取向数对非球形沙尘气溶胶光学特性的影响

利用离散偶极子近似法研究了旋转椭球体沙尘气溶胶粒子在尺度参数变化范围为0.1~23时(波长0.55!m对应有效半径为0.01~2!m)的光学特性,并通过分析比较不同取向数下光学特性的差别,研究取向数对非球形沙尘粒子光学特性的影响。对单分散系,较少的取向数使旋转椭球体沙尘气溶胶粒子的各光学参量对于取向的选取敏感,但随着取向数的增多,沙尘粒子的各光学量逐步趋于一致。对多分散系,受粒子谱分布积分效果的影响,旋转椭球体沙尘气溶胶粒子对取向的敏感度,相比单分散系要稍低一些。粒子的非球形程度对获得随机取向光学特性取向数的选取也有影响,粒子非球形特征越明显,获得随机取向光学特性所需要的取向数越多。以多分散的旋转椭球体沙尘粒子为例,要获得随机取向沙尘粒子的消光效率因子、单次散射反照率和不对称因子(相对偏差在1%以内),轴半径比为16的非球形程度所需的取向数超过500,而轴半径比为2的非球形程度所需的取向数则仅超过100。     

掺杂对随机取向团簇粒子辐射特性的影响

利用Bruggeman有效介质理论得到了占有不同体积份额杂质的团簇粒子的等效复折射率.采用离散偶极子近似方法对包含有不同化学成分的随机取向团簇粒子的散射相函数、消光、吸收、散射效率因子、单次散射反照率以及不对称因子等辐射特性参量进行了数值计算,深入探讨了掺杂量对随机取向团簇粒子辐射特性的影响.研究表明,掺杂对随机取向团...     

取向比对椭球气溶胶粒子散射特性的影响

利用T矩阵和离散坐标法研究了取向比对椭球粒子散射特性的影响, 计算了小尺度范围内椭球粒子的散射特征参量, 包括消光效率因子、不对称因子、单次散射反照率、散射相矩阵及双向反射函数(BRDF). 结果表明, 椭球粒子的散射特性与取向比密切相关, 粒子取向比会影响散射参量的振荡频率和振幅, 与球形粒子散射参量的相对差异也呈周期振荡趋势. 研究还发现, 某些特殊粒子尺寸的散射参量与粒子取向比基本无关. 在多次散射条件下, 分析不同取向比粒子群的BRDF随反射角和光学厚度的变化特性. 结果显示: 不同取向比粒子群的BRDF随反射角的变化趋势基本一致, 球形粒子群比非球形粒子群的BRDF曲线波动振幅更大; 球形-非球形粒子的BRDF相对差异随光学厚度和取向比的增大而减小, 随入射角的增大而增大.     

掺杂对随机取向团簇粒子辐射特性的影响

利用Bruggeman有效介质理论得到了占有不同体积份额杂质的团簇粒子的等效复折射率.采用离散偶极子近似方法对包含有不同化学成分的随机取向团簇粒子的散射相函数、消光、吸收、散射效率因子、单次散射反照率以及不对称因子等辐射特性参量进行了数值计算,深入探讨了掺杂量对随机取向团簇粒子辐射特性的影响.研究表明,掺杂对随机取向团簇粒子的辐射特性产生显著的影响,并且此影响随着粒子尺度参量的变化而变化.这一工作对研究多种化学成分组成的混合气溶胶的辐射及气候效应具有重要科学价值.     

取向比对圆柱状冰晶粒子光散射特性的影响

利用T矩阵方法研究卷云中圆柱状粒子取向比对散射特性的影响,计算了在小尺度范围内圆柱状冰晶粒子的散射特征量如散射相函数、消光效率因子、不对称因子及单次散射反照率,并将计算结果与等表面积、等体积及等效体积与投影面积比三种情况下的球形粒子的相应值进行了对比.结果表明:体积与投影面积比等效最接近真实值;取向比对不同尺度柱状粒子散射特性的影响存在相似性且有必要加以考虑;此外,发现等表面积、不同取向比粒子的散射相函数有一交点.     

