Three-dimensional Chemical Transport Model Research Articles

Development and application of a computationally efficient particulate matter apportionment algorithm in a three-dimensional chemical transport model

An on-line and an off-line version of a computationally efficient particulate matter source apportionment algorithm have been developed and compared using the three-dimensional chemical transport model PMCAMx. Both versions of the algorithm use source specific-species that track the contributions of source locations or source classes. The two versions showed a good agreement with each other and with more accurate, computationally demanding methods. The off-line algorithm (Particulate Source Apportionment Technology, PSAT) is simpler to implement, has a lower computational cost and is suitable for a range of source apportionment studies. As a first application, PSAT was used to investigate the contribution of power plant SO 2 emissions to particulate sulfate concentrations in the Eastern United States. The impact of the transport of SO 2 emissions from the Chicago, IL area and the impact of these emissions on particulate sulfate concentration in surrounding areas were also studied as a second application. The implementation of PSAT for the SO 2/particulate sulfate system only resulted in a 1% increase in computation time over the base simulation. The algorithm provides a computationally efficient platform for the study of pollutant transport and source contributions on regional scales.

A model inter-comparison study focussing on episodes with elevated PM10 concentrations

Five three-dimensional chemical transport models of different complexity were applied to Central Europe to assess the ability of models to reproduce PM10 concentrations under highly polluted conditions. The participating models were the French CHIMERE model, the Dutch LOTOS-EUROS model, as well as the REM-CALGRID, the EURAD and the LM–MUSCAT models from Germany. In the selected 80-day period, observed PM10 daily mean concentrations reached values well above 50 μg m −3 on many days in large parts of Northern Germany. This model evaluation shows that there is an increasing underestimation of primary and secondary species with increasing observed PM10. The high PM levels were observed under stagnant weather conditions, which are difficult to simulate with either prognostic or diagnostic, interpolation-based meteorological models. Thus, it is quite likely that uncertainties in PM emissions and incomplete process sub-modules each separately account for only a portion of the underestimation of high PM. Uncertainties in key boundary layer parameters, which can differ by a factor of two or more between the models, represent an additional source of error—both as direct sources of error through the transporting meteorological fields and indirect sources of error through the physico-chemical modules which rely on key boundary layer parameters.

Response of Inorganic Fine Particulate Matter to Emission Changes of Sulfur Dioxide and Ammonia: The Eastern United States as a Case Study

A three-dimensional chemical transport model (PMCAMx) was used to investigate changes in fine particle (PM2.5) concentrations in response to changes in sulfur dioxide (SO2) and ammonia (NH3) emissions during July 2001 and January 2002 in the eastern United States. A uniform 50% reduction in SO2 emissions was predicted to produce an average decrease of PM2.5 concentrations by 26% during July but only 6% during January. A 50% reduction of NH3 emissions leads to an average 4 and 9% decrease in PM2.5 in July and January, respectively. During the summer, the highest concentration of sulfate is in South Indiana (12.8 μg m-3), and the 50% reduction of SO2 emissions results in a 5.7 μg m-3(44%) sulfate decrease over this area. During winter, the SO2 emissions reduction results in a 1.5 μg m-3 (29%) decrease of the peak sulfate levels (5.2 μg m-3) over Southeast Georgia. The maximum nitrate and ammonium concentrations are predicted to be over the Midwest (1.9 μg m-3 in Ohio and 5.3 μg m-3 in South Indiana, respectively) in the summer whereas in the winter these concentrations are higher over the Northeast (3 μg m-3 of nitrate in Connecticut and 2.7 μg m-3 of ammonium in New York). The 50% NH3 emissions reduction is more effective for controlling nitrate, compared with SO2 reductions, producing a 1.1 μg m-3 nitrate decrease over Ohio in July and a 1.2 μg m-3 decrease over Connecticut in January. Ammonium decreases significantly when either SO2 or NH3 emissions are decreased. However, the SO2 control strategy has better results in July when ammonium decreases, up to 2 μg m-3 (37%), are predicted in South Indiana. The NH3 control strategy has better results in January (ammonium decreases up to 0.4 μg m-3 in New York). The spatial and temporal characteristics of the effectiveness of these emission control strategies during the summer and winter seasons are discussed.

