Regression approach to analyzing the informativity and interpretation of aerosol optical measurements

A regression approach is proposed for planning aerosol optical experiments and for estimating the potential accuracy of the derived microphysical parameters of atmospheric aerosols taking the features of the apparatus and the available a priori information into account. This method is used to evaluate the informativity of polarization spectronephelometer measurements with respect to the microphysical parameters of continental aerosols. The problem of choosing the most informative aerosol optical characteristics with respect to the mass concentrations of the PM _2.5 and PM ₁₀ respirable fractions is examined and regression equations are derived for determining these concentrations from lidar probe data at wavelengths of 0.355 and 1.064 μm, as well as from reference measurements at 0.37 and 0.98 μm. The theoretical results obtained here are compared with AERONET data.     

大气气溶胶偏振遥感研究进展

POLDER-1是国际上第一个可以获取偏振光观测的星载对地探测器, 随着POLDER/PARASOL等偏振仪器的应用, 偏振遥感在国际上已成为一个快速发展的研究领域, 并在大气气溶胶监测等方面发挥了重要的作用, 取得了一系列研究成果。从POLDER/PARASOL,APS(aerosol polarimetry sensor)和航空偏振相机、地基偏振观测平台三个方面综述了大气气溶胶偏振遥感近20年(1993-2013)的研究进展, 重点介绍: (1)POLDER/PARASOL陆地上空和海洋上空气溶胶参数反演算法; POLDER/PARASOL气溶胶光学厚度(AOD)产品精度验证、应用以及与MODIS等卫星AOD产品的对比分析。(2)MICROPOL,RSP和APS陆地上空和海洋上空气溶胶参数反演算法; 国产多角度航空偏振相机(directional polarimetric camera, DPC)的气溶胶参数反演算法。(3)CE318-2和CE318-DP的气溶胶地基偏振反演算法。其中卫星、航空和地面气溶胶参数反演的结果包括总的AOD、细粒子AOD、粗粒子AOD、粒子谱分布、粒子形状、复折射指数、单次散射反射率、散射相函数、偏振相函数以及云顶AOD。在以上研究基础上, 提出了大气气溶胶偏振遥感研究存在的问题及展望, 为大气气溶胶偏振遥感研究提供有价值的参考。     

航空偏振遥感数据反演陆地上空气溶胶光学厚度

在陆地上空气溶胶遥感中,地表多样性会导致地表反射率计算误差增加,降低地气解耦精度,进而影响气溶胶反演精度。多角度、多光谱和偏振观测数据的引入有利于解决地气解耦精度和气溶胶参数的提取精度受限的问题。基于多角度偏振辐射计(AMPR)航空多光谱遥感数据,结合气溶胶散射和地表偏振反射规律,提出了在1 640 nm波段对AMPR观测偏振反射率进行连续大气辐射校正,实现地气解耦的方法。在此基础上,构建了陆地上空气溶胶偏振反演算法。运算过程中使用665和865 nm波段观测数据进行气溶胶参数提取,使用1 640 nm波段观测数据结合提取的气溶胶参数进行大气偏振辐射校正,重新获取地表偏振反射率。在反演过程中引入迭代,逐步逼近大气与地表真实辐射值,实现地气解耦,并利用查找表的方法实现气溶胶光学厚度反演。通过AMPR在京津唐地区5个架次的航空观测实验数据对反演算法进行了验证,结果与地基CE318观测数据一致性较好,在气溶胶光学厚度小于0.5的情况下,反演平均误差为约0.03。     

Chemical composition and mass closure for PM10 aerosols during the 2005 dry season at a rural site in Morogoro,Tanzania

