随机分布黑碳-硅酸盐混合凝聚粒子的消光特性研究

基于分形理论,采用蒙特卡罗方法对随机分布的混合凝聚粒子的空间结构进行了仿真模拟。利用Bruggeman有效介质理论得到了占有不同体积份额黑碳的内混合凝聚粒子的等效复折射率。采用离散偶极子近似方法对随机分布混合凝聚粒子在内外混合状态下的吸收、散射和消光效率因子等消光特性参量进行了数值计算,深入探讨了混合方式、容积含量、入射波长以及基本粒子粒径和数量对混合凝聚粒子消光特性的影响规律。通过将所得数值结果与T矩阵方法的数值结果进行比较发现,两种数值方法计算的结果非常相近。结果表明,随机分布混合凝聚粒子的散射效率因子对混合方式非常敏感,消光效率因子对混合方式较敏感,而吸收效率因子对混合方式不敏感。随着凝聚粒子尺度参数的增大,混合方式对散射和消光效率因子的影响逐渐显著。内外混合方式下,随着黑碳体积比的增大随机分布混合凝聚粒子的吸收、散射和消光效率因子均近似线性增大,并且增大的幅度随着粒子尺度参数的增大而增大。     

两种按比例混合颗粒系的多次散射模拟

一种颗粒与其他种类的颗粒混合后, 会使其散射特性发生变化, 本文研究了水云中混有黑炭气溶胶后的散射特性变化. 根据Mie理论计算了水云和黑炭气溶胶散射相函数、单次散射反照率和不对称因子. 给出了混合颗粒系的蒙特卡罗模拟方法, 给出了颗粒碰撞类型抽样、自由程抽样和根据Mie相函数进行散射方向抽样的方法. 计算了光垂直入射时, 水云和黑炭气溶胶混合颗粒系的反射光强随观测角的变化, 并计算了平面反照率随入射角的变化, 讨论了黑炭气溶胶的有效半径、混合比例对整个混合颗粒系散射特性的影响. 计算结果表明, 水云中混合黑炭会加强其吸收, 且黑炭的比例和尺寸不同其散射特性差异较大.     

内混合强吸收气溶胶粒子光散射的等效性

 以黑碳和水两种成分组成的内混合单分散气溶胶粒子为例,根据其各消光效率因子、吸收效率因子和散射相函数,分析了用等效折射率来描述含有不同成分的内混合气溶胶系统的适用性。结果表明：在瑞利散射区和几何光学区内,内核（碳粒）体积比为0.01,0.1,0.5,0.9时,消光效率在大多数尺度参数下等效性都很好,但在米散射区内相对较差;当体积比大于0.3时,其吸收效率、消光效率等效性较好;除瑞利散射区外,散射相函数在各体积比下的等效性都很差。当考虑内混合气溶胶粒子系统的散射和吸收特性时,一般不难找到等效折射率,但在光散射技术中,应用相函数反演等效折射率的可靠性还有待商榷。     

A method for estimating optical properties of dusty cloud

Based on the scattering properties of nonspherical dust aerosol, a new method is developed for retrieving dust aerosol optical depths of dusty clouds. The dusty clouds are defined as the hybrid system of dust plume and cloud. The new method is based on transmittance measurements from surface-based instruments multi-filter rotating shadowband radiometer （MFRSR） and cloud parameters from lidar measurements. It uses the difference of absorption between dust aerosols and water droplets for distinguishing and estimating the optical properties of dusts and clouds, respectively. This new retrieval method is not sensitive to the retrieval error of cloud properties and the maximum absolute deviations of dust aerosol and total optical depths for thin dusty cloud retrieval algorithm are only 0.056 and 0.1, respectively, for given possible uncertainties. The retrieval error for thick dusty cloud mainly depends on lidar-based total dusty cloud properties.     