An observed and analysed stratospheric ozone intrusion over the high Canadian Arctic UTLS region during the summer of 2003

An exceptional ozone increase in the upper troposphere–lower stratosphere region has been recorded by an ozone sounding performed over the high Canadian Arctic at the beginning of August 2003. Simultaneously observed low humidity and low tropopause height suggest that this anomalous ozone enhancement is attributed to a downward transport from the stratosphere. This latter transport is investigated by using the Ertel potential vorticity field calculated from the ECMWF analyses. The occurrence of such high ozone concentrations is shown to be due to stratospheric ozone-rich air intrusions. These latter mesoscale phenomena are successfully captured using the assimilation of Envisat/MIPAS ozone profiles into the global three-dimensional chemistry transport model of Meteo-France (MOCAGE). This study shows that Envisat/MIPAS ozone profiles assimilation adds value in the sense that the analyses capture the whole stratospheric intrusion episode, whereas the raw model simulation does not. Copyright © 2007 Royal Meteorological Society

Examination of the 2002 major warming in the southern hemisphere using ground-based and Odin/SMR assimilated data: stratospheric ozone distributions and tropic/mid-latitude exchange

Following an exceptionally active winter, the 2002 Southern Hemisphere (SH) major warming occurred in late September. It was preceded by three minor warming events that occurred in late August and early September, and yielded vortex split and break-down over Antarctica. Ozone (O3 and nitrous oxide (N2O) profiles obtained during that period of time (15 August – 4 October) by the Sub-Millimetre Radiometer (SMR) aboard the Odin satellite are assimilated into MOCAGE (Modélisation Isentrope du transport Mésoéchelle de l'Ozone Stratosphérique par Advection), a global three-dimensional chemistry transport model of Météo-France. The assimilated algorithm is a three-dimensional-FGAT built by the European Centre for Research and Advance Training in Scientific Computation (CERFACS) using the PALM (Projet d'Assimilation par Logiciel Multi-méthode) software. The assimilated O3 and N2O profiles and isentropic distributions are compared to ground-based measurements (LIDAR and balloon-sonde) and to maps of advected potential vorticity (APV). The latter is computed by the MIMOSA (Modélisation Isentrope du transport Mésoéchelle de l'Ozone Stratosphérique par Advection) model, a high-resolution advection transport model, using meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). It is found that O3 concentrations retrieved by the MOCAGE–PALM assimilation system show a reasonably good agreement in the 20–28 km height range when compared with ground-based profiles. This altitude range corresponds to the intersection between the MOCAGE levels (0–28 km) and SMR O3 retrievals (20–50 km). Moreover, comparison of N2O assimilated fields with MIMOSA APV maps indicates that the dramatic split and subsequent break-down of the polar vortex, as well as the associated mixing of mid- and low-latitude stratospheric air, are well resolved and pictured by MOCAGE–PALM. The present study demonstrates also that the tremendous dynamics and associated polar vortex deformations during the 2002-austral-winter have modified ozone and nitrous oxide distributions not only at the vicinity of the polar vortex, but over topics and subtropics as well. PACS Nos.: 92.60.H–, 92.60.Hd, 92.70.Cp, 92.70.Gt

Mid-latitude ozone changes: studies with a 3-D CTM forced by ERA-40 analyses

Abstract. We have used an off-line three-dimensional (3-D) chemical transport model (CTM) to study long-term changes in stratospheric O3. The model was run from 1977–2004 and forced by ECMWF ERA-40 and operational analyses. Model runs were performed to examine the impact of increasing halogens and additional stratospheric bromine from short-lived source gases. The analyses capture much of the observed interannual variability in column ozone, but there are also unrealistic features. In particular the ERA-40 analyses cause a large positive anomaly in northern hemisphere (NH) column O3 in the late 1980s. Also, the change from ERA-40 to operational winds at the start of 2002 introduces abrupt changes in some model fields (e.g. temperature, ozone) which affect analysis of trends. The model reproduces the observed column increase in NH mid-latitudes from the mid 1990s. Analysis of a run with fixed halogens shows that this increase is not due to a significant decrease in halogen-induced loss, i.e. is not an indication of recovery. The model predicts only a small decrease in halogen-induced loss after 1999. In the upper stratosphere, despite the modelled turnover of chlorine around 1999, O3 does not increase because of the effects of increasing ECMWF temperatures, decreasing modelled CH4 at this altitude, and abrupt changes in the SH temperatures at the end of the ERA-40 period. The impact of an additional 5 pptv stratospheric bromine from short-lived species decreases mid-latitude column O3 by about 10 DU. However, the impact on the modelled relative O3 anomaly is generally small except during periods of large volcanic loading.