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     

随机取向椭球粒子的吸收特性

用Ｔ矩阵方法计算了折射率虚部的范围在０．００１至０．１的几种椭球粒子随机取向时在几种等效尺度参数下的光散射与吸收特性，并与等效的球形粒子的光散射结果进行了比较。分析结果表明：椭球粒子的吸收特性与等效的球形粒子的吸收特性存在着差别，这种差别随粒子的形状、尺度和折射率而改变，考虑到目前气溶胶粒子复折射率虚部的测量精度，以等效的球体粒子处理非球形粒子的吸收不会带来显著的误差。     

随机取向六角形冰晶粒子的散射特性研究

利用离散偶极子近似方法研究卷云中随机取向六角形冰晶粒子的取向比对散射特性的影响,数值计算了在小尺度范围内随机取向六角形冰晶粒子的散射特征量,包括散射相函数、消光效率因子、不对称因子、单次散射反照率和线偏振度。研究表明:取向比对随机取向六角形冰晶粒子散射特征量的影响比较明显,并且此影响随着粒子尺度参数的变化而变化,与入射波长无关;相同尺度参量和不同取向比粒子的散射相函数的角分布曲线均有一个交点,并且随着粒子尺度参量的增加,交点所对应的散射角度值逐渐向小角度方向移动。此研究结果为气溶胶粒形检测和识别提供了理论依据。     

沙尘暴粒子的非球形模型及其对激光的多次散射特性研究

计算沙尘暴对电磁波的衰减特性,以及利用卫星反射率遥感反演沙尘暴的光学厚度时,通常假设沙尘粒子为球形,但实验室和现场测量结果都表明,自然界中的沙尘粒子为非球形,因此利用球形粒子模型模拟沙尘暴对激光的散射和衰减特性将带来较大误差。利用具有一定尺寸分布、形状分布、随机取向的椭球粒子模型模拟自然界中的沙尘粒子,利用T矩阵方法计算了其单次散射特性,并与球形粒子模型进行了比较,结果表明,混合椭球粒子的相函数随角度分布是平滑的、无特征的、且在侧散射方向上是平坦的,这和自然界中的沙尘粒子散射特性非常类似。最后利用累加法计算了沙尘暴对激光的多次散射特性,结果表明,利用任何一种单一形状的粒子模拟沙尘粒子的散射特性都会带来较大的误差。     

随机取向气溶胶凝聚粒子光学特性研究北大核心CSCD

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.     

Modeling the radiative properties of nonspherical soil-derived mineral aerosols

Mineral dust aerosols have complex nonspherical shapes and varying composition. This study utilizes data on morphology (size and shape) and composition of dust particles to determine the extent to which the optical properties of real particles differ from those of spheres. A method for modeling the optical properties of complex particle mixtures is proposed. The method combines dust particle composition-shape-size (CSS) distributions reconstructed from the electron microscopy data, effective medium approximations and discrete dipole approximation. The method is used to compute optical characteristics of realistic dust mixtures representative of Saharan and Asian dust. We demonstrate that considered CSS distributions result in various differences in the extinction coefficient, single scattering albedo, asymmetry parameter and the scattering phase function relative to the volume-equivalent spheres and the mixtures of the randomly oriented oblate and prolate spheroids. Implications of these differences for radiation/climate modeling and remote sensing are discussed.     

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.     

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。     

On the impact of non-sphericity and small-scale surface roughness on the optical properties of hematite aerosols

We perform a comparative modelling study to investigate how different morphological features influence the optical properties of hematite aerosols. We consider high-order Chebyshev particles as a proxy for aerosol with a small-scale surface roughness, and spheroids as a model for nonspherical aerosols with a smooth boundary surface. The modelling results are compared to those obtained for homogeneous spherical particles. It is found that for hematite particles with an absorption efficiency of order unity the difference in optical properties between spheres and spheroids disappears. For optically softer particles, such as ice particles at far-infrared wavelengths, this effect can be observed for absorption efficiencies lower than unity. The convergence of the optical properties of spheres and spheroids is caused by absorption and quenching of internal resonances inside the particles, which depend both on the imaginary part of the refractive index and on the size parameter, and to some extent on the real part of the refractive index. By contrast, small-scale surface roughness becomes the dominant morphological feature for large particles. This effect is likely to depend on the amplitude of the surface roughness, the relative significance of internal resonances, and possibly on the real part of the refractive index. The extinction cross section is rather insensitive to surface roughness, while the single-scattering albedo, asymmetry parameter, and the Mueller matrix are strongly influenced. Small-scale surface roughness reduces the backscattering cross section by up to a factor of 2-3 as compared to size-equivalent particles with a smooth boundary surface. This can have important implications for the interpretation of lidar backscattering observations.     

