A new polar nephelometer for measurement of atmospheric aerosols

The angular dependence of light scattered by aerosol particles in the atmosphere—the aerosol phase function—is one of the key properties of every radiative transfer and climate model. Side-scattering in the atmosphere is currently believed to be underestimated by most of the radiative transfer models in certain cases. The aerosol phase function can be measured with polar nephelometers.An innovative polar nephelometer able to measure the phase function of ambient aerosol directly is presented in this publication. The performance of the device was simulated completely using ray-tracing techniques. The results of these simulations are used to interpret the measurement data precisely. The measurements with the new polar nephelometer are fully automated. The quality of the measurement results was verified using different approaches. The values of the statistical and systematic error in measuring atmospheric aerosol are about 4% each. Scattering angles from 10° to 160° were measured and it is shown that with the same design this range can be extended to 3-177° in steps of 0.16° with an aperture of less than 1.8°.Measurements of the aerosol phase function are presented and compared with data taken with an integrating nephelometer and measurements of the particulate matter concentration. All data correlate very well. The described polar nephelometer can measure the phase function and the scattering coefficient of atmospheric aerosol with high accuracy and can be used for continuous monitoring measurements as well as in field campaigns.     

Improved S-approximation for dielectric particles

The range of the applicability of the soft particles approximation (S-approximation) has been extended by means of the procedure which may be considered as a specific form of the analytic continuation. The initial element is represented by the standard version of the approximation while the branch of the continuation should be chosen in correspondence with the short wavelength asymptotic of the optical characteristic under consideration. As for the extinction efficiency of dielectric spherical particles, the improved version of the S-approximation fairly well describes the behaviour of Mie curves for particles with the refractive indices up to 2.0 or more and may be useful in order to get in the analytical form the “smoothed” Mie curves when the ripple-type fluctuations were averaged. The leading role of the van de Hulst approximation both for the electric and magnetic components of the extinction efficiency has been shown.     

Angle step selection for geometrical-optics approximation in light scattering

On the basis of the Shannon sampling theorem, we present a relationship between the maximal scattering angle step and the radius of particles in the calculation of light scattering intensity distribution. For the first rainbow intensity application, the relationship between the maximal scattering angle step and radius of particles is derived from that between the ripple frequency and radius and refractive index of particles using this method. For the geometrical-optics approximation, the incident angle is used to calculate the scattering intensity distribution. To get the highest speed, the maximal incident angle step is necessary. The relationship between the maximal step of incident angle and radius of particles is deduced from the maximal scattering angle step equation. As indicated by our result, the maximal step of the incident angle is not a constant and it varies with incident angle.     

适用于测量大气气溶胶吸收系数的光声光谱系统的研究

外部噪声和环境温湿度变化对光声池性能的影响是光声光谱技术在实际大气气溶胶吸收测量应用中遇到的主要问题。详细分析了环境温湿度变化引起的共振频率漂移对光声信号的影响,提出了抑制流动噪声和采样泵振动噪声的方法,研制完成了一套测量大气气溶胶吸收的光声光谱系统,探测极限为1.4×10-8 W·cm-1·Hz-1/2。利用NO₂气体在532 nm的吸收对光声池进行了标定,并对实际大气气溶胶的吸收特性进行了测量,结果表明光声光谱测量系统可以满足自然悬浮状态下的气溶胶吸收系数的实时测量。     

Light scattering by large Saharan dust particles: Comparison of modeling and experimental data for two samples

Light scattering by large mineral-dust particles with small-scale surface roughness is investigated by comparing model simulations with laboratory-measured scattering matrices of two distinct dust samples collected from the Sahara desert. The samples have been chosen on the basis of their large effective radii, and the simulations are based on their measured size distributions. Size parameters larger than about 30 are modeled using a modified ray-optics model RODS (Ray optics with diffuse and specular interactions), while smaller particles are simulated with a T-matrix model. RODS allows us to mimic the surface roughness of large dust particles by covering the particle surface by a thin layer of external scatterers with specific single-scattering properties. The Gaussian-random-sphere geometry is used for the shapes of large dust particles. Small particles are modeled as an axial-ratio distribution of spheroids with smooth surfaces. One of the samples consists wholly of large particles and its scattering matrix can be reproduced very well by the RODS model, except for the phase function. The incorporation of wavelength-scale roughness is, however, necessary for good fits. The other sample, consisting of both small and large particles, proves more challenging to match with simulations. The analysis indicates, however, that the difficulties arise at least partially from the small-particle contribution, while RODS results are consistent with the measurements. Further, the results imply that the agreement with measurements would improve if roughness could also be accounted for in the small-particle simulations. Overall, the RODS method seems promising for modeling the optical properties of mineral-dust particles much larger than the wavelength.     