Light absorption and scattering by aggregates: Application to black carbon and snow grains

A geometric-optics surface-wave approach has been developed for the computation of light absorption and scattering by nonspherical particles for application to aggregates and snow grains with external and internal mixing structures. Aggregates with closed- (internal mixing) and open-cell configurations are constructed by means of stochastic procedures using homogeneous and core-shell spheres with smooth or rough surfaces as building blocks. The complex aggregate shape and composition can be accounted for by using the hit-and-miss Monte Carlo geometric photon tracing method. We develop an integral expression for diffraction by randomly oriented aggregates based on Babinet's principle and a photon-number weighted geometric cross section. With reference to surface-wave contributions originally developed for spheres, we introduce a nonspherical correction factor using a non-dimensional volume parameter such that it is 1 for spheres and 0 for elongated particles. The extinction efficiency, single-scattering albedo, and asymmetry factor results for randomly oriented columns and plates compare reasonably well with those determined from the finite-difference time domain (FDTD) and the discrete dipole approximation (DDA) computer codes for size parameters up to about 20. The present theoretical approach covers all size ranges and is particularly attractive from the perspective of efficient light absorption and scattering calculations for complex particle shape and inhomogeneous composition.We show that under the condition of equal volume and mass, the closed-cell configuration has larger absorption than its open-cell counterpart for both ballistic and diffusion-limited aggregates. Because of stronger absorption in the closed-cell case, most of the scattered energy is confined to forward directions, leading to a larger asymmetry factor than the open-cell case. Additionally, light absorption for randomly oriented snowflakes is similar to that of their spherical counterparts under the condition of equal geometrical cross section area for both external and internal mixing states; however, nonspherical snowflakes scatter less light in forward directions than spheres, resulting in a substantial reduction of the asymmetry factor. We further demonstrate that small soot particles on the order of 1 μm internally mixed with snow grains could effectively reduce snow albedo by as much as 5-10%. Indeed, the depositions of black carbon would substantially reduce mountain-snow albedo, which would lead to surface warming and snowmelt, critical to regional climatic surface temperature amplification and feedback.     

相态对冰水混合云微观特性反演的影响研究

当云层的温度在－40℃~0℃之间时, 云层中会存在冰和水两种相态的云滴, 其散射特性与纯水云以及纯冰云特性有较大差异, 因此遥感反演混合相云层的微观和宏观物理特性具有重要的意义。本文采用冰水双层球模型模拟了冰水混合云中的云滴, 利用Mie理论计算了纯水、纯冰和冰水颗粒的单次散射特性, 分析了单次散射相函数, 不对称因子, 单次散射反照率等随着有效半径、相态、内外半径比等的变化特性。利用离散纵标法(DISORT)计算了水云和冰云对0.75 μm、2.16 μm和3.3 μm的双向反射函数, 讨论了利用纯水滴和纯冰滴反演冰水混合云滴的误差。分析结果表明, 利用0.75 μm和2.16 μm的太阳光反演冰水混合云的光学厚度和有效半径时, 光学厚度误差较大, 有效半径误差较小; 结合0.75 μm和3.3 μm的太阳光反演冰水混合云的光学厚度和有效半径时, 光学厚度误差较小, 有效半径误差较大, 其会高估其有效半径; 另外结合0.75 μm和3.3 μm这两个波长的反射函数反演冰水云的冰水混合比更为有效。     

水云增长过程中的云滴谱及散射特性分析

基于大气物理学研究了水云云滴增长过程中的粒谱及散射特性.研究结果表明,凝结增长使粒谱半高宽和有效半径不断增加,碰并增长使粒谱出现多峰分布,有效半径增加.在凝结增长和碰并增长共同作用下,有效半径的平均增长速率为8 nm/s.凝结增长和碰并增长单独作用下,消光系数和散射系数随时间呈线性变化.在二者共同作用下,除3.2 mm波长外,消光系数和散射系数随时间呈指数增长;1.064, 2.2, 3.7, 12和22μm波长的不对称因子逐渐趋于稳定,200μm的不对称因子呈指数增长,3.2 mm的不对称因子基本保持不变;1.064和2.2μm波长的雷达比在20 sr附近波动,3.7μm波长的雷达比呈大幅振荡.云滴增长过程中,水云在1.064, 2.2和3.7μm波长的单次散射反照率逐渐降低,在12μm, 22μm, 200μm和3.2 mm波长的单次散射反照率逐渐增加,波长指数的绝对值逐渐减小.研究结果可为天气预报、地气辐射平衡研究和遥感数据校正提供重要的参考.     