Predicted Secondary Organic Aerosol Concentrations from the Oxidation of Isoprene in the Eastern United States

Isoprene, the most abundant non-methane hydrocarbon emitted into the troposphere, has generally not been considered a major source of SOA due to the relatively high volatility of its oxidation products. In this study, the SOA formed from the oxidation of isoprene is predicted using a three-dimensional chemical transport model, PMCAMx, across the eastern U.S. for July, October, January, and April 2001-2002. The variability of the measured SOA yields in the available smog chamber studies is captured by combining the base case scenario with upper and lower bound estimates of the measurements. For the base case simulation, the predicted annual average isoprene SOA concentration in the southeast is 0.09 microg m(-3) (bounds 0.04-0.23 microg m(-3)). Isoprene is predicted to produce 70% less SOA across the entire domain for spring and fall than during the summer and negligible amounts of SOA during the winter. During the summer, the average concentrations in the northeast are predicted to be 0.11 microg m(-3) (bounds 0.04-0.31 microg m(-3)) and in the southeast 0.19 microg m(-3) (bounds 0.11 -0.58 microg m(-3)). PMCAMx predictions are compared to available measurements of some isoprene SOA components in North Carolina and New York State. These modeling results suggest that on an annual basis isoprene oxidation is a small but non-negligible organic aerosol source in the eastern U.S. Its contribution is relatively more important during the summer and in the southeast U.S.

Technical Note: A new SIze REsolved Aerosol Model (SIREAM)

Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation-nucleation. A quasi-stationary sectional approach is used to describe the size distribution change due to condensation/evaporation, and a hybrid equilibrium/dynamical mass-transfer method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM Sartelet et al. (2006). It is hosted in the modeling system Polyphemus Mallet et al., 2007, but can be linked to any other three-dimensional Chemistry-Transport Model.

Measurements of mid-stratospheric formaldehyde from the Odin/SMR instrument

Measurements of mid-stratospheric formaldehyde (H 2CO) have been obtained from the limb-viewing sub-millimeter radiometer (SMR) instrument aboard the Odin satellite. The analysis is based upon the only weak (8 08→7 07) rotational transition line of H 2CO that can be measured by Odin/SMR at 576.7083150 GHz in the band dedicated to the measurement of carbon monoxide (CO). The signal-to-noise ratio is increased by averaging about 1000 spectra within 2-km width vertical layers in the stratosphere over periods from 1 to 7 days and within 3 latitude bands: Southern Hemisphere (90°S–45°S), tropics (30°S–30°N), and Northern Hemisphere (45°N–90°N). The faint H 2CO line can then be retrieved using the standard scientific ground-segment developed for the Odin/SMR measurements. The mid-stratospheric H 2CO shows maxima in the tropics for every period considered (January 2006, February 2005, March 2005, and September 2005). The spring-time extra-tropical mid-stratospheric H 2CO is more intense than the fall-time extra-tropical amounts. The simulations from the three-dimensional chemical-transport model Reprobus satisfactorily show these general features.

Source contributions to primary organic aerosol: Comparison of the results of a source-resolved model and the chemical mass balance approach

A source-resolved model has been developed to predict the contribution of different sources to primary organic aerosol concentrations. The model was applied to the eastern US during a 17 day pollution episode beginning on 12 July 2001. Primary organic matter (OM) and elemental carbon (EC) concentrations are tracked for eight different sources: gasoline vehicles, non-road diesel vehicles, on-road diesel vehicles, biomass burning, wood burning, natural gas combustion, road dust, and all other sources. Individual emission inventories are developed for each source and a three-dimensional chemical transport model (PMCAMx) is used to predict the primary OM and EC concentrations from each source. The source-resolved model is simple to implement and is faster than existing source-oriented models. The results of the source-resolved model are compared to the results of chemical mass balance models (CMB) for Pittsburgh and multiple urban/rural sites from the Southeastern Aerosol Research and Characterization (SEARCH) network. Significant discrepancies exist between the source-resolved model and the CMB model predictions for some of the sources. There is strong evidence that the organic PM emissions from natural gas combustion are overestimated. It also appears that the OM and EC emissions from wood burning and off-road diesel are too high in the Northeastern US. Other similarities and discrepancies between the source-resolved model and the CMB model for primary OM and EC are discussed along with problems in the current emission inventory for certain sources.