随机取向团簇自然气溶胶光学特性

利用离散偶极子近似法计算分析了随机取向团簇自然气溶胶(包含灰尘和海盐)在等效半径变化范围为0.01～2 m（波长为0.55 m时对应尺度参数为0.1～23)时的光学特性。通过考察成分和形状的影响,计算结果表明:成分对团簇自然气溶胶的散射、后向散射效率因子,不对称因子,以及米散射区范围内的消光效率因子的影响均较小,其中对尺度参数为9～23时的消光效率因子和尺度参数小于2.3时的不对称因子几乎没有影响;成分对瑞利散射区范围内的消光效率因子及吸收效率因子的影响相对较大。形状对团簇自然气溶胶在尺度参数小于0.7时的消光、吸收、散射效率因子及后向散射效率因子的影响可以不计;当尺度参数大于4.6时,粒子的内在对称性和表面的突变会带来明显的影响。另外,团簇自然气溶胶在米散射区内、尺度参数较大时,散射相函数有明显的后向散射加强效应。     

沙尘气溶胶粒子群的散射和偏振特性

根据Mie散射理论,以对数正态分布函数描述沙尘气溶胶粒子群的粒径尺度分布,计算了沙尘气溶胶粒子群在0.2～40μm波段间对太阳短波辐射和地球大气长波辐射的单次散射反照率、散射相矩阵函数,揭示了不同相对湿度时,沙尘粒子群对入射辐射的散射和偏振的特征。结果表明,沙尘粒子群的单次散射反照率随着入射波长的增加有较大起伏,不同相对湿度条件下,变化趋势基本一致;在可见光、近红外波段单次散射反照率随湿度增加而变大,湿度95%时非常接近于1;大于10μm的热红外波段单次散射反照率随相对湿度增加而减小,具有较强的吸收辐射能力。散射辐射强度受湿度影响较小,随散射角的增加呈现先减小后增大的趋势,且增大的趋势随着波长的增加而减弱;不同波段上,线偏振和圆偏振随散射角和相对湿度变化存在差异;在前向和后向仅对入射辐射为圆偏振辐射产生圆偏振散射;散射光的偏振特性及其湿度差异主要表现在后向散射区,多以拱形形式体现。拱顶峰值散射角位置存在差异,且峰值散射角随相对湿度的降低向后向漂移。     

The single scattering properties of the aerosol particles as aggregated spheres

The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.     

Radiative properties of cirrus clouds in the infrared (8–13 μm) spectral region

Atmospheric radiation in the infrared (IR) 8–13 μm spectral region contains a wealth of information that is very useful for the retrieval of ice cloud properties from aircraft or space-borne measurements. To provide the scattering and absorption properties of nonspherical ice crystals that are fundamental to the IR retrieval implementation, we use the finite-difference time-domain (FDTD) method to solve for the extinction efficiency, single-scattering albedo, and the asymmetry parameter of the phase function for ice crystals smaller than 40 μm. For particles larger than this size, the improved geometric optics method (IGOM) can be employed to calculate the asymmetry parameter with an acceptable accuracy, provided that we properly account for the inhomogeneity of the refracted wave due to strong absorption inside the ice particle. A combination of the results computed from the two methods provides the asymmetry parameter for the entire practical range of particle sizes between 1 and 10,000 μm over the wavelengths ranging from 8 to 13 μm. For the extinction and absorption efficiency calculations, several methods including the IGOM, Mie solution for equivalent spheres (MSFES), and the anomalous diffraction theory (ADT) can lead to a substantial discontinuity in comparison with the FDTD solutions for particle sizes on the order of 40 μm. To overcome this difficulty, we have developed a novel approach called the stretched scattering potential method (SSPM). For the IR 8–13 μm spectral region, we show that SSPM is a more accurate approximation than ADT, MSFES, and IGOM. The SSPM solution can be further refined numerically. Through a combination of the FDTD and SSPM, the extinction and absorption efficiencies are computed for hexagonal ice crystals with sizes ranging from 1 to 10,000 μm at 12 wavelengths between 8 and 13 μm.