Aerosol light absorption and its measurement: A review

Light absorption by aerosols contributes to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer. Besides the direct radiative effect, the heating can evaporate clouds and change the atmospheric dynamics. Aerosol light absorption in the atmosphere is dominated by black carbon (BC) with additional, significant contributions from the still poorly understood brown carbon and from mineral dust. Sources of these absorbing aerosols include biomass burning and other combustion processes and dust entrainment.For particles much smaller than the wavelength of incident light, absorption is proportional to the particle volume and mass. Absorption can be calculated with Mie theory for spherical particles and with more complicated numerical methods for other particle shapes.The quantitative measurement of aerosol light absorption is still a challenge. Simple, commonly used filter measurements are prone to measurement artifacts due to particle concentration and modification of particle and filter morphology upon particle deposition, optical interaction of deposited particles and filter medium, and poor angular integration of light scattered by deposited particles. In situ methods measure particle absorption with the particles in their natural suspended state and therefore are not prone to effects related to particle deposition and concentration on filters. Photoacoustic and refractive index-based measurements rely on the heating of particles during light absorption, which, for power-modulated light sources, causes an acoustic signal and modulation of the refractive index in the air surrounding the particles that can be quantified with a microphone and an interferometer, respectively. These methods may suffer from some interference due to light-induced particle evaporation. Laser-induced incandescence also monitors particle heating upon absorption, but heats absorbing particles to much higher temperatures to quantify BC mass from the thermal radiation emitted by the heated particles. Extinction-minus-scattering techniques have limited sensitivity for measuring aerosol light absorption unless the very long absorption paths of cavity ring-down techniques are used. Systematic errors can be dominated by truncation errors in the scattering measurement for large particles or by subtraction errors for high single scattering albedo particles. Remote sensing techniques are essential for global monitoring of aerosol light absorption. While local column-integrated measurements of aerosol light absorption with sun and sky radiometers are routinely done, global satellite measurements are so far largely limited to determining a semi-quantitative UV absorption index.     

一种内混合气溶胶粒子模型光散射的等效性

以包含灰尘、黑碳和水三种成分的单分散内混合初次气溶胶为例,利用消光、吸收、散射效率因子和不对称因子,探讨了以等效折射率描述具有不同成分的内混合气溶胶粒子系统的适用性。结果表明,在尺度参数为0.1～25时不同半径比下,消光、吸收和散射效率因子的等效性较好,相对误差分别在3%、3%和4%以内;不对称因子的等效性相对稍差,相对误差在13%以内。当半径比a/b小于1/5,即内混合体中所含灰尘和黑碳较少时,等效折射率实部和虚部值基本可以确定,而不必考虑尺度参数的影响。用除散射相函数之外的其他光学量来等效时,较为容易找到等效的气溶胶粒子。     

Aerosol scattering of supercontinuum radiation formed upon femtosecond laser pulse filamentation in the atmosphere

We report numerical calculations of scattering and backscattering efficiency factors of water droplets illuminated by a quasi-white light radiation (a supercontinuum radiation) that results from self-focusing of a high-power femtosecond laser pulse in the atmosphere. The behavior of these integral optical characteristics for a wide range of droplet sizes that covers the size spectra of fog and cloud particles is analyzed. The results are compared to the values of the scattering factors obtained by the Lorentz-Mie theory.     

