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1.
Satellite observations of atmospheric CO2 are able to truly capture the variation of global and regional CO2 concentration.The model simulations based on atmospheric transport models can also assess variations of atmospheric CO2 concentrations in a continuous space and time,which is one of approaches for qualitatively and quantitatively studying the atmospheric transport mechanism and spatio-temporal variation of atmospheric CO2 in a global scale.Satellite observations and model simulations of CO2 offer us two different approaches to understand the atmospheric CO2.However,the difference between them has not been comprehensively compared and assessed for revealing the global and regional features of atmospheric CO2.In this study,we compared and assessed the spatio-temporal variation of atmospheric CO2 using two datasets of the column-averaged dry air mole fractions of atmospheric CO2(XCO2)in a year from June 2009 to May 2010,respectively from GOSAT retrievals(V02.xx)and from Goddard Earth Observing System-Chemistry(GEOS-Chem),which is a global 3-D chemistry transport model.In addition to the global comparison,we further compared and analyzed the difference of CO2 between the China land region and the United States(US)land region from two datasets,and demonstrated the reasonability and uncertainty of satellite observations and model simulations.The results show that the XCO2 retrieved from GOSAT is globally lower than GEOS-Chem model simulation by 2 ppm on average,which is close to the validation conclusion for GOSAT by ground measures.This difference of XCO2 between the two datasets,however,changes with the different regions.In China land region,the difference is large,from 0.6 to 5.6 ppm,whereas it is 1.6 to 3.7 ppm in the global land region and 1.4 to 2.7 ppm in the US land region.The goodness of fit test between the two datasets is 0.81 in the US land region,which is higher than that in the global land region(0.67)and China land region(0.68).The analysis results further indicate that the inconsistency of CO2concentration between satellite observations and model simulations in China is larger than that in the US and the globe.This inconsistency is related to the GOSAT retrieval error of CO2 caused by the interference among input parameters of satellite retrieval algorithm,and the uncertainty of driving parameters in GEOS-Chem model.  相似文献   

2.
A high-accuracy surface modeling (HASM) method based on the fundamental theorem of surfaces, is developed to simulate XCO2 surfaces using the GOSAT retrieval XCO2 data. Two tests are designed to investigate the simulation accuracy. The first test divides the existing satellite retrieval XCO2 data into training points and testing points, and simulates the XCO2 surface using the training points while computing the simulation error using the testing points. The absolute mean error (MAE) of the testing points is 1.189 ppmv, and the corresponding values of the comparison methods, Ordinary Kriging, IDW, and Spline are 1.203, 1.301, and 1.355 ppmv, respectively. The second test simulates the XCO2 surface using all the satellite retrieval points and uses the TCCON (Total Carbon Column Observing Network) site observation values as the ture values. For the six typical TCCON sites, the HASM simulation MAE is 1.688 ppmv, and the satellite retrieval MAE at the same sites is 2.147 ppmv. These results indicate that HASM can successfully simulate XCO2 surfaces based on satellite retrieval data.  相似文献   

3.
The spectra of O_2 A-band(0.76 μm) and CO_2 near-infrared emissions(1.6 μm) are simulated by the SCIATRAN radiative transfer model(V3.1.23), and compared with those observed by GOSAT-FTS(Greenhouse gases Observing SATellite-Fourier Transform Spectrometer). Systematic deviations between the observed and simulated spectra are found to exist,especially for the O_2 A-band. The discrepancies are characterized by their mean differences averaged over the observed spectral ranges. A correction is applied to the observed GOSAT-FTS L1B(V141.141) spectra by scaling the spectral intensity measured by TANSO-FTS(Thermal and Near infrared Sensor for carbon Observation Fourier Transform Spectrometer) onboard GOSAT.The average columnar CO_2 concentrations(XCO_2) are retrieved from the observed and the corrected GOSAT-FTS spectra by using the SCIATRAN inversion algorithm. Compared with the GOSAT-FTS L2 XCO_2 data products retrieved from the observed spectra of GOSAT-FTS, the SCIATRAN retrievals from the corrected spectra show a much better agreement, with the relative error less than 1%. But the results of GOSAT TANSO-FTS(V161.160) show smaller residuals than GOSAT TANSO-FTS(V141.141) without mean residual correction. The results indicate that the mean residual correction would increase the precision of XCO_2 retrieval for spectra with systematic deviations.  相似文献   