An intensive aerosol field campaign was carried out from 11 July to 11 August 2005 (dry season) at a rural site in Morogoro, Tanzania. The objectives were to determine the chemical composition of the atmospheric particulate matter (PM) and to examine to which extent the gravimetric PM mass can be explained by the measured aerosol components. Two low‐volume filter samplers were deployed, a PM₁₀ filter holder with two Whatman QM‐A quartz fibre filters in series and a Gent PM₁₀ stacked filter unit (SFU) sampler with coarse and fine Nuclepore polycarbonate filters. The samplers operated in parallel and a total of 51 parallel collections were made. All samples were analysed for the PM mass by weighing. Depending on the sampler type and/or collection substrate, further analyses were performed for 25 elements by particle‐induced x‐ray emission spectrometry, for major water‐soluble inorganic ions by ion chromatography, and for organic carbon and elemental carbon by a thermal—optical transmission technique. The PM₁₀ mass, as derived from the SFU samples, was, on an average, 46 ± 12 µg/m³. Aerosol chemical mass closure calculations were made for this PM₁₀ mass; eight aerosol components were considered and they explained 93% of the average PM₁₀ mass. Organic matter (OM) and crustal matter were the dominant aerosol components; they accounted for, on an average, 44% and 33%, respectively, of the PM₁₀ aerosol. The large contribution from OM is thought to originate mainly from the burning of biomass, especially of charcoal and agricultural residues. Copyright © 2009 John Wiley & Sons, Ltd.     

Lead speciation of PM2.5 collected from Greater Cairo,Egypt and Zarqa,Jordan: An energy dispersive X-ray fluorescence and X-ray absorption near edge structure study

Fine aerosol particles with an aerodynamic diameter equal or less than 2.5 μm (PM_2.5) have been collected from two sites (residential and industrial) in Greater Cairo, Egypt and one site in Zarqa, Jordan. Based on the elemental quantitative analysis of PM_2.5 using energy dispersive X-ray fluorescence with Mo secondary target, Pb concentrations increased remarkably during winter season regardless of the sampling location. Moreover, it reached the maximum concentration at the industrial location of Greater Cairo, Egypt, and it equals 415 ± 485 ng/m³. The remarkable high standard deviation is due to the significant variation of Pb concentration from time to time during that winter season. Depending on the energy dispersive X-ray fluorescence results, specific PM_2.5 samples that have the highest concentration of Pb (two samples/location) have been selected for the X-ray absorption near edge structure measurements to estimate the oxidation state of Pb species. The X-ray absorption near edge structure measurements including 13 Pb references have been carried out at Pb-L₃ absorption edge (13.039 keV) using fluorescence mode. It was shown that PM_2.5 contains divalent and tetravalent lead in both industrial site in Greater Cairo, Egypt and urban site of Zarqa, Jordan although that of a residential area of Greater Cairo-Egypt is almost divalent lead.     

Seasonal variation of tropospheric aerosol properties by direct and scattered solar radiation spectroscopy

Long-term characterization of tropospheric aerosol has been carried out at Chiba, Japan, using a compact, stand-alone spectroradiometer under clear-sky conditions between August 2007 and March 2009. The spectra of direct solar radiation, aureole, and scattered solar radiation in various directions are observed in a wavelength range between 350 and 1050 nm with an optical resolution of 10 nm. Radiative transfer calculation using the MODTRAN4 code is employed to retrieve aerosol optical parameters such as aerosol optical depth (AOD), extinction coefficient, single-scattering albedo, scattering phase function, and asymmetry parameter, as well as water vapor column amount. The retrieved value of AOD varies in the range 0.1-0.5, while the water vapor column amount changes from 0.2 to 4 g/cm², showing reasonable agreements with the concurrent measurements with a sunphotometer and a microwave radiometer, respectively. The seasonal variation of the retrieved parameters indicates the major impacts of dust particles in spring, sea salt particles in summer, and anthropogenic fine particles in winter.     

