Sulfur dioxide and dimethyl sulfide in the central Pacific troposphere

Boundary-layer and free-troposphere measurements of sulfur dioxide, dimethyl sulfide, and carbon disulfide were made during transits of the central and southern Pacific Ocean between Hawaii and Australia. Sulfur dioxide was generally less than 100 pptv and highly variable with no correlation with respect to geographic location or altitude. Dimethyl sulfide in the boundary layer had a concentration range of <10 to 200 pptv. Highest concentrations of DMS were in the equatorial region of the southern hemisphere although the concentrations were dependent on location and meteorological regime. In the region of the Fiji Islands several boundary layer samples had SO₂, DMS, and CS₂. In 1989, additional SO₂ measurements were made between Hawaii and the equator and to the west of Hawaii downwind of the Kilauea volcano plumes.Paper submitted to the 7th International Symposium of the Commission for Atmospheric Chemistry and Global Pollution on the Chemistry of the Global Atmosphere held in Chamrousse, France, from 5 to 11 September 1990.     

Modelling of aerosol processes in plumes

A modelling platform for studying photochemical gaseous and aerosol phase processes from localized (e.g., point) sources has been presented. The current approach employs a reactive plume model which extends the regulatory model RPM‐IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, nitrate, ammonium material of aerosols are treated and attributed to the PM size distribution. A modified version of the carbon bond IV chemical mechanism is included to model the formation of organic aerosol. Aerosol dynamics modeled include mechanisms of nucleation, condensation, dry deposition and gas/particle partitioning of organic matter. The model is first applied to a number of case studies involving emissions from point sources and sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions. In addition, the model is compared with field data from power plant plumes with satisfactory predictions against gaseous species and total sulphate mass measurements. Finally, the plume model is applied to study secondary organic matter formation due to various emission categories such as vehicles and the oil production sector.     

Fluxes,sizes, morphology and compositions of particles in the Mt. Erebus volcanic plume,December 1983

Use of an airborne quartz crystal microbalance cascade impactor instrument together with a correlation spectrometer has allowed the flux of particles and their size distribution to be determined at Mount Erebus. The plume contributes 21±3 metric tomnes/day of aerosol particles to the Antarctic upper troposphere. The aerosol particles consist of larger (5–25 m) particles of elemental sulfur and silica, a middle sized group of iron oxides and smaller particles (less than 1 m) of complex liquids. Unlike many volcanic plumes, the Erebus plume has only a small amount of sulfate particles. The concentrations of particles in the Erebus plumes was 70–370 m/m³. Limited sampling of the Antarctic atmosphere at 8 km altitude but hundreds of km away from Erebus obtained a few large particles of sulfur and silicates, suggesting a similarity with the Erebus plume. The fallout of these particles occurs slowly over a broad area of the Antarctic continent.     

Desert dust aerosol air mass mapping in the western Sahara, using particle properties derived from space-based multi-angle imaging

Coincident observations made over the Moroccan desert during the Sahara mineral dust experiment (SAMUM) 2006 field campaign are used both to validate aerosol amount and type retrieved from multi-angle imaging spectroradiometer (MISR) observations, and to place the suborbital aerosol measurements into the satellite's larger regional context. On three moderately dusty days during which coincident observations were made, MISR mid-visible aerosol optical thickness (AOT) agrees with field measurements point-by-point to within 0.05–0.1. This is about as well as can be expected given spatial sampling differences; the space-based observations capture AOT trends and variability over an extended region. The field data also validate MISR's ability to distinguish and to map aerosol air masses, from the combination of retrieved constraints on particle size, shape and single-scattering albedo. For the three study days, the satellite observations (1) highlight regional gradients in the mix of dust and background spherical particles, (2) identify a dust plume most likely part of a density flow and (3) show an aerosol air mass containing a higher proportion of small, spherical particles than the surroundings, that appears to be aerosol pollution transported from several thousand kilometres away.     