Inter-annual Variations of Ozone and Nitrogen Dioxide Over Europe During 1958–2003 Simulated with a Regional CTM

Inter-annual variability of surface ozone (O3) and nitrogen dioxide (NO2) over Europe has been studied over the period 1958–2003 using a three-dimensional Chemistry-Transport Model coupled to meteorological data from the ERA40 data set produced at the European Centre of Medium-range Weather Forecasts (ECMWF). Emissions and boundary conditions were kept at present levels throughout the simulation period. It was found that the annual mean NO2 concentration varies between ±50% and the summer mean O3 concentration varies between −10 and +20 percent (%) compared to the 46-year average over the model domain. There is also variation in ozone and NO2 over longer time scales. The last 22 years display high concentrations of ozone in central and south-western Europe and low concentrations in north-eastern Europe. The first 22 years display very high concentrations of NO2 over the North Sea. There is indication of trends in ozone and nitrogen dioxide but this has to be investigated further. Such information is one factor that should be taken into account when considering future control strategies.

Development and application of a three-dimensional aerosol chemical transport model, PMCAMx

A three-dimensional chemical transport model (PMCAMx) is used to simulate PM mass and composition in the eastern United States for a July 2001 pollution episode. The performance of the model in this region is evaluated, taking advantage of the highly time and size-resolved PM and gas-phase data collected during the Pittsburgh Air Quality Study (PAQS). PMCAMx uses the framework of CAMx and detailed aerosol modules to simulate inorganic aerosol growth, aqueous-phase chemistry, secondary organic aerosol formation, nucleation, and coagulation. The model predictions are compared to hourly measurements of PM 2.5 mass and composition at Pittsburgh, as well as to measurements from the AIRS and IMPROVE networks. The performance of the model for the major PM 2.5 components (sulfate, ammonium, and organic carbon) is encouraging (fractional errors are in general smaller than 50%). Additional improvements are possible if the rainfall measurements are used instead of the meteorological model predictions. The modest errors in ammonium predictions and the lack of bias for the total (gas and particulate) ammonium suggest that the improved ammonia inventory used is reasonable. The significant errors in aerosol nitrate predictions are mainly due to difficulties in simulating the nighttime formation of nitric acid. The concentrations of elemental carbon (EC) in the urban areas are significantly overpredicted. This is a problem related to both the emission inventory but also the different EC measurement methods that have been used in the two measurement networks (AIRS and IMPROVE) and the actual development of the inventory. While the ability of the model to reproduce OC levels is encouraging, additional work is necessary to confirm that that this is due to the right reasons and not offsetting errors in the primary emissions and the secondary formation. The model performance against the semi-continuous measurements in Pittsburgh appears to be quite similar to its performance against daily average measurements in a wide range of stations across the Eastern US. This suggests that the skill of the model to reproduce the diurnal variability of PM 2.5 and its major components is as good as its ability to reproduce the daily average values and also the significant value of high temporal resolution measurements for model evaluation.

Role of ammonia chemistry and coarse mode aerosols in global climatological inorganic aerosol distributions

We use an inorganic aerosol thermodynamic equilibrium model in a three-dimensional chemical transport model to understand the roles of ammonia chemistry and natural aerosols on the global distribution of aerosols. The thermodynamic equilibrium model partitions gas-phase precursors among modeled aerosol species self-consistently with ambient relative humidity and natural and anthropogenic aerosol emissions during the 1990s. Model simulations show that accounting for aerosol inorganic thermodynamic equilibrium, ammonia chemistry and dust and sea-salt aerosols improve agreement with observed SO 4, NO 3, and NH 4 aerosols especially at North American sites. This study shows that the presence of sea salt, dust aerosol and ammonia chemistry significantly increases sulfate over polluted continental regions. In all regions and seasons, representation of ammonia chemistry is required to obtain reasonable agreement between modeled and observed sulfate and nitrate concentrations. Observed and modeled correlations of sulfate and nitrate with ammonium confirm that the sulfate and nitrate are strongly coupled with ammonium. SO 4 concentrations over East China peak in winter, while North American SO 4 peaks in summer. Seasonal variations of NO 3 and SO 4 are the same in East China. In North America, the seasonal variation is much stronger for NO 3 than SO 4 and peaks in winter. Natural sea salt and dust aerosol significantly alter the regional distributions of other aerosols in three main ways. First, they increase sulfate formation by 10–70% in polluted areas. Second, they increase modeled nitrate over oceans and reduce nitrate over Northern hemisphere continents. Third, they reduce ammonium formation over oceans and increase ammonium over Northern Hemisphere continents. Comparisons of SO 4, NO 3 and NH 4 deposition between pre-industrial, present, and year 2100 scenarios show that the present NO 3 and NH 4 deposition are twice pre-industrial deposition and present SO 4 deposition is almost five times pre-industrial deposition.