Improvements for ground-based remote sensing of atmospheric aerosol properties by additional polarimetric measurements

We discuss the improvements in the aerosol properties characterization resulting from the additional multi-wavelength polarization measurements measured by a new CIMEL polarized sun/sky-photometer, CE318-DP. In order to process direct-sun, sky and polarization measurements in a wide spectral range (340–1640 nm), we developed new calibration methods and strategies, e.g. using the Langley plot method to calibrate both direct-sun irradiance and sky radiance, as well as combining laboratory facilities with a vicarious method to calibrate the polarized sky measurements. For studying the impact of new polarimetric measurements on the retrievals of aerosol properties, we have processed an extensive record of field measurements using an updated Dubovik and King retrieval algorithm [Dubovik O, Sinyuk A, Lapyonok T, Holben BN, Mishchenko MI, et al. Application of spheroid models to account for aerosol particle nonsphericity in remote sensing of desert dust. J Geophys Res 2006;111:D11208.]. A preliminary analysis shows that adding polarization in the inversion can reduce possible errors (notably for about 30% of our field cases) in the fine mode size distribution, real part of refractive index and particle shape parameter retrievals, especially for small particles.     

Algorithms to retrieve optical properties of three component aerosols from two-wavelength backscatter and one-wavelength polarization lidar measurements considering nonsphericity of dust

We developed backward and forward types of algorithms for estimating the vertical profiles of extinction coefficients at 532 nm for three component aerosols (water-soluble, dust, and sea salt) using three-channel Mie-scattering lidar data of the backscatter (β) at 532 and 1064 nm and the depolarization ratio (δ) at 532 nm. While the water-soluble and sea-salt particles were reasonably assumed to be spherical, the dust particles were treated as randomly oriented spheroids to account for their nonsphericity. The introduction of spheroid models enabled us to more effectively use the three-channel data (i.e., 2β+1δ data) and to reduce the uncertainties caused by the assumption of spherical dust particles in our previously developed algorithms. We also performed an extensive sensitivity study to estimate retrieval errors, which showed that the errors in the extinction coefficient for each aerosol component were smaller than 30% (60%) for the backward (forward) algorithm when the measurement errors were ±5%. We demonstrated the ability of the algorithms to partition aerosol layers consisting of three aerosol components by applying them to shipborne lidar data. Comparisons with sky radiometer measurements revealed that the retrieved optical thickness and angstrom exponent of aerosols using the algorithms developed in this paper agreed well with the sky radiometer measurements (within 6%).     

被动多轴差分吸收光谱大气气溶胶光学厚度监测方法研究

介绍了基于太阳散射光的被动多轴差分吸收光谱（MAX-DOAS）技术在大气气溶胶光学厚度（aerosol optical density,AOD）监测中的应用. MAX-DOAS根据氧的二聚物（O₄）在紫外、可见波段的特征吸收来确定气溶胶参数,实验中利用测量得到的O₄在360 nm处斜柱浓度,并结合O₄垂直柱浓度基本稳定等信息,在选取合适的气溶胶单次散射反照率、非对称因子及其廓线形状等条件下,基于大气辐射传输模型采用迭代算法解析出大气气溶胶光学厚度. 经过与太阳光度计(CE318)测量结果的对比,两者相关性达到87%. 关键词： 多轴差分吸收光谱 大气气溶胶 光学厚度     

Dust aerosol forward scattering effects on ground-based aerosol optical depth retrievals

Monte Carlo radiative transfer calculations are performed to examine the forward scattering effects on retrievals of dust aerosol optical depth (AOD) from ground-based instruments. We consider dust aerosols with different AOD, effective radius and imaginary refractive index at 0.5 μm wavelength. The shape of dust aerosols is assumed to be spheroids and the equivalent spheres that preserve both volume and projected area (V/P) are also considered. The single-scattering albedos and asymmetry factors of spheroids and V/P-equivalent spheres have small differences, but the scattering phase functions are very different for the scattering angle range ∼90-180°. The relative errors of retrieved AOD caused by forward scattering effects due to the differences between the single-scattering properties of spheroids and spheres are similar. It is shown that at solar zenith angle (SZA) smaller than ∼70° the effect of the forward scattering is generally small although the relative errors in retrieved AOD can be as large as −10% when r_e=2. However, the largest relative errors, which can reach −40%, appear at high SZA (>∼70°) with AOD larger than 1. This is not caused by the increase of forward scattering intensity, but is due to the strong attenuation of solar direct beam.     