Optimizing the discrete-dipole approximation for sequences of scatterers with identical shapes but differing sizes or refractive indices

We study scattering of light by small particles with identical shapes but either moderately differing sizes or refractive indices by utilizing the discrete-dipole approximation (DDA). Assuming that accurate DDA solutions are available for either a sequence of sizes or refractive indices, we initialize the iterative conjugate gradient solver for a new size or refractive index by making “educated guesses” of the electric field vectors using classical Lagrange, rational-function, and modified Adams–Bashforth–Moulton extrapolation schemes. In the present pilot study, we assess the initialization schemes for spherical and cubic particles. As compared to the common initialization using the incident electric field, we show that careful extrapolation can significantly reduce the number of iterations. At best, the computing time can decrease by an order of magnitude whereas, typically, the improvement is some tens of percent for sizes comparable to the wavelength. In solving large numbers of single-particle scattering problems, initialization via extrapolation can yield substantial savings in computing time. In particular, the present approach should prove useful when the precise scatterer sizes and refractive indices are unknown, e.g., when interpreting astronomical observations of atmosphereless solar-system objects and experimental measurements.     

Efficient numerical orientation averaging of light scattering properties with a quasi-Monte-Carlo method

We studied numerical orientation averaging with three methods for selection of orientations: lattice-grid division, crude Monte-Carlo (CMC) method, and quasi-Monte-Carlo (QMC) method. Numerical orientation averaging with these methods are carried out with a fixed orientation version of the T-matrix method for clusters of spheres. The errors of numerical orientation averaging as a function of number of orientations are investigated by comparison with results from analytical orientation averaging of the T-matrix method.We studied four types of aggregates: a bisphere, ballistic cluster-cluster aggregates of 4 and 128 monomers (BCCA4 and BCCA128), and a ballistic particle-cluster aggregate of 128 monomers (BPCA128).We studied convergence of the scattering efficiency Q_sca, absorption efficiency Q_abs, asymmetry parameter g, intensity , and degree of linear polarization P=-S₁₂/S₁₁. For the polarization, scattering angles of maximum (Θ_max) and minimum (Θ_min) polarization in results of analytical orientation averaging are considered. For the intensity, in addition to Θ_max and Θ_min, forward scattering angle (Θ=10^°) is also considered.Q_sca, Q_abs and g of bisphere, BCCA4, and BPCA128 can be obtained accurately with smallest number of orientations by using QMC among three methods. Errors in Q_sca, Q_abs and g of BCCA128 were already small for smaller number of orientations (e.g., 100) with all the three methods.P(Θ_min) generally shows slow convergence requiring several thousands of orientations to have errors less than 1%. There are also cases where convergence of P(Θ_min) within 1% error is not attained even for largest number of orientations studied in this paper (i.e., BCCA4 with lattice-grid, BCCA128 with lattice-grid, BCCA128 with CMC).Intensity of Θ=10^°, Θ_max and Θ_min, and polarization of Θ_max generally show convergence within 1% error for several hundreds to 1000 orientations with three methods for selection of orientation angles. Among three methods, QMC requires smallest number of orientations for intensity and polarization.We also investigated convergence of Θ_max and Θ_min. Convergence of Θ_max and Θ_min is generally attained for 100-1000 orientations.We also described the application of the method to the discrete dipole approximation. In these calculations, we considered three shape models with different number of dipoles and different dipole representations to describe BCCA4. The results show that scattering and absorption efficiencies, and asymmetry parameter can generally be obtained within 1% errors for all the three shape models. On the other hand, errors are larger for intensity (up to 10%) and polarization (up to 50-70%).     

Geometrical optics approximation for light scattering by absorbing spherical particles

By means of geometrical optics, an approximation method is presented to compute the light scattering intensity of absorbing spherical particles illuminated by a plane wave. For absorbing particles, the effective refractive index and the effective refractive angle are related to the complex refractive index and incident angle. The formulas for calculation of the break of phases of reflection and refraction, which are different from the case of transparent particles, are exactly derived. Verification of the geometrical optics approximation (GOA) was performed by case studies and comparison of the present results with the Mie scattering. It is found that agreement between the GOA and the Mie theory is excellent in forward directions for weakly/moderately absorbing particles. Differently, for strongly absorbing particles, good agreement between the calculation methods is in the forward directions and large scattering angles. The agreement between the GOA and the Mie theory is better for larger particles.     

介质球的各向异性瑞利散射

基于电磁场的多尺度理论,研究了各向异性介质球内、外电场的规律,导出了各向异性目标散射场的表达式,得到了各向异性介质目标散射振幅、散射截面等的解析表达式,并对其正确性进行了检验.仿真结果表明:各向异性介质球的散射具有偶极辐射的特点,介电常量越大,产生的偶极矩也愈大,散射也越强.其结果可为各向异性目标监测、各向异性光散射研究等提供理论支持.     

