基于光学传输矩阵的太赫兹时域光谱分析

提出了基于光学传输矩阵的提取太赫兹时域光谱光学参数的理论方法。相比于传统的提取主脉冲方法,该方法在未来可以推广用以分析主脉冲与次脉冲无法分辨的太赫兹时域光谱。利用该方法得到了蓝宝石(α-Al2O3)样品在0.3~1.0太赫兹频段的复折射率。通过与利用提取主脉冲方法得到的复折射率的结果比较,验证了基于光学传输矩阵的理论分析方法的可靠性和精确性。所提出的方法为今后主次脉冲无法分辨的太赫兹时域光谱的准确分析提供了坚实的理论基础。     

基于衰减全反射式太赫兹时域光谱技术的食用油光谱特性研究

食用油是人类营养和能量的重要来源,为人体提供必需的脂肪酸,研究食用油在太赫兹波段光学特性,对食用油成分分析及品质评价具有重要价值。衰减全反射式太赫兹时域光谱技术是一种新型的太赫兹时域光谱技术,通过样品与倏逝波的相互作用,获取样品的太赫兹光谱。与透射式或反射式太赫兹时域光谱技术相比,该技术能有效地避免测量食用油等液体样品时样品池对光学参数的影响,并能获得样品的精确光学参数。分别利用透射式太赫兹时域光谱技术和衰减全反射式太赫兹时域光谱技术测量了大豆油的吸收光谱。结果表明,与透射式太赫兹时域光谱技术相比,衰减全反射式太赫兹时域光谱技术能更有效地提取大豆油的吸收系数、吸收峰分布等光学特性。进一步利用衰减全反射式太赫兹时域光谱技术研究了大豆油、核桃油、葡萄籽油在太赫兹波段的光学特性,获得了三种食用油在1~1.8 THz范围内的折射率谱和吸收光谱。利用密度泛函理论计算了食用油中四种主要成分(软脂酸、硬脂酸、油酸和亚油酸)在太赫兹波段的振动、转动模式,理论计算结果同实验测量结果吻合较好。研究表明,在太赫兹波段食用油的吸收峰与所含脂肪酸分子种类与含量有关,其主要来源为脂肪酸分子的低频振动和转动。研究成果对食用油成分定性定量分析及品质检测等具有指导意义。     

延迟线位置偏差对太赫兹时域光谱系统的测量不确定度影响分析

太赫兹时域光谱技术可以快速准确地提取材料在太赫兹波段的光学常数。然而,其各组成部分在控制精度、响应误差、系统噪音以及实验操作、数据处理等方面的误差,将影响系统对材料光学常数提取的准确性。基于透射式太赫兹时域光谱系统的测量原理,分析了系统延迟线位置偏差对提取材料复折射率准确度的影响,建立了误差在样品测量过程中的传递模型,并利用MATLAB仿真了误差对提取样品复折射率影响。结果表明,样品折射率和消光系数的不确定度受到了系统延迟线位置偏差的影响,且系统延迟线位置偏差越大,样品的复折射率提取的不确定度也就越大。同时,相比消光系数,延迟线位置的偏差对样品折射率的不确定度具有更大的影响。该模型具有一定的实际意义和理论参考价值,可分析系统延迟线位置偏差对太赫兹时域光谱系统提取材料光学常数不确定度的影响,为优化太赫兹时域光谱系统提供理论指导。     

非极性有机溶剂光学参数的太赫兹波精确测量

利用太赫兹时域光谱技术对六种常用非极性有机溶剂进行了测量,其中包括正己烷、环己烷、石油醚、甲苯、四氯化碳和二硫化碳.由于这些非极性有机溶剂常用于溶解其他有机物,因此测量非极性有机溶剂的光学参数,有助于进一步研究其他有机物在太赫兹波段的各种特性.在提取有机溶剂光学参数的过程中,考虑了用于盛放液体的比色皿对太赫兹信号的影响...     

基于太赫兹时域光谱技术的光学参数提取方法的研究进展

光学参数是宏观上表征材料光学性质的物理量,间接反映了材料的微观特性,对光学参数准确的提取可以研究材料的微观性质和机理。近年来,太赫兹时域光谱技术作为一种新兴的光谱分析手段已经成为研究的热点。由于太赫兹辐射能量低并且脉冲宽度窄(皮秒量级),太赫兹时域光谱技术在提取光学参数方面具有无损伤和高时间分辨率的特点。本文总结了基于太赫兹透射和反射时域光谱技术的光学参数提取方法的研究进展,着重阐述了几种经典方法,分析了每种方法的优缺点,并讨论了太赫兹时域光谱技术用于提取材料光学参数的挑战。研究结果表明,透射法适用于对太赫兹波吸收较弱的物质,而反射法则适用于对太赫兹波有强烈吸收的材料。     

超薄金属膜在太赫兹波段的光学特性研究

超薄金属膜在太赫兹波段的探测器、反射镜、波导器件以及太赫兹量子级联激光器中得到了广泛应用。超薄金属膜的光学常数不