被动多轴差分吸收光谱大气气溶胶光学厚度监测方法研究

介绍了基于太阳散射光的被动多轴差分吸收光谱（MAX-DOAS）技术在大气气溶胶光学厚度（aerosol optical density,AOD）监测中的应用. MAX-DOAS根据氧的二聚物（O₄）在紫外、可见波段的特征吸收来确定气溶胶参数,实验中利用测量得到的O₄在360 nm处斜柱浓度,并结合O₄垂直柱浓度基本稳定等信息,在选取合适的气溶胶单次散射反照率、非对称因子及其廓线形状等条件下,基于大气辐射传输模型采用迭代算法解析出大气气溶胶光学厚度. 经过与太阳光度计(CE318)测量结果的对比,两者相关性达到87%.     

Aerosol influence on polarization and intensity in near-infrared O2 and CO2 absorption bands observed from space

We study the intensity and degree of linear polarization of reflected solar radiation at the top of the atmosphere within two carbon dioxide bands and one oxygen absorption band in the near-infrared. In particular, we are interested in the sensitivity of the degree of linear polarization and intensity to changes of aerosol and cirrus cloud layer heights, microphysical properties, and surface albedo. For the simulations we use spectral response functions representative of the Orbiting Carbon Observatory (OCO). Inside the O₂A band at 760 nm and strong CO₂ band at 2060 nm we find a strong influence of the aerosol and cirrus cloud layer height on the degree of linear polarization. An increase of the aerosol or cirrus cloud layer height can lead either to a decrease or increase of the polarization within the band, depending on the microphysical and optical properties of the scatterers, surface albedo, and absorption strength in the bands. The results for the O₂A band also indicate that even over land OCO enables an estimation of the height of an aerosol or cirrus cloud layer. Inside the weak CO₂ band at 1610 nm the influence of aerosol or cirrus cloud layer heights is lower as compared to the O₂A band and CO₂ band at 2060 nm, due to the relatively stronger surface influence. Here an increase of aerosol or cirrus cloud layer height leads to an increase of the degree of linear polarization even in case of low surface albedo and for weakly polarizing scatterers. For the weak CO₂ band at 1610 nm we also study the influence of the aerosol or cirrus cloud layer height on the column CO₂ estimate and the errors resulting from ignoring polarization in simulations of backscatter measurements by space-based instruments such as OCO. Depending on the surface albedo, misinterpretations of the height of atmospheric scatterers might strongly affect the column CO₂ estimates.     

Aerosol extinction coefficient profile retrieval in the oxygen A-band considering multiple scattering atmosphere. Test case: SCIAMACHY nadir simulated measurements

A multiple scattering inversion procedure for the aerosol extinction coefficient profile retrieval and error assessment in the oxygen A-band, for passive remote sensing instruments, has been developed. The procedure has been applied to SCIAMACHY nadir simulated measurements to investigate its effectiveness in the troposphere.The inversion procedure consists of a multiple scattering Forward Model, an inversion method and a complete sensitivity and error assessment tool. The Forward Model is based on LIDORT code; the inversion method, the sensitivity study and the complete error assessment are based on Optimal Estimation. The sensitivity and error analysis has been derived to investigate the profile retrieval errors due to the uncertainty of different aerosol optical properties, molecular and surface parameters.The analysis confirms that the profile retrieval accuracy and vertical resolution are strongly dependent on the oxygen A-band spectral resolution. The moderately high SCIAMACHY spectral resolution (0.4 nm in the oxygen A-band) results in distinguishing a maximum of three aerosol layers in troposphere. The SCIAMACHY tropospheric aerosol profile retrieval is shown to be highly sensitive to aerosol optical properties as phase function and single scattering albedo. The sensitivity study reveals an improvement of information content increasing the solar zenith angle and decreasing the surface albedo. As regards the forward model, negligible errors occur as the number of streams exceeds 6.     