4.
Atmospheric SO2 has a significant impact on the urban environment and global climate. Band Residual Difference Algorithm (BRD) and Differential Optical Absorption Spectroscopy (DOAS) were used respectively by NASA and ESA science team to derive SO2 columns from satellite observations, but there are few studies on the comparison and validation of BRD and DOAS SO2 retrievals under the same observation conditions. In this study, the radiative transfer model SCIATRAN was firstly used to validate the accuracies of BRD and DOAS SO2 retrievals, and analyse the uncertainty of SO2 retrieval caused by band selection, O3 absorption, aerosol, surface reflectance, solar and viewing zenith angle. Finally, BRD and DOAS algorithms were applied to the same radiances from satellite observations, and comparisons of BRD and DOAS SO2 retrievals were conducted over volcanic eruption and North China. Results show that, for the case with low SO2 columns, BRD SO2 retrievals have higher retrieval accuracy than DOAS, but typical seasonal variation with high SO2 column in winter and low in summer can be more clearly discernible in DOAS SO2 retrievals than BRD from satellite observations. For the case with high SO2 columns, the differences between BRD (310.8–314.4 nm) and DOAS (315–327 nm) retrievals are large, and the value and accuracy of BRD (310.8–314.4 nm) SO2 retrievals are lower than those of DOAS (315–327 nm) retrievals. Compared with the SO2 inputs in forward model, both BRD (310.8–314.4 nm) and DOAS (315–327 nm) SO2 retrievals are underestimated for the case with high SO2 columns. The selection of wavelength range can significantly affect the accuracy of SO2 retrieval. The error of BRD SO2 retrieval from 310.8–314.4 nm is lower than other bands in the ultraviolet spectral region (306–327 nm). The increase of wavelength in the ultraviolet spectral region 306–330 nm can reduce the underestimation of DOAS SO2 retrievals in the case of high SO2 column, but slight overestimation of SO2 retrieval is found from the 315–327 nm range in the case of low SO2 column. The values of BRD and DOAS SO2 retrieval decrease with atmospheric O3 column and aerosol optical depth increasing, but increase with surface reflectance increasing. Large solar zenith angle and viewing zenith angle can introduce more errors to the BRD and DOAS SO2 retrievals. This study is important for the improvement of retrieval algorithm and the application of SO2 products from satellite observations.  相似文献   

5.
A numerical simulation was conducted to predict the change of pCO2 in the ocean caused by CO2 leaked from an underground aquifer, in which CO2 is purposefully stored. The target space of the present model was the ocean above the seafloor. The behavior of CO2 bubbles, their dissolution, and the advection-diffusion of dissolved CO2 were numerically simulated. Here, two cases for the leakage rate were studied: an extreme case, 94,600 t/y, which assumed that a large fault accidentally connects the CO2 reservoir and the seafloor; and a reasonable case, 3800 t/y, based on the seepage rate of an existing EOR site. In the extreme case, the calculated increase in ΔpCO2 experienced by floating organisms was less than 300 ppm, while that for immobile organisms directly over the fault surface periodically exceeded 1000 ppm, if momentarily. In the reasonable case, the calculated ΔpCO2 and pH were within the range of natural fluctuation.  相似文献   