Electrochemical properties of TiO2 nanoparticle/nanorod composite photoanode for dye-sensitized solar cells

A unique composite of TiO₂ nanoparticles (NPs) and nanorods (NRs) has been used to fabricate a photoelectrode for developing dye-sensitized solar cells (DSSCs) with higher sensitivity. The TiO₂ nanorods were synthesized using a mechanical process, in which electrospun TiO₂ nanofibers was grinded in a controlled way to obtain uniform size distribution. The characteristics of electron transport, recombination lifetime and charge collection were investigated by intensity-modulated photocurrent spectroscopy (IMPS) and intensity-modulated photovoltage spectroscopy (IMVS). Photoelectrodes prepared with the composites of NRs and NPs showed significant improvements in electron transportation compared to only NP photoelectrodes, which would enhance the photovoltaic performance of DSSCs. IMPS and IMVS measurements show that fast electron transport and slightly decreased recombination lifetime resulted in the improvement of efficiency. The highest energy conversion efficiency obtained from the photoelectrodes fabricated with the as-prepared rutile TiO₂ nanofibers at 5 wt% NR content was up to 6.1% under AM1.5G solar illumination. The results demonstrate that the composite nanostructure can take advantage of both the fast electron transport of the nanorods and the high surface area of the nanoparticles.     

Anomalous diffraction approximation method for retrieval of spherical and spheroidal particle size distributions in total light scattering

Using total light scattering technique to measure the particle size distribution has advantages of simplicity in measurement principle and convenience in the optical arrangement. However, the calculation of extinction efficiency based on Mie theory for a spherical particle is expensive in both time and resources. Thus, a simple but accurate approximation formula for the exact extinction efficiency may be very desirable. The accuracy and limitations of using the anomalous diffraction approximation (ADA) method for calculating the extinction efficiency of a spherical particle are investigated. Meanwhile, the monomodal and bimodal particle size distributions of spherical particles are retrieved using the genetic algorithm in the dependent model. Furthermore, the spheroidal model in the retrieval of non-spherical particle size distribution is also discussed, which verifies the non-sphericity has a significant effect on the retrieval of particle size distribution compared with the assumed homogeneous isotropic sphere. Both numerical computer simulations and experimental results illustrate that the ADA can be successfully applied to retrieve the particle size distributions for spherical and spheroidal particles with high stability even in the presence of random noise. The method has advantages of simplicity, rapidity, and suitability for in-line particle size measurement.     

宽带腔增强吸收光谱法测量大气NO2定标方法研究

非相干宽带腔增强吸收光谱法定量探测大气痕量气体浓度需要准确定标。以定量探测大气NO₂为目的,建立了基于蓝色发光二极管光源的非相干宽带腔增强吸收光谱测量系统,研究了(1)仅使用浓度已知的NO₂吸收光谱、(2)同时使用浓度已知的NO₂和纯氧气中氧气二聚体O₂-O₂吸收光谱、(3)利用纯氮气和纯氦气的瑞利散射消光差异等三种方法,分别获取非相干宽带腔增强吸收光谱在430～490 nm波段的镜片反射率定标曲线。三种方法得到的镜片反射率最大值对应波长均约为460 nm,但这些最大值存在一定差异,分别为0.999 25,0.999 33和0.999 37。利用NO₂样气吸收测量对比了三种定标方法,发现方法(1)与另外两种方法的测量结果不一致性分别约为14%和19%,而后两种方法所测结果的不一致性仅为4%。测量结果表明,NO₂标准气体浓度的不准确性以及壁损耗等因素恶化了方法(1)的定标精度,应尽量避免使用该定标方法。通过对实际大气中NO₂和O₂-O₂在440～485 nm波段内的同时测量,进一步验证了非相干宽带腔增强吸收光谱法的高灵敏度以及所用标定方法的有效性。     

Experimental investigation of a modified Beckmann-Kirchhoff scattering theory for the in-process optical measurement of surface quality

An experimental investigation of a modified Beckmann-Kirchhoff scattering theory applied in an in-process optical measurement of surface quality is described. The proposed theory describes the scattered light intensity distribution from a surface with the additional layers, and can be employed to analyze the surface characteristics in in-process measurement. Based on light scattering principle and machine vision method, the surface roughness is extracted to testify the correction of the modified Beckmann-Kirchhoff scattering theory. The experimental apparatus consists of a collimated laser diode, a beam splitter, a screen, a measuring lens and a camera. Test specimens with different surface roughness are studied. The results obtained demonstrate the feasibility of in-process optical measurement of surface quality using the modified model.     