Interannual variation and trends in air pollution over Europe due to climate variability during 1958–2001 simulated with a regional CTM coupled to the ERA40 reanalysis

A three-dimensional Chemistry Transport Model was used to study the meteorologically induced interannual variability and trends in deposition of sulphur and nitrogen as well as concentrations of surface ozone (O3), nitrogen dioxide (NO2) and particulate matter (PM) and its constituents over Europe during 1958–2001. The model was coupled to the meteorological reanalysis ERA40, produced at the European Centre for Medium-range Weather Forecasts. Emissions and boundary conditions of chemical compounds and PM were kept constant at present levels.The average European interannual variation, due to meteorological variability, ranges from 3% for O3, 5% for NO2, 9% for PM, 6–9% for dry deposition, to about 20% for wet deposition of sulphur and nitrogen. For the period 1979–2001 the trend in ozone, due to climate variability is increasing in central and southwestern Europe and decreasing in northeastern Europe, the trend in NO2 is approximately opposite. The trend in PM is positive in eastern Europe. There are negative trends in wet deposition in southwestern and central Europe and positive trends in dry deposition overall. A bias in ERA40 precipitation could be partly responsible for the trends. The variation and trends need to be considered when interpreting measurements and designing measurement campaigns.

Key aspects of stratospheric tracer modeling using assimilated winds

Abstract. This study describes key aspects of global chemistry-transport models and their impact on stratospheric tracer transport. We concentrate on global models that use assimilated winds from numerical weather predictions, but the results also apply to tracer transport in general circulation models. We examined grid resolution, numerical diffusion, air parcel dispersion, the wind or mass flux update frequency, and time interpolation. The evaluation is performed with assimilated meteorology from the "operational analyses or operational data" (OD) from the European Centre for Medium-Range Weather Forecasts (ECMWF). We also show the effect of the mass flux update frequency using the ECMWF 40-year re-analyses (ERA40). We applied the three-dimensional chemistry-transport Tracer Model version 5 (TM5) and a trajectory model and performed several diagnoses focusing on different transport regimes. Covering different time and spatial scales, we examined (1) polar vortex dynamics during the Arctic winter, (2) the large-scale stratospheric meridional circulation, and (3) air parcel dispersion in the tropical lower stratosphere. Tracer distributions inside the Arctic polar vortex show considerably worse agreement with observations when the model grid resolution in the polar region is reduced to avoid numerical instability. The results are sensitive to the diffusivity of the advection. Nevertheless, the use of a computational cheaper but diffusive advection scheme is feasible for tracer transport when the horizontal grid resolution is equal or smaller than 1 degree. The use of time interpolated winds improves the tracer distributions, particularly in the middle and upper stratosphere. Considerable improvement is found both in the large-scale tracer distribution and in the polar regions when the update frequency of the assimilated winds is increased from 6 to 3 h. It considerably reduces the vertical dispersion of air parcels in the tropical lower stratosphere. Strong horizontal dispersion is not necessarily an indication of poor wind quality, as observations indicate. Moreover, the generally applied air parcel dispersion calculations should be interpreted with care, given the strong sensitivity of dispersion with altitude. The results in this study provide a guideline for stratospheric tracer modeling using assimilated winds. They further demonstrate significant progress in the use of assimilated meteorology in chemistry-transport models, relevant for both short- and long-term integrations.

Global Modelling of the Atmospheric Methyl Bromide Budget

A global three-dimensional chemical transport model has been used to identify and evaluate possible candidates for the `missing' surface source required to balance the atmospheric budget of methyl bromide. Both natural and anthropogenic emissions of methyl bromide are `coloured' in the model, thus allowing the global CH3Br distribution to be broken-down into its source components. These coloured CH3Br tracers are then combined in various ways to create one base-line emission scenario and five further plausible scenarios. The additional emission scenarios are specifically designed to test whether the geographical distribution and seasonal cycles of additional vegetation and/or increased biomass burning emissions are consistent with atmospheric observations of methyl bromide mixing ratios. Due to an imbalance in our current understanding of the methyl bromide budget, simulated CH3Br mixing ratios from the base-line emission scenario are significantly lower than atmospheric measurements. Both the inclusion of a vegetation source in the tropics and a double strength biomass burning source substantially improve the agreement between model simulations and atmospheric measurements compared with the base-line emission scenario. While measurement data provides useful information on global fluxes and regional CH3Br seasonal cycles, small differences between the simulated seasonal cycles of different emission scenarios makes it difficult to distinguish between the relative likelihoods of model scenarios containing a tropical vegetation source or an increased biomass burning source. Further measurements performed in continental mid-to-high northern latitudes, central-southern Africa and South America would be of particular benefit in future attempts to constrain the location and magnitude of the natural terrestrial sources of methyl bromide.