6.
We propose an algorithm that combines a pre-processing step applied to the a priori state vector prior to retrievals, with the modified damped Newton method (MDNM), to improve convergence. The initial constraint vector pre-processing step updates the initial state vector prior to the retrievals if the algorithm detects that the initial state vector is far from the true state vector in extreme cases where there are CO2 emissions. The MDNM uses the Levenberg-Marquardt parameter γ, which ensures a positive Hessian matrix, and a scale factor α, which adjusts the step size to optimize the stability of the convergence. While the algorithm iteratively searches for an optimized solution using observed spectral radiances, MDNM adjusts parameters γ and α to achieve stable convergence. We present simulated retrieval samples to evaluate the performance of our algorithm and comparing it to existing methods. The standard deviation of our retrievals adding random noise was less than 3.8 ppmv. After pre-processing the initial estimate when it was far from the true value, the CO2 retrieval errors in the boundary layers were within 1.2 ppmv. We tested the MDNM algorithm’s performance using GOSAT L1b data with cloud screening. Our preliminary validations comparing the results to TCCON FTS measurements showed that the average bias was less than 1.8 ppm and the correlation coefficient was approximately 0.88, which was larger than for the GOSAT L2 product.  相似文献   

7.
Submersible observations and sampling were carried out in the rift valley of the Mid-Atlantic Ridge (MAR) near 34°40′N–35°N. The 4-km-wide rift valley consists of a Neo Volcanic Zone (NVZ) (<1 km wide) bounded at the west by a Median Ridge (MR) (5 km wide and 20 km long) and at the east by the first scarps of the eastern wall. The MR and the eastern wall are characterized by volcanic cones about 200–300 m height culminating at depths of 1500–1900 m which are made up of volcaniclastic deposits (pyroclasts and hyaloclasts) suggestive of explosive volcanism. Based on their surface morphology, degree of vesicularity, and composition, the erupted deposits are classified into four groups: (1) poorly vesicular (<15% vesicles) N- and T-MORBs (K/Ti <0.25, Na2O+K2O<2.9%) consisting of sheet flows and pillows formed during fissure eruptions in the NVZ at 2000–2300 m depths; (2) vesicular (15–30% vesicles) E-MORBs (K/Ti=0.25−0.45,Na2O+K2O>2.8−3.2%) and alkali basalts (K/Ti=0.45−0.70,Na2O+K2O>3.3−4) made up mainly of pillows; (3) highly vesicular (>35% vesicles) pillow lava and pyroclastic (scoria-like) alkali basalts (K/Ti>0.45−0.80,Na2O+K2O>3−4%); and (4) hyaloclastites consisting of glassy shards of alkali basalt composition. The total water and carbon contents of the deposits increase with the incompatible element concentrations. The estimated initial H2O content for the N- and T-MORBs is less than 3500 ppm, whereas for the E-MORBs and alkali basalts the H2O content is near 4000 and 7000 ppm, respectively. While the H2O is mainly in the melt, the carbon is in the form of CO2 filling vesicles. The vesicles are formed from magma with an initial carbon content of 1000–3000 for the N- and T-MORBs, 3000–6500 ppm for the E-MORBs and higher than 1 wt% for the alkali basalts.The various lava types were derived from a heterogeneous mantle source composed of enriched and depleted components during sequential eruptions of N-, T- and E-MORBs and alkali basalts (K/Ti>0.7). The amount of CO2 and H2O in equilibrium with the dissolved species present in the vesicles indicates that CO2 (XCO2=1−0.84) was the main exsolved compound responsible for bubble nucleation. The increase in the degree of vesicularity and pressure of the volatile phases is mainly due to the early exsolution of CO2 from an alkali melt. The exsolution of significant amounts of dissolved water occurred only for the alkali basalt a few hundred meters beneath the seafloor and contributed to late bubble expansion. This subsequent addition of magmatic water to the vesicles increased the gas pressure and triggered explosions. An alternative hypothesis for the explosive volcanism is based on field observations. During crater collapsed, seawater could have been trapped in fractured volcanic conduits and later sealed by hydrothermal fluid circulation and precipitation. In such an environment, this seawater will be heated and vaporized during renewed magmatic upwelling. Both scenarios give rise to fragmented debris (hyaloclasts and pyroclasts) and the explosive events create turbulent flows followed by differential gravity settling of the particles (shards versus lapilli) through the seawater.  相似文献   

