmental Prediction (NCEP) Regional Spectral Model (RSM). The NCEP/DOE reanalysis data is used to provide large-scale forcings for RSM simulations, configured with an approximately 50-km grid over East Asia, centered on the Korean peninsula. The RSM with a variant of spectral nudging, that is, the scale selective bias correction (SSBC), is forced by perfect boundary conditions during the summers (June–July–August) from 1979 to 2004. The two summers of 2000 and 2004 are investigated to demonstrate the impact of SSBC on precipitation in detail. It is found that the effect of SSBC on the simulated seasonal precipitation is in general neutral without a discernible advantage. Although errors in large-scale circulation for both 2000 and 2004 are reduced by using the SSBC method, the impact on simulated precipitation is found to be negative in 2000 and positive in 2004 summers. One possible reason for a different effect is that precipitation in the summer of 2004 is characterized by a strong baroclinicity, while precipitation in 2000 is caused by thermodynamic instability. The reduction of convective rainfall over the oceans by the application of the SSBC method seems to play an important role in modeled atmosphere.     

Asthenospheric ice-load effects in a global dynamical-system model of the Pleistocene climate

In a previous dynamical model the late Cenozoic climate variations were simulated, taking into account free and forced variations of atmospheric carbon dioxide acting in concert with changes in global ice mass and the deep ocean thermal state, all under the influence of the known earth-orbital radiative changes. This model is now extended by adding another relevant variable, bedrock/asthenosphere depression, including its associated ice-calving effects. Within the context of this extended model we (1) demonstrate the main results of previous bedrock/ice sheet models in what we believe is the simplest possible manner, (2) show how these previous models can exhibit the mid-Pleistocene transition with the inclusion of CO₂ effects, (3) discuss the limitations of these previous bedrock models, and (4) illustrate the possibility of removing some of these limitations and accounting for further aspects of the paleoclimate record by using the full dynamical system that includes forced and free effects of CO₂, as well as effects of bedrock depression and Milankovitch forcing. As one example of a new possibility, with bedrock effects included in the full system we can obtain a solution characterized by irregularly spaced, intermittent episodes in which the behavior is dominated either by near-40 kyr period oscillations or by near-100 kyr periods (such as prevailed over the Pleistocene).     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.