Meteorological responses to Mt. Baekdu volcanic eruption over east asia in an offline global climate-chemistry model: A pilot study

We examine the meteorological responses due to the probable eruption of Mt. Baekdu using an off-line Climate-Chemistry model that is composed of the National Center for Atmospheric Research (NCAR) Climate Atmosphere Model version 3 (CAM3) and a global chemistry transport model (GEOS-Chem). Using the aerosol dataset from the GEOS-Chem driven by GEOS-5 meteorology, experiment and control simulations of the climate model are performed and their meteorological differences between the two simulations are analyzed. The magnitudes of volcanic eruption and column injection height were presumably set to 1/200 of the Mt. Pinatubo eruption and 9 km, respectively. Significant temperature drop in the lower troposphere (850 hPa), which is mainly due to a direct effect of prescribed volcanic aerosols from Mt. Baekdu, has been simulated up to about ?4 K. The upper atmosphere (150 hPa) right above the volcano, however, shows significant warming due to the absorption of the infrared radiation by volcanic aerosols. As a result of the volcanic eruption in the climate model, wave-like patterns are shown in both the geopotential height and horizontal wind. The changes in the lower atmospheric temperature are well associated with the modification of the atmospheric circulation through the hydrostatic balance. In spite of limitations in our current simulations due to several underlying assumptions, our results could give a clue to understanding the meteorological impacts from Mt. Baekdu eruptions that are currently attracting considerable public attention.     

Transformation of Aerosol Chemical Properties due to Transport Over a City

The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.     

源项对FLEXPART模式模拟福岛核事故放射性物质长距离传输的影响

对包括拉格朗日粒子模式在内的大气扩散模式,提供准确的源项有助于获取更好的模拟结果。以日本福岛核电站2011年3月发生的核泄漏事故为研究对象,采用日本原子能机构Terada源项以及挪威大气研究所Stohl源项,利用FLEXPART(FLEXible PARTicle dispersion mode)模拟了放射性物质137Cs在全球大气中扩散传输的过程,并利用大气辐射监测数据讨论了基于两种源项模拟烟云的时空分布特征,探讨了源项对模拟结果的不确定性影响。结果显示:Terada源项及Stohl源项之间释放总量、释放速率、释放高度等虽然略有差别,但总体趋势描述相似,使得基于两源项的模拟烟云的扩散过程及影响区域基本一致。两模拟烟云在中纬度西风带作用下,均表现为自西向东扩散,经过太平洋、美洲大陆、欧洲,最后在整个北半球传输。基于两源项在亚洲—太平洋及北美大陆等近距离的模拟烟云的首次到达时间与首次监测时间吻合度较好,在全球尺度上基于Stohl源项的模拟在首次到达时间方面表现更优。其次,基于两源项进行全球尺度的模拟,近距离站点的模拟效果优于远距离站点模拟效果,且基于Stohl源项的模拟精度较好,Terada源项可能存在低估。另外模式进行全球尺度的模拟时,针对不同粒子数目对模拟结果的影响进行了分析,发现粒子数目的多寡对模拟精度有所影响,也影响模拟烟云扩散后期的疏密程度。     

The Northern Path of Asian Dust Transport from the Gobi Desert to North America

The aerosol index (AI) of the Total Ozone Mapping Spectrometer (TOMS) satellite data (1979 2001) was analyzed to reveal the climatological long-distance path of dust transport from Asia to North America. The AI in the west coast of the United States is highly correlated with that in the Gobi desert. Additionally, from the TOMS satellite images, it can be seen that very strong plumes advect from Asia to the west coast of North America in typical dust storm cases. When applying the sourcereceptor relationship to detect the northern dust transport path between the Gobi source region and the west coast of the United States receptor region, it is evident that the dust plume can be transported northward beyond 60°N from its source region and that it takes 5 to 6 days to reach the west coast of the United States. The cross correlation technique shown in this work is a useful tool that can be applied in other regions to give useful insights into relationships between major dust sources and downwind receptor locations by using remotely sensed dust observations.     

A similarity model for maximum ground-level concentration in a freely convective atmospheric boundary layer

A model of buoyancy- and momentum-driven industrial plumes in a freely convective boundary layer is proposed. The development combines the Lagrangian similarity models of Yaglom for non-buoyant releases in the convective surface layer with the Scorer similarity model for industrial plumes. Constraints on the validity of the extension of Yaglom’s model to the entire convective planetary boundary layer, arrived at by consideration of Batchelor’s formulation for diffusion in an inertial subrange, are often met in practice. The resulting formulation applies to an interval of time in which the entrainment of the atmosphere by the plume is balanced by the entrainment of the plume by the atmosphere. It is argued that during this interval, both maximum plume rise and ground contact are achieved. Further examination of the physical interrelationship with the Csanady-Briggs formulation serves to consolidate the model hypotheses, as well as to simplify the derivation of maximum ground-level concentrations. Experimental evidence is presented for the validity of the model, based on Moore’s published data.     