On geometric optics and surface waves for light scattering by spheres

A geometric optics approach including surface wave contributions has been developed for homogeneous and concentrically coated spheres. In this approach, a ray-by-ray tracing program was used for efficient computation of the extinction and absorption cross sections. The present geometric-optics surface-wave (GOS) theory for light scattering by spheres considers the surface wave contribution along the edge of a particle as a perturbation term to the geometric-optics core that includes Fresnel reflection–refraction and Fraunhofer diffraction. Accuracies of the GOS approach for spheres have been assessed through comparison with the results determined from the exact Lorenz–Mie (LM) theory in terms of the extinction efficiency, single-scattering albedo, and asymmetry factor in the size–wavelength ratio domain. In this quest, we have selected a range of real and imaginary refractive indices representative of water/ice and aerosol species and demonstrated close agreement between the results computed by GOS and LM. This provides the foundation to conduct physically reliable light absorption and scattering computations based on the GOS approach for aerosol aggregates associated with internal and external mixing states employing spheres as building blocks.     

随机取向双层椭球粒子偏振散射特性研究

基于T矩阵方法,给出了随机取向、轴对称、含核椭球粒子的散射计算方法.散射体的核和外壳均可为非球形粒子,整个粒子具有轴对称性.以含核椭球粒子为模型,计算了含有吸收性内核(黑炭,black carbon)的水凝物气溶胶的散射特性,分析了核的大小、形状对消光系数、散射系数、吸收系数、不对称因子、单次散射反照率以及Muller矩阵等的影响. 关键词： 光散射 T矩阵 Muller矩阵 椭球粒子     

Aqueous Droplet Sizing by Inertial Classification

The particle size distribution of an aerosol generated from an aqueous system is difficult to analyse because of the shrinkage of the droplets due to solvent evaporation. These problems are very important for the characterization of medical nebulizers, since most of the drugs delivered via inhalation are water soluble. In situ methods for droplet size analysis, such as laser diffraction, phase Doppler anemometry and light scattering, do not determine either the initial or the equilibrium size distribution. With the residual technique, which means evaporating the droplets and measuring the size and concentration of the residuals, the instability of the aqueous droplets plays no role and the necessary radioactive labelling of the sprayed material allows a direct determination of the mass flow rate at the mouthpiece of the nebulizer. In this way it is possible to discriminate between the delivered drug solution and the water necessary to humidify the incoming air. The output of nebulizers of different designs is given for various operating conditions, filling volumes and solution concentrations. The measured droplet size distribution of a nebulizer is found to be fixed mainly by its internal impaction system.     

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.     

Radiative transfer calculations through an aerosol cloud

A radiative transfer calculation of the EM radiation through an aerosol cloud is presented. The effects taken into account are elastic and inelastic scattering of the incident radiation and self-emission by the aerosol cloud. The elastic scattering effects include multiple scattering of the incident photons. We describe the model and calculational procedure based on the multiple scattering approach. The results of the present model are compared with other models for the two given aerosol clouds.     

外混合气溶胶粒子光散射的等效性

以两种典型的气溶胶粒子组成的单分散和多分散处理混合气溶胶粒子系统的光散射的各效率因子，各散射截面和散射相函数分析了以等效折射率描述由具有不同折射率的各种粒子组成的混合气溶胶粒子系统的适用性，结果表明，对单分散系统，本不同的混合比下对于许多尺度参数吸收效率因子和散射相函数的等效性很差，对多分散系统，在不同的混合比下等效性较稳定但各散射光学量的余差很大，因而对多分散系外混合气溶胶粒子系统如使用等效折射     