Calculations of the cirrus bulk scattering and absorption properties are performed for 30 size distributions obtained from various field campaigns for midlatitude and tropical cirrus cloud systems. Ice crystals are assumed to be hexagonal columns randomly oriented in space. The bulk scattering properties are parameterized through the use of second-order polynomial functions for the extinction efficiency and the single-scattering albedo and a power-law expression for the asymmetry parameter. We note that the volume-normalized extinction coefficient can be separated into two parts: one is inversely proportional to effective size and is independent of wavelength, and the other is the wavelength-dependent effective extinction efficiency. Unlike conventional parameterization efforts, the present parameterization scheme is more accurate because only the latter part of the volume-normalized extinction coefficient is approximated in terms of an analytical expression. After averaging over size distribution, the single-scattering albedo is shown to decrease with an increase in effective size for wavelengths shorter than 10.0 μm whereas the opposite behavior is observed for longer wavelengths. The variation of the asymmetry parameter as a function of effective size is substantial when the effective size is smaller than 50 μm. For effective sizes larger than 100 μm, the asymmetry parameter approaches its asymptotic value. The results derived in this study can be useful to remote sensing studies of ice clouds involving IR window bands.     

Test of Mie-based single-scattering properties of non-spherical dust aerosols in radiative flux calculations

We simulate the single-scattering properties (SSPs) of dust aerosols with both spheroidal and spherical shapes at a wavelength of 0.55 μm for two refractive indices and four effective radii. Herein spheres are defined by preserving both projected area and volume of a non-spherical particle. It is shown that the relative errors of the spheres to approximate the spheroids are less than 1% in the extinction efficiency and single-scattering albedo, and less than 2% in the asymmetry factor. It is found that the scattering phase function of spheres agrees with spheroids better than the Henyey–Greenstein (HG) function for the scattering angle range of 0–90°. In the range of ～90–180°, the HG function is systematically smaller than the spheroidal scattering phase function while the spherical scattering phase function is smaller from ～90° to 145° but larger from ～145° to 180°.We examine the errors in reflectivity and absorptivity due to the use of SSPs of equivalent spheres and HG functions for dust aerosols. The reference calculation is based on the delta-DISORT-256-stream scheme using the SSPs of the spheroids. It is found that the errors are mainly caused by the use of the HG function instead of the SSPs for spheres. By examining the errors associated with the delta-four- and delta-two-stream schemes using various approximate SSPs of dust aerosols, we find that the errors related to the HG function dominate in the delta-four-stream results, while the errors related to the radiative transfer scheme dominate in the delta-two-stream calculations. We show that the relative errors in the global reflectivity due to the use of sphere SSPs are always less than 5%. We conclude that Mie-based SSPs of non-spherical dust aerosols are well suited in radiative flux calculations.     

Influence of the vertical profile of Saharan dust on the visible direct radiative forcing

The vertical profile of Saharan dust in the atmosphere is generally characterized by a large aerosol concentration in the mid troposphere, differently from the climatological distribution of other types of particles, that show a peak at the surface and a rapid decrease with height. Saharan dust is also characterized by particles of relatively large size of irregular shape, and variable values of the single scattering albedo (the ratio between radiation scattering and extinction). The dust's peculiar vertical distribution is expected to produce an effect on the calculation of the direct aerosol radiative forcing at the surface and at the top of the atmosphere. This effect is investigated by comparing estimates of aerosol direct visible radiative forcing at the surface and at the top of the atmosphere for dust vertical profiles measured in the Mediterranean, and for the climatological profile. The radiative forcing is estimated by means of an accurate radiative transfer model, and for the ocean surface. The sensitivity of the results on the solar zenith angle, aerosol optical depth, and aerosol absorption is also investigated. The aerosol radiative forcing at the surface shows a very small dependency on the aerosol vertical profile. At the top of the atmosphere, the radiative forcing is weakly dependent on the vertical profile (up to 10% variation on the daily average forcing) for low absorbing particles; conversely, it shows a strong dependency (the daily radiative forcing may vary up to 100%) for absorbing particles. The top of the atmosphere visible radiative forcing efficiency produced by dust having single scattering albedo <0.7 is higher by 4 W m⁻² when the observed vertical profile instead of the standard profile is used in the calculations (i.e. it produces a lower cooling). For values of the single scattering albedo around 0.67, the sign of the forcing depends on the vertical profile. The influence of the vertical distribution on the radiative forcing is largest at small values of the solar zenith angle, and at short wavelengths.