A Similarity Model for Maximum Ground-Level Concentration in a Freely Convective Atmospheric Boundary Layer

A model of buoyancy- and momentum-driven industrial plumes in a freely convective boundary layer is proposed. The development combines the Lagrangian similarity models of Yaglom for non-buoyant releases in the convective surface layer with the Scorer similarity model for industrial plumes. Constraints on the validity of the extension of Yaglom’s model to the entire convective planetary boundary layer, arrived at by consideration of Batchelor’s formulation for diffusion in an inertial subrange, are often met in practice. The resulting formulation applies to an interval of time in which the entrainment of the atmosphere by the plume is balanced by the entrainment of the plume by the atmosphere. It is argued that during this interval, both maximum plume rise and ground contact are achieved. Further examination of the physical interrelationship with the Csanady-Briggs formulation serves to consolidate the model hypotheses, as well as to simplify the derivation of maximum ground-level concentrations. Experimental evidence is presented for the validity of the model, based on Moore’s published data.     

A one-dimensional model for the parameterization of deep convection in the ocean

A one-dimensional penetrative plume model has been constructed to parameterize the process of deep convection in ocean general circulation models (OGCMs). This research is motivated by the need for OGCMs to better model the production of deep and intermediate water masses. The parameterization scheme takes the temperature and salinity profiles of OGCM grid boxes and simulates the subgrid-scale effects of convection using a one-dimensional parcel model. The model moves water parcels from the surface layer down to their level of neutral buoyancy, simulating the effect of convective plumes. While in transit, the plumes exchange water with the surrounding environment; however, the bulk of the plume water mass is deposited at e level of neutral buoyancy. Weak upwelling around the plumes is included to maintain an overall mass balance. The process continues until the negative buoyant energy of the one-dimensional vertical column is minimized. The parameterized plume entrainment rate, which plays a central role in the parameterization, is calculated using modified equations based on the physics of entraining buoyant plumes. This scheme differs from the convective adjustment techniques currently used in OGCMs, because the parcels penetrate downward with the appropriate degree of mixing until they reach their level of neutral stability.     

大气气溶胶的垂直非均一对向上亮度和卫星遥感地表反射率的效应

均一模式和两层模式是两个忽略气溶胶垂直非均一、并广泛用于卫星遥感的辐射模式。通过两个模式的数值模拟，分析了气溶胶的垂直非均一对向上天空亮度和卫星遥感地面反射率的效应。数值模拟选用了２４个有代表性的气溶胶模式。对于具有强分子散射的卫星短波通道，由于分子和气溶胶散射性的明显不同，应用均一和两层模式计算的向上亮度往往存在较大误差。对长波通道，如果气溶胶的光学特性随高度变化不大，该亮度误差较小，但如果存在不同散射相函数和一次散射反照率的气溶胶层，该误差仍可能较大。对于干净的大气，由均一和两层模式计算的亮度误差可分别高达３１．４％和３１．５％，而对于混浊的大气，该误差可分别高达６７．８％和５９．２％。该亮度误差可以引起地表反射率解存在大的不确定性，特别是对于短波通道和强吸收的气溶胶。对于包含强吸收气溶胶的混浊大气，均一和两层模式不适合于大气订正应用。     

On the Retrieval of Volcanic Sulfur Dioxide Emissions from GOME Backscatter Measurements

We focus on the retrieval of volcanic sulfur dioxide (SO₂) emissions from an analysis of atmospheric UV backscatter spectra obtained by the Global Ozone Monitoring Experiment (GOME) spectrometer on board the ESA European Remote Sensing Satellite (ERS-2). Here, the last major eruptions of Mt. Etna on Sicily (Italy) in July/August 2001 and October/November 2002 provided an excellent opportunity to study the retrieval of SO₂ columnar amounts from ground-based, LIDAR and satellite measurements. Our study shows that the bulk of emitted SO₂ was confined in the troposphere, mainly between 700 hPa and 400 hPa which is confirmed by trajectory analysis, by LIDAR observations and AVHRR observations. The area of influence of Mt. Etna eruptions ranges from the Western Saharan Desert to Greece and the near east states and even down to the basin of Tschad, Africa. Our analysis revealed that information about the plume height of volcanic eruptions and aerosol parameters is necessary for a reliable quantitative retrieval of SO₂ from space-borne sensor data at periods perturbed by volcanic eruptions.     