A method for retrieval of the profiles of atmospheric backscattering coefficients by three-wavelength lidar and nephelometric measurements

A method for retrieval of the profiles of atmospheric aerosol backscattering coefficients β _a along horizontal and inclined paths from the results of three-wavelength probing by laser location systems based on a Nd: YAG laser is proposed. The method uses a power dependence between the spectral values of β _a and includes spectral nephelometric measurements of the scattering coefficients by an angle of 33°, which characterize the relative spectral dependence of aerosol extinction. The sensitivity of this method to spatial variations in the above coefficients, to the deviation of β _a from the dependence used, and to errors in calibration and measurement of signals is studied. The method is demonstrated to be stable both upon using the absolute calibration of the lidar and at an arbitrary position of the reference point.     

Retrieval of aerosol physical and chemical properties from mid-infrared extinction spectra

We report several results that validate the accuracy of a retrieval method for the determination of a number of aerosol particle properties from their mid infrared (600-6000 cm⁻¹) extinction spectra. These properties include the number density, chemical composition, phase, size distribution, and to some extent, shape. The approach is based on information obtained in laboratory studies of micron-sized particles using the aerosol flow tube (AFT) technique. We report here experiments in which our method is used to measure a variety of aerosols including SiO₂ micro-spheres as well as solid NaCl, (NH₄)₂SO₄, ice and liquid water particles. The uncertainties in the retrieved aerosol properties associated with the particle shapes (spheres, spheroids, cylinders, hexagonal and rectangular prisms) as well as the effect of variations in the spectral range were evaluated. To assess the accuracy of the retrieved size distributions and particle shapes, the properties calculated from infrared spectra were compared with corresponding properties determined using alternative methods. We used scanning electron microscopy (SEM) for solid (NH₄)₂SO₄ and NaCl aerosols and direct particle imaging with an optical microscope assembly for liquid water aerosols. On the basis of the validation results, we discuss the boundaries of applicability of the most popular spectral model, single scattering by spherical, homogeneous aerosol particles.     

Evaluation of errors from neglecting polarization in the forward modeling of O2A band measurements from space, with relevance to CO2 column retrieval from polarization-sensitive instruments

Sensitivity studies have been performed to evaluate the errors resulting from ignoring polarization in analyzing spectroscopic measurements of the O₂A band from space, using the Orbiting Carbon Observatory (OCO) as a test case. An 11-layer atmosphere, with both gas and aerosol loading, and bounded from below by a lambertian reflecting surface, was used for the study. The numerical computations were performed with a plane-parallel vectorized discrete ordinate radiative transfer code. Beam and viewing geometry, surface reflectance and aerosol loading were varied one at a time to evaluate and understand the individual errors. Different behavior was observed in the line cores and the continuum because of the different paths taken by the photons in the two cases. The errors were largest when the solar zenith angle was high, and the aerosol loading and surface reflectance low. To understand the effect of neglecting polarization on CO₂ column retrievals, a linear error analysis study was performed on simulated measurements from the OCO spectral regions, viz. the 1.61 and 2.06 μm CO₂ bands and the O₂A band. It was seen that neglecting polarization could introduce errors as high as 10 ppm, which is substantially larger than the required retrieval precision of ∼2 ppm. A variety of approaches, including orders of scattering, spectral binning and the use of lookup tables are being explored to reduce the errors.     

利用差分吸收光谱法测量亚硝酸和反演气溶胶参数

利用差分光学吸收光谱仪(DOAS)进行亚硝酸(HONO)气体的测量并同时在固定的波长范围内(3 07—380 nm)反演气溶胶参数包括气溶胶的平均直径、总个数和总比表面积等. 实验结果表 明利用自测的NO₂标准吸收截面可以更加准确地拟合HONO的浓度，同时在较短的 波长范围内能准确反演气溶胶参数. 关键词： 差分光学吸收光谱(DOAS) 亚硝酸 气溶胶参数     

Effect of instrumental particle sizing resolution on the modelling of aerosol radiative parameters