On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that the modelling of the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

Fast Ozone Loss Around the Polar Vortex During 2002/2003 Arctic Winter Deep Minihole Event

A three-dimensional (3D) off-line chemical transport model (CTM) has been used to study an Arctic ozone minihole event in early December 2002, when the meteorological conditon were severely colder than in recent years. The minimum temperatures were below 188 K on 6 December 2002 and remained below 195 K for the entire month. Such temperatures are low enough for the formation of PSCs (polar stratospheric clouds) which were observed by a visible/near infrared solar occultation instrument by the Polar Ozone and Aerosol Measurement (POAM) III experiment. The SLIMCAT model compares well with the depth and evolution of the ozone distribution as observed by the second European Remote Sensing Satellite (ERS-2) Global Ozone Monitoring Experiment (GOME). The combined effect of a very strong and large intrusion of sub-tropical air, and uplifting of air masses of low ozone concentrations from the troposphere plays important role in the fomation of the ozone minihole. The modelled chemical ozone loss rate was relatively fast in the lower stratosphere in the region of frequent PSCs and higher levels of ClO and BrO. The observed PSCs in the vicinity of the minihole supports the model-predicted location of PSCs and chlorine activation. However, ozone miniholes have been attributed almost entirely to dynamical effects due to its short duration.

Global Model Simulations of the Transport of Asian and Sahara Dust: Total Deposition of Dust Mass in Japan

We simulated the global transport of dust emitted from all major dust source regions on earth by using a global three-dimensional chemical transport model for the year 2000. A modified dust emission flux scheme and an advanced nonlocal diffusion scheme for accurately determining the atmospheric eddy diffusivity in the atmospheric boundary layer were implemented to improve the chemical transport model. We specifically examined and analyzed dust storms that occurred in China and northern Africa. Four scenarios representing the global transport of dust from dust storms originating in the Loess region and the Gobi, Takla Makan, and Sahara deserts, respectively, were simulated. The results of each scenario were then compared with those resulting from all major dust source regions on earth, to identify which deserts have a major impact on dust transport and its deposition in Japan. The dust from the Sahara desert, most from the western part that was found in this study, reached Japan in 9–10 days, while Gobi and Loess region dust took 2 to 3 days, and 4 days for Takla Makan dust. The model-calculated monthly total deposition of dust mass from all major dust source regions was compared with comprehensive measurements of total deposition collected at sampling stations distributed over Japan, and good agreement was generally found. From these analyses, it was also indicated that dust emitted from other deserts, including the Turkestan, Iranian, and Arabian, could have a significant impact on dust deposition on Japan.

Predictability of Total Ozone Using a Global Three-Dimensional Chemical Transport Model Coupled with the MRI/JMA98 GCM

Abstract A global three-dimensional chemical transport model is being developed for forecasting total ozone. The model includes detailed stratospheric chemistry and transport and couples with a dynamical module of the Meteorological Research Institute/Japan Meteorological Agency 1998 (MRI/JMA98) general circulation model, which can yield realistic atmospheric fields through a meteorological assimilation system. Its predictability on total ozone is investigated for up to 4 weeks from 1997 to 2000. Global root-mean-square errors (rmses) of a control run are approximately 10 DU (3% of total ozone) throughout a year; the control run results are used as initial values for hindcast experiments. Rmses of the hindcast experiments globally range from 10 to 30 DU. The anomaly correlation between the 5-day forecasts and satellite measurements is approximately 0.6 throughout a year in the mid- and high latitudes of both the Northern and Southern Hemispheres. Thus, the model has potential for utilization on total ozone forecasts up to 5 days. In the northern mid- and high latitudes, the model produces better total ozone forecasts than the persistence up to 2 weeks, indicating that the deterministic limit of the total ozone forecasts is durationally comparable to that of weather forecasts. Good correlations between changes in total ozone and 100-hPa geopotential height reveal that the predictability of the dynamical field in the lower stratosphere critically affects the predictability of total ozone.