8.
胡季平  陈德玲 《湖泊科学》1995,7(2):185-190
藏北高原恶劣的自然地理条件使扎仓茶－卡珍贵的锂资源的开发极为困难,必须采用尽可能简化的提取工艺才能降低成本,本文提出了一种经ＣａＯ,（ＮＨ４）２Ｃ２Ｏ４和Ｎａ２ＣＯ３三步沉积得到粗Ｌｉ２ＣＯ３的简化工艺,其产品纯度可达８５．６２％,总回收率约２０％,卤旦回收率约为７６％。  相似文献   

9.
The long-term effect of elevated CO2 concentrations on needle dark respiration of two coniferous species-Pinus koraiensis and Pinus sylvestriformis on the Changbai Mountain was investigated using open-top chambers. P. Koraiensis and P. Sylvestriformis were exposed to 700,500μmol·mol-1 CO2 and ambient CO2(approx.350 μmol·mol-1)for four growing seasons. Needle dark respiration was measurd during the second, third and fourth growing seasons' exposure to elevated CO2.The results showed that needle dark respiration rate increased for P. Koraiensis and P. Sylvestriformis grown at elevated CO2 concentrations during the second growing season, could be attributed to the change of carbohydrate and/or nitrogen content of needles. Needle dark respiration of P. Koraiensis was stimulated and that of P. Sylvestriformis was inhibited by elevated CO2 concentrations during the third growing season. Different response of the two tree species to elevated CO2 mainly resulted from the difference in the growth rate. Elevated CO2 concentrations inhibited needle dark respiration of both P. Koraiensis and P. Sylvestriformis during the fourth growing season. There was consistent trend between the short-term effect and the long-term effect of elevated CO2 on needle dark respiration in P. Sylvestriformis during the third growing season by changing measurement CO2 concentrations. However, the short-term effect was different from the long-term effect for P. Koraiensis. Response of dark respiration of P. Koraiensis and P. Sylvestriformis to elevated CO2 concentrations was related to the treatment time of CO2 and the stage of growth and development of plant. The change of dark respiration for the two tree species was determined by the direct effect of CO2 and long-term acclimation. The prediction of the long-term response of needle dark respiration to elevated CO2 concentration based on the short-term response is in dispute.  相似文献   

10.
Zusammenfassung Zwischen 50° bis 85°N Breite wurde die atmosphärische CO2-Konzentration während mehrerer Messflüge registriert. Diese war oberhalb der Tropopause bis zu 7 ppm (im Mittel etwa 2 ppm) niedriger als in der oberen Troposphäre. Im Jahresmittel entspricht diese CO2-Konzentrationsdifferenz einem Fluss von etwa 10–2 g CO2/cm2 Jahr aus der nördlichen Troposphäre in die Stratosphäre. Die Bedeutung dieser CO2-Konzentrationsunterschiede für den atmosphärischen CO2-Haushalt sowie für die Strahlungsbilanz im Tropopausenniveau kann erst nach Vorlage weiterer, über das ganze Jahr verteilter Messdaten erfolgen.
Summary CO2-concentration was measured during several flights in northern latitudes (50°–85°). Above Tropopause CO2-concentration was up to 7 ppm (as a mean some 2 ppm) smaller than in upper troposphere. As a mean this difference in CO2-concentration cm2 year conforms to a CO2-flux of some 10–2 g CO2/cm2 year from northern troposphere into stratosphere. The importance of these CO2-differences for atmospheric CO2-system and for radiation balance in tropopause-height may be considered as soon as more CO2-concentration data for the whole year are available.
  相似文献   

11.
Two year measurements of aerosol concentration and size distribution (0.25 μm < d < 30 μm) in the atmospheric surface layer, collected in L’Aquila (Italy) with an optical particle counter, are reported and analysed for the different modes of the particle size distribution. A different seasonal behaviour is shown for fine mode aerosols (largely produced by anthropogenic combustion), coarse mode and large-sized aerosols, whose abundance is regulated not only by anthropogenic local production, but also by remote natural sources (via large scale atmospheric transport) and by local sources of primary biogenic aerosols. The observed total abundance of large particles with diameter larger than 10 μm is compared with a statistical counting of primary biogenic particles, made with an independent technique. Results of these two observational approaches are analysed and compared to each other, with the help of a box model driven by observed meteorological parameters and validated with measurements of fine and coarse mode aerosols and of an atmospheric primary pollutant of anthropogenic origin (NOx). Except in winter months, primary biogenic particles in the L’Aquila measurement site are shown to dominate the atmospheric boundary layer population of large aerosol particles with diameter larger than 10 μm (about 80 % of the total during summer months), with a pronounced seasonal cycle, contrary to fine mode aerosols of anthropogenic origin. In order to explain these findings, the main mechanisms controlling the abundance and variability of particulate matter tracers in the atmospheric surface layer are analysed with the numerical box-model.  相似文献   