Nuclear effects in the F3 structure function for finite and asymptotic Q

We study nuclear effects in the structure function F₃ which describes the parity violating part of the charged-current neuitrino nucleon deep inelastic scattering. Starting from a covariant approach we derive a factorized expression for the nuclear structure function in terms of the nuclear spectral function and off-shell nucleon structure functions valid for arbitrary momentum transfer Q and in the limit of weak nuclear binding, i.e. when a nucleus can be treated as a non-relativistic system. We develop a systematic expansion of nuclear structure functions in terms of a Q⁻² series caused by nuclear effects (“nuclear twist” series). Basing ourselves on this expansion we calculate nuclear corrections to the Gross-Llewellyn-Smith sum rule as well as to higher moments of F₃. We show that corrections to the GLS sum rule due to nuclear effects cancel out in the Bjorken limit and calculate the corresponding Q⁻² correction. Special attention is paid to the discussion of the off-shell effects in the structure functions. A sizable impact of these effects both on the Q² and x dependence of nuclear structure functions is found.     

Using the 13C/12C carbon isotope ratio to characterise the emission sources of airborne particulate matter: a review of literature

ABSTRACT

Particulate matter (PM) from atmospheric aerosols contains carbons that are harmful for living organisms and the environment. PM can originate from vehicle emissions, wearing of vehicle components, and dust. Size and composition determine PM transport and penetration depth into the respiratory system. Understanding PM emission characteristics is essential for developing strategies to improve air quality. The number of studies on carbon isotope composition (¹³C/¹²C) of PM samples to characterise emission factors has increased. The goal of this review is to integrate and interpret the findings from ¹³C/¹²C carbon isotope ratio (δ¹³C, ‰) analyses for the most common types of emission sources. The review integrates data from 25 studies in 13 countries. The range of δ¹³C of PM from vehicle emissions was from ?28.3 to ?24.5?‰ and for non-vehicle anthropogenic emissions from ?27.4 to ?23.3?‰. In contrast, PM ranges for δ¹³C from biomass burning sources differed markedly. For C₃ plants, δ¹³C ranged from ?34.7 to ?25.4?‰ and for C₄ plants from ?22.2 to ?13.0?‰. The ¹³C/¹²C isotope analysis of PM is valuable for understanding the sources of pollutants and distinguishing vehicle emissions from biomass burning. However, additional markers are needed to further distinguish other anthropogenic sources.     

Discrete sources method for light scattering analysis from 3D asymmetrical features on a substrate

The discrete sources method is extended to analyze polarized light scattering by three-dimensional asymmetrical features on a plane penetrable substrate. The strict mathematical model and corresponding numerical scheme are described. Computer simulation results of non-spherical micro-particle scattering show that particle shape has a stronger effect on measured response for normal incident scanners.     

Electron impact total ionisation cross sections for simple bio-molecules: a theoretical approach

In this article, we have reported electron impact total ionisation cross sections for the bio-molecules pyridine, pyrimidine, n-propylamine, urea, formamide and N-methylformamide from ionisation threshold to 2000 eV. The present calculations are based on the spherical complex optical potential formalism and complex scattering potential ionisation contribution method. The results obtained for pyridine and pyrimidine are compared with available theoretical and experimental results and are found to be in excellent agreement with existing data. The ionisation cross sections for other molecules are reported for the first time. An interesting relation between the peak of inelastic and ionisation cross sections with target parameters is also reported. It was found that both the cross sections at their maximum depend linearly with these parameters, confirming the consistency of the values reported here.     

Additivity rule for electron--molecule total cross section calculations at 50--5000eV: a new geometrical approach

Taking into consideration the changes of the geometric shielding effect in a molecule as the energy of incident electrons varies, this paper presents an empirical fraction, which depends on the energy of incident electrons, the target＇s molecular dimension and the atomic and electronic numbers in the molecule. Using this empirical fraction, it proposes a new formulation of the additivity rule. Employing the new additivity rule, it calculates the total cross sections of electron scattering by C2H4, C6H6, C6H14 and C8H18 over the energy range from 50 to 5000eV. In order to exclude the calculation deviations caused by solving the radial Schrodinger equation of electron scattering by atoms, here the atomic cross sections are derived from the experimental total cross section results of simple molecules （H2, O2, CO） via the inversion algorithm. The quantitative total cross sections are compared with those obtained by experiments and other theories, and good agreement is obtained over a wide energy range, even at energy of several tens of eV.     

Dipole-driven dynamics for near-threshold electron/positron interactions with pyrimidinic DNA bases: a path to compound formations

ABSTRACT

Calculations are reported for electron and positron scattering from isolated cytosine and thymine, where the two pyrimidinic single-ring DNA bases, in the gas-phase at energies near the elastic threshold, they reveal the special features of the dipole-driven scattering states. All molecules examined exhibit, in fact, supercritical (>1.67 D) permanent dipoles which can therefore also support, below threshold, excited bound compound states (M·e^? and M·e⁺) classified as dipole-bound states. The possible paths for going from above to below the energy threshold to form whole, unfragmented bound complexes are discussed for both leptonic projectiles.