Specifying the atmospheric pollutant distribution forecast using the mathematical modeling and measurement data

Considered is a possibility of specifying the forecast of volcanic aerosol distribution in the atmosphere using the data of ground-based actinometric measurements. To simulate the aerosol distribution, the FlexPart software (Norwegian Institute for Air Research) was used. Using the FlexGraph software (Planeta Research Center for Space Hydrometeorology), the visualization and interactive analysis were carried out of aerosol concentration fields at different time moments. The prognostic concentration of volcanic ash from Grímsvötn volcano (May 2011) is bound to the results of measurements of aerosol optical depth in Hamburg at one of the points of AERONET global network. The comparison of the corrected aerosol concentration with the measurements at other AERONET points demonstrated the competence of the proposed approach. To specify the aerosol cloud distribution forecast on the territory of Russia, the Roshydromet actinometric network data can be used.     

Intercomparison of Two Box Models of the Chemical Evolution in Biomass-Burning Smoke Plumes

Results from two independently developed biomass-burning smoke plume models are compared. Model results were obtained for the temporal evolution of two nascent smoke plumes originating from significantly different fire environments (an Alaskan boreal forest and an African savanna). The two smoke plume models differed by 1%–10% for [O₃], with similar differences for NO _x and formaldehyde (relative percent differences). Smaller intermodel differences were observed for the African savanna smoke plume as compared to the plume from the Alaskan boreal fire. Mechanistic differences between the models are heightened for the Alaskan smoke plume due to the higher VOC emission ratios as compared to the African savanna fire. The largest deviations result from the differences in oxidative photochemical mechanisms, with a smaller contribution attributable to the calculation of photolysis frequencies. The differences between the two smoke plume models are significantly smaller than the uncertainties of available photokinetic data or field measurements. Model accuracy depends most significantly on having the fullest possible VOC data, a requirement that is constrained by currently available instrumentation.     

Volcanos and El Niño: signal separation in Northern Hemisphere winter

The frequent coincidence of volcanic forcing with El Niño events disables the clear assignment of climate anomalies to either volcanic or El Niño forcing. In order to select the signals, a set of four different perpetual January GCM experiments was performed (control, volcano case, El Niño case and combined volcano/El Niño case) and studied with advanced statistical methods for the Northern Hemisphere winter. The results were compared with observations. The signals for the different forcings are discussed for three variables (temperature, zonal wind and geopotential height) and five levels (surface, 850 hPa, 500 hPa, 200 hPa and 50 hPa). The global El Niño signal can be selected more clearly in the troposphere than in the stratosphere. In contrast, the global volcano signal is strongest in the stratospheric temperature field. The amplitude of the perturbation for the volcano case is largest in the Atlantic region. The observed effect of local cooling due to the volcanic reduction of shortwave radiation over large land areas (like Asia) in subtropical regions, the observed advective warming over Eurasia and the advective cooling over Greenland are well simulated in the model. The radiative cooling near the surface is important for the volcano signal in the subtropics, but it is weak in high latitudes during winter. A statistically significant tropospheric signal of El Niño forcing occurs in the subtropics and in the midlatitudes of the North Pacific. The local anomalies in the El Niño forcing region in the tropics, and the warming over North America in middle and high latitudes are simulated as observed. The combined signal is different from a simple linear combination of the separate signals. It leads to a climate perturbation stronger than for forcing with El Niño or stratospheric aerosol alone and to a somewhat modified pattern.     