12.
The climate warming is mainly due to the increase in concentrations of anthropogenic greenhouse gases, of which CO2 is the most important one responsible for radiative forcing of the climate. In order to reduce the great estimation uncertainty of atmospheric CO2 concentrations, several CO2-related satellites have been successfully launched and many future greenhouse gas monitoring missions are planned. In this paper, we review the development of CO2 retrieval algorithms, spatial interpolation methods and ground observations. The main findings include: 1) current CO2 retrieval algorithms only partially account for atmospheric scattering effects; 2) the accurate estimation of the vertical profile of greenhouse gas concentrations is a long-term challenge for remote sensing techniques; 3) ground-based observations are too sparse to accurately infer CO2 concentrations on regional scales; and 4) accuracy is the primary challenge of satellite estimation of CO2 concentrations. These findings, taken as a whole, point to the need to develop a high accuracy method for simulation of carbon sources and sinks on the basis of the fundamental theorem of Earth’s surface modelling, which is able to efficiently fuse space- and ground-based measurements on the one hand and work with atmospheric transport models on the other hand.  相似文献   

13.
Magmatic gases extracted and analysed from basaltic rocks collected in the FAMOUS area near 36°50′ N in the Atlantic ocean show that the total amount of gas included in the samples varies between about 500 ppm to 1600 ppm. The main gaseous phases included in the various types of basalts consist of CO2 (270–700 ppm), CO (150–800 ppm), HCl (100–1000 ppm), H2 (0–50 ppm), SO2 (up to 175 ppm), N2 (up to about 213 ppm) and traces of hydrocarbons (up to about 24 ppm). The relative amount of CO, CO2 and SO2 varies with both the degree of crystallinity of the rock and with fractional crystallization and/or fractional melting. The glassy margin of pillow lavas have a higher CO/CO2 ratio than the more crystalline interior. The most fractionated rocks of the series rich in clinopyroxene are depleted in the CO/CO2 ratio and have a higher SO2 content than do the most mafic end members rich in olivine. Early-formed olivine was crystallized in a reducing environment rich in CO and H2 with respect to later formed mineral associations. It is likely that the carbon and sulfur oxidation is taking place at a relatively shallow depth during magmatic ascent or during volcanism. The ocean floor volcanics when compared to subaerial basalts are depleted in SO2 and have on the average ten times more H2.  相似文献   

14.
Solar geoengineering has been proposed as a potential mechanism to counteract global warming. Here we use the University of Victoria Earth System Model (UVic) to simulate the effect of idealized sunshade geoengineering on the global carbon cycle. We conduct two simulations. The first is the A2 simulation, where the model is driven by prescribed emission scenario based on the SRES A2 CO2 emission pathway. The second is the solar geoengineering simulation in which the model is driven by the A2 CO2 emission scenario combined with sunshade solar geoengineering. In the model, solar geoengineering is represented by a spatially uniform reduction in solar insolation that is implemented at year 2020 to offset CO2-induced global mean surface temperature change. Our results show that solar geoengineering increases global carbon uptake relative to A2, in particular CO2 uptake by the terrestrial biosphere. The increase in land carbon uptake is mainly associated with increased net primary production (NPP) in the tropics in the geoengineering simulation, which prevents excess warming in tropics. By year 2100, solar geoengineering decreases A2-simulated atmospheric CO2 by 110 ppm (12%) and causes a 60% (251 Pg C) increase in land carbon accumulation compared to A2. Solar geoengineering also prevents the reduction in ocean oxygen concentration caused by increased ocean temperatures and decreased ocean ventilation, but reduces global ocean NPP. Our results suggest that to fully access the climate effect of solar geoengineering, the response of the global carbon cycle should be taken into account.  相似文献   