A more realistic estimation of the scattering and hemispheric backscattering coefficients, σ_sp and σ_bsp, and their respective optical cross section, C_sca and C_bk, of aerosol particles is presented on the basis of the exact resolution of the width of the size bins of the particle counter instruments when size distribution measurements are used, and, with the exact optical detector instruments ability. The scattering and hemispheric backscattering cross sections, C_sca and C_bk, of the particles are averaged over the full size bins of the particle counter instrument, while these quantities are usually estimated only on the value of the mean geometric diameter of each size bin. Six instruments, the APS, ASASP-X, DMPS, FSSP-100, ELPI, and SMPS frequently used in particle size distribution measurements are reviewed, for spherical sea-salt particles at a wavelength λ=0.55 μm. The comparison using the conventional geometric mean diameter versus the use of the full size bin leads to large amount of errors for the optical cross section with non-negligible effects on their respective optical coefficients. The maximal accuracy expected for these optical quantities depend on the particle diameter as well as on the channel width of the instruments, and are also function of the angular detector probe used to measure them.     

Influence of local waste burning on atmospheric aerosol properties in urban environment

Aerosols affect the radiative energy budget on both the regional and global scales. The wavelength-dependent aerosol optical depth (AOD) is a fundamental determinant of the amount by which extra-terrestrial incoming sunlight and outgoing terrestrial radiation are being attenuated in the atmosphere. The present study addresses the influence of local waste burning on aerosol characteristics, black carbon (BC) aerosol mass concentration and spectral solar irradiance using ground-based measurements over the tropical urban environment of Hyderabad, India. AOD has been observed to be maximum during burning days compared to normal days. Aerosol size spectra suggest bimodal distributions during pre-and post-burning periods and trimodal distributions during burning periods. Angstrom wavelength exponent estimated from spectral variation of AOD suggested dominance of accumulation mode particle loading during burning days compared to normal days. Diurnal variation of BC on normal days showed a broad nocturnal peak during ∼20:00 to ∼24:00 h with a maximum value of BC aerosol concentration of ∼14,000 ng m⁻³ whereas on local waste burning days enormous increases in BC concentrations have been observed with a peak at ∼60,000 ng m⁻³. Relative attenuation of global solar irradiance during burning days has been found to be of the order of 30% in the visible and 28% in the near-infrared regions. The results are discussed in detail in this paper.     

Assembly of γ-Fe2O3/polyaniline nanofilms with tuned dipolar interaction

The internal morphology and magnetic properties of layer-by-layer assembled nanofilms of polyaniline (PANI) and maghemite (γ-Fe₂O₃—7.5-nm diameter) were probed with cross-sectional transmission electron microscopy (TEM) and magnetization measurements (magnetic hysteresis loops, magnetization using zero-field cooled/field-cooled protocols, and ac magnetic susceptibility). Additionally, simulations of the as-produced samples were performed to assess both the nanofilm’s morphology and the corresponding magnetic signatures using the cell dynamic system (CDS) approach and Monte Carlo (MC) through the standard Metropolis algorithm, respectively. Fine control of the film thickness and average maghemite particle–particle within this magnetic structure was accomplished by varying the number of bilayers (PANI/γ-Fe₂O₃) deposited onto silicon substrates or through changing the concentration of the maghemite particles suspended within the colloidal dispersion sample used for film fabrication. PANI/γ-Fe₂O₃ nanofilms comprising 5, 10, 25 and 50 deposited bilayers displayed, respectively, blocking temperatures (T _B) of 30, 35, 39 and 40 K and effective energy barriers (ΔE/k _B) of 1.0 × 10³, 2.3 × 10³, 2.8 × 10³ and 2.9 × 10³ K. Simulation of magnetic nanofilms using the CDS model provided the internal morphology to carry on MC simulation of the magnetic properties of the system taking into account the particle–particle dipolar interaction. The simulated (using CDS) surface–surface particle distance of 0.5, 2.5 and 4.5 nm was obtained for nanofilms with thicknesses of 36.0, 33.9 and 27.1 nm, respectively. The simulated (using MC) T _B values were 33.0, 30.2 and 29.5 K for nanofilms with thicknesses of 36.0, 33.9 and 27.1 nm, respectively. We found the experimental (TEM and magnetic measurements) and the simulated data (CDS and MC) in very good agreement, falling within the same range and displaying the same systematic trend. Our findings open up new perspectives for fabrication of magnetic nanofilms with pre-established (simulated) morphology and magnetic properties.