积雪与气溶胶粒子混合的光谱反照率模拟研究

积雪中的黑碳气溶胶粒子会导致积雪光谱反射率显著下降,进而引起的气候辐射变化会推迟或提前积雪融化时间,严重影响了干旱区地表径流特征、区域水循环过程,由此引起的干旱区生态水文问题也越来越受到关注。2018年1月在新疆北疆地区开展积雪中气溶胶粒子观测实验,借助ASD地物光谱仪、Snow Folk积雪特性仪与HR-1024外场分光辐射度计等仪器获取原始积雪光谱数据与其他积雪参数,应用Snow,Ice,and Aerosol Radiation model(SNICAR)模型模拟了不同雪粒径下、不同太阳天顶角、不同Black Carbon(BC)浓度下的积雪光谱反照率变化状况,讨论了BC、雪粒径在不同光谱范围内敏感性,结果表明:太阳天顶角对雪面光谱反照率的影响在近红外波段比其他波段表现得更明显,在积雪光谱曲线中太阳天顶角从0°变化到80°,可见光波段600 nm处光谱反照率升高了0.045,近红外波段1000,1200和1300 nm处光谱反照率分别升高了0.16,0.225和0.249;在天顶角为60°时,雪粒径从100μm增大到800μm,对应的光谱反照率减少量最大可达到0.15,且100~300μm范围内的雪粒径比400~800μm范围内的引起光谱反照率的下降量明显增大,雪粒径的增大能使吸光性颗粒物的光吸收效应增强;随着BC浓度的增加,积雪反照率会显著下降,且不同浓度的BC对积雪的反照率的差值不同,随着BC浓度的增加,反照率的差值量越来越小。不同的BC浓度在近红外波段对光谱反照率影响较小,影响较大的范围主要集中可见光波段,在光谱800和1100 nm处,5μg·g-1的BC浓度使光谱反照率减小了0.13和0.04,5μg·g-1的BC可使350与550 nm处的光谱反照率减小0.25与0.23;比较不同粒径下,BC浓度对积雪光谱宽波段反照率的减少情况可发现,在BC存在的情况下,雪粒径的增加会增大BC的光吸收效应,且浓度越高,吸收增加的越多;从光谱指数角度表明BC在可见光波段350~740 nm比较敏感,相关系数较高;雪粒径在近红外波段1100~1500 nm比较敏感,尤其在1000与1300 nm左右,BC与雪粒径在积雪光谱曲线中的敏感波段相关性都较高,R 2高达0.9以上;最后将模型模拟的积雪反照率与实测数据进行验证对比,R 2为0.738,模拟效果较好,可为干旱区积雪光谱反照率的研究奠定数据基础。     

Influence of complex component and particle polydispersity on radiative properties of soot aggregate in atmosphere

The effects of morphological structure, water coating, dust mixing and primary particle size distribution on the radiative properties of soot fractal aggregates in atmosphere are investigated using T-matrix method. These fractal aggregates are numerically generated using a combination of the particle-cluster and cluster-cluster aggregation algorithms with fractal parameters representing soot aggregate in atmosphere. The radiative properties of compact aggregate notably deviate from that of the branched one, and the effect of morphology changes on the radiative properties in wet air cannot be neglected. However it is reasonable to use realization-averaged radiative properties to represent that of the aggregates with certain morphology. In wet air, the scattering, absorption and extinction cross-section and symmetry parameter of soot aggregates coated with water notably increase with water shell thickness. The mixing structures of dust have little effect on radiative properties of aggregates, but the volume fraction of dust has an obvious effect on extinction, scattering and absorption cross-section of aggregates when the size parameters are above the Rayleigh limit. Although the primary particle size distribution of soot aggregate has mild effect on the scattering albedo and asymmetry parameter, the deviations of the extinction, scattering, absorption cross-section among the three size distributions are significant in this study. The size distribution has a significant effect on forward scattering of phase function, while the effect can be neglected as the size parameter approaches to the Rayleigh limit.     

随机取向气溶胶凝聚粒子光学特性研究

利用Cluster-cluster aggregation (CCA)模型,模拟了由64个球形原始微粒凝聚而成的四种随机取向气溶胶凝聚粒子。结合离散偶极子近似方法,分别得到了不同入射角和不同尺寸参数情况下气溶胶凝聚粒子的吸收、散射、消光效率因子和不对称因子的数值结果,并比较分析了四种形状气溶胶凝聚粒子吸收、散射、消光效率因子和不对称因子的差异。结果显示：对于相同数目原始微粒的气溶胶凝聚粒子,其光学特性明显依赖于入射光的入射角度和气溶胶凝聚粒子的形状;对于不同尺寸参数的气溶胶凝聚粒子,当入射光波长给定时,吸收、散射和消光效率因子最初随尺寸参数增大而快速增大,随后又随尺寸参数增大缓慢变小,但在尺寸参数变化过程中存在一个极大值;不对称因子则随尺寸参数的增大一直呈增大趋势,且随尺寸参数的增大趋近于1。