15.
CO2 concentrations at depths of 15,30, and 50 cm were determined over a one-year period in six karst soils in the Malay peninsula. Evidence suggests that the highest single CO2 value (MAXCO2, per cent) recorded at each site/depth provides the best estimate of conditions during groundwater recharge events. Soil depth (cm) and bulk density (BDEN) are the best predictors of MAXCO2, with the equation loglo(MAXCO2) = 1·146 (BDEN) + 0·00698 (DEPTH) - 1·227 accounting for 86 per cent of the variation. This equation is used to model MAXCO2 at seven, more remote sites. Soil throughflow patterns and groundwater recharge points are estimated from slope pantometer and soil depth surveys in order to assess the CO2 concentration with which soil waters ultimately equilibrate before entering the limestone. Limestone weathering seems to be predominantly of the open system type, the overall mean MAXCO2 of 1·65 per cent corresponding with a weathering potential of 167 ppm CaCO3. Weathering potentials vary markedly, ranging from 62–82 ppm on rocky hilltops to more than 280 ppm on certain tower karst footslopes in Selangor and the Kinta Valley and on moderate hillslopes developed in impure limestones in the Boundary Range.  相似文献   

16.
We present new analyses of volatile, major, and trace elements for a suite of glasses and melt inclusions from the 85°E segment of the ultra-slow spreading Gakkel Ridge. Samples from this segment include limu o pele and glass shards, proposed to result from CO2-driven explosive activity. The major element and volatile compositions of the melt inclusions are more variable and consistently more primitive than the glass data. CO2 contents in the melt inclusions extend to higher values (167–1596 ppm) than in the co-existing glasses (187–227 ppm), indicating that the melt inclusions were trapped at greater depths. These melt inclusions record the highest CO2 melt concentrations observed for a ridge environment. Based on a vapor saturation model, we estimate that the melt inclusions were trapped between seafloor depths (～ 4 km) and ～ 9 km below the seafloor. However, the glasses are all in equilibrium with their eruption depths, which is inconsistent with the rapid magma ascent rates expected for explosive activity. Melting conditions inferred from thermobarometry suggest relatively deep (25–40 km) and cold (1240°–1325 °C) melting conditions, consistent with a thermal structure calculated for the Gakkel Ridge. The water contents and trace element compositions of the melt inclusions and glasses are remarkably homogeneous; this is an unexpected result for ultra-slow spreading ridges, where magma mixing is generally thought to be less efficient based on the assumption that steady-state crustal magma chambers are absent in these environments. All melts can be described by a single liquid line of descent originating from a pooled melt composition that is consistent with the aggregate melt calculated from a geodynamic model for the Gakkel Ridge. These data suggest a model in which deep, low degree melts are efficiently pooled in the upper mantle (9–20 km depth), after which crystallization commences and continues during ascent and eruption. Based on our melting model and the assumption that CO2 is perfectly incompatible, we show that the highest CO2 concentrations of the melt inclusions (～ 1600 ppm) are consistent with the calculated CO2 concentrations of primary undegassed melts. The highest measured CO2/Nb ratio (443) of Gakkel Ridge melt inclusions predicts a mantle CO2 content of 134 ppm and would result in a global ridge flux of 2.0 × 1012 mol CO2/yr.  相似文献   