火山喷发对气候影响信号的检测

该文从时序叠加和序列分析两个方面系统地评述了近年来火山活动影响气候的研究进展和代表性工作。给出了火山活动特征，如火山喷发强度、喷发位置和季节等对气候影响的时空分布规律。讨论了与之有关的几个重要问题，如火山指标，火山活动影响气候的途径及其和ENSO的联系等。最后指出了今后研究的几个方向。     

Numerical Study of Dual-Plume Interference in a Turbulent Boundary Layer

Direct numerical simulation is used to investigate the interference arising from the dispersion of passive scalar plumes released from a pair of point sources in a fully-developed wall-bounded shear flow. Four different lateral separations of the two sources for both near ground-level and elevated releases are considered. The downwind evolution of the correlation between the plume concentrations along the centreline between the two sources and the behaviour of the lateral profiles of the correlation at various locations downwind of the two sources are examined in detail. Differences in the exceedance probability over a high concentration level for a single plume and the total plume are highlighted and studied, and the effects of destructive and constructive interferences on the exceedance probabilities for the total plume are used to explain these differences. One significant result is that all higher-order (third-order and above) moments of the total concentration can be inferred from the application of a clipped-gamma distribution using the information embodied in only the first- and second-order concentration moments of each single plume, and in the cross-correlation coefficient of the instantaneous concentration of the two plumes.     

A Model for the Transport of Sea-Spray Aerosols in the Coastal Zone

We study the dynamics of sea-spray particles in the coastal region of La Reunion Island on the basis of numerical simulations using the transport aerosol model MACMod (Marine Aerosol Concentration Model) and a survey of the aerosol size distributions measured at four locations at two different heights in the north-west part of the island. This allows evaluation of the performance of our model in case of pure marine air masses with implementation of accurate boundary conditions. First of all, an estimate of the aerosol concentration at 10-m height at the upwind boundary of the calculation domain is obtained using a revisited version of the MEDEX (Mediterranean Extinction) model. Estimates of the vertical profile of aerosol concentrations are then provided using aerosol data obtained at two different heights at the upwind boundary of the calculation domain. A parametrization of the vertical profiles of aerosol concentrations for maritime environment is proposed. The results are then compared to the vertical profiles of 0.532 \(\upmu \)m aerosol particle extinction coefficient obtained from lidar data provided by the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) and also to the data provided by the Aerosol Robotic Network (AERONET). This allows validation of the complete vertical profiles in the mixed layer and shows the validity of satellite data for determination of the vertical profiles. Two kinds of simulation were made: one without a particle advection flux at the upwind boundary of the numerical domain, whereas the second simulation was made with a particle advection flux. In the first case, the influence of the distance to the shoreline on the local sea-spray dynamics is investigated. In the second set of simulation, the particles issued from the local production in the surf zone near the shoreline are mixed with aerosols advected from the remote ocean. A good agreement between the model calculations using our boundary conditions and the data was found. The present results then attest the ability of this kind of model, as a first approach to predicting the local transport of sea-spray particles in a pure marine environment.     

A case study of the direct radiative effect of biomass burning aerosols on precipitation in the Eastern Amazon

Numerical experiments with the Brazilian additions to the Regional Atmospheric Modeling System were performed with two nested grids (50 and 10 km horizontal resolution, respectively) with and without the effect of biomass burning for 8 different situations for 96 h integrations. Only the direct radiative effect of aerosols is considered. The results were analyzed in large areas encompassing the BR163 road (one of the main areas of deforestation in the Amazon), mainly where most of the burning takes place. The precipitation change due to the direct radiative impact of biomass burning is generally negative (i.e., there is a decrease of precipitation). However, there are a few cases with a positive impact. Two opposite forcing mechanisms were explored: (a) the thermodynamic forcing that is generally negative in the sense that the aerosol tends to stabilize the lower atmosphere and (b) the dynamic impact associated with the low level horizontal pressure gradients produced by the aerosol plumes. In order to understand the non-linear relationship between the two effects, experiments were performed with 4-fold emissions. In these cases, the dynamic effect overcomes the stabilization produced by the radiative forcing and precipitation increase is observed in comparison with the control experiment. This study suggests that, in general, the biomass burning radiative forcing decreases the precipitation. However, very large concentrations of aerosols may lead to an increase of precipitation due to the dynamical forcing associated with the horizontal pressure gradients.