17.
The continuous measurement of molecular hydrogen (H2) emissions from passively degassing volcanoes has recently been made possible using a new generation of low-cost electrochemical sensors. We have used such sensors to measure H2, along with SO2, H2O and CO2, in the gas and aerosol plume emitted from the phonolite lava lake at Erebus volcano, Antarctica. The measurements were made at the crater rim between December 2010 and January 2011. Combined with measurements of the long-term SO2 emission rate for Erebus, they indicate a characteristic H2 flux of 0.03?kg s–1 (2.8?Mg? day–1). The observed H2 content in the plume is consistent with previous estimates of redox conditions in the lava lake inferred from mineral compositions and the observed CO2/CO ratio in the gas plume (～0.9 log units below the quartz–fayalite–magnetite buffer). These measurements suggest that H2 does not combust at the surface of the lake, and that H2 is kinetically inert in the gas/aerosol plume, retaining the signature of the high-temperature chemical equilibrium reached in the lava lake. We also observe a cyclical variation in the H2/SO2 ratio with a period of ～10?min. These cycles correspond to oscillatory patterns of surface motion of the lava lake that have been interpreted as signs of a pulsatory magma supply at the top of the magmatic conduit.  相似文献   

18.
A heterogeneous chemical model is developed by coupling aerosol, gas-phase and liquid-phase chemical model. SO2 oxidation rates on the aerosol surface are calculated and the influence of some factors is discussed. Model simulations indicate that SO2 heterogeneous oxidation rates are sensitive to the mass concentration and chemical composition of aerosols, relative humidity, initial values of SO2 and H2O2. The heterogeneous chemical model is coupled with a Eulerian deposition model. Model results show that oxidation of SO2 on the aerosol surface is found to reduce SO2 levels by 5%–33%, to increase SO 4 2- - concentrations by 8%–50% in the surface layer. Project supported by the National “85-912” Key Science and Technology Project.  相似文献   

19.
There is widespread use of passive remote sensing techniques to quantify trace gas column densities in volcanic plumes utilizing scattered sunlight as a light source. Examples include passive DOAS, COSPEC, and the SO2 camera. In order to calculate trace gas concentrations or volcanic emission fluxes, knowledge about the optical path through the plume is necessary. In the past, a straight photon path through the plume has always been assumed although it was known that this is not always true. Here we present the results of model studies conducted specifically to quantify the effects of realistic radiative transfer in and around volcanic plumes on ground-based remote sensing measurements of SO2. The results show that measurements conducted without additional information on average photon paths can be inaccurate under certain conditions, with possible errors spanning more than an order of magnitude. Both over and underestimation of the true column density can occur. Actual errors depend on parameters such as distance between instrument and plume, plume SO2 concentration, plume aerosol load, as well as aerosol conditions in the ambient atmosphere. As an example, a measurement conducted with an SO2 camera is discussed, the results of which can only be correctly interpreted if realistic radiative transfer is considered. Finally, a method is presented which for the first time allows the retrieval of actual average photon paths in spectroscopic (i.e. DOAS) measurements of adequate resolution. By allowing for a wavelength dependent column density during the evaluation of DOAS measurements, we show how radiative transfer effects can be corrected using information inherently available in the measured spectra, thus greatly enhancing the accuracy of DOAS measurements of volcanic emissions.  相似文献   

20.
Solar, sky, and aureole radiance data from Kensington, Australia, and Lagos, Nigeria, are analysed. The values of the aerosol optical thickness at Lagos are comparable to measured values elsewhere in the subregion (Abidjan) under light haze. The values at Kensington are close to those of the “background aerosol.” Identical and anomalous values of aerosol optical thickness occurred at 1.67 μm at both stations as less than 15% of the values can be accounted for by aerosols. The high optical depths are therefore explained in terms of absorption, possibly mainly by CO2 (59–65%) and, to a lesser extent, by H2O (20–26%). Following correction for molecular multiple scattering, the aerosol scattering phase function increases substantially at 0.5 μm in Kensington and decreases considerably at 0.76 μm in Lagos when compared to the uncorrected function, confirming the relative fineness of the Kensington aerosol. The Lagos aerosol size distribution for moderately dusty air is reasonably bimodally log-normal with modal radiusr m=0.49 μm (1.36 μm) for the moder≤1 μm (r>1 μm). The Kensington aerosol resembles one withr m=0.05 μm forr<1 μm. There the Born approximation appears appropriate, and the weighted mean square radiusp 2=0.13 μm2. In the near forward direction the aerosol scattering phase funciton for Lagos resembles Deirmendjian’s simulations for a silicate-L haze and, for Kensington, a silicate-H haze.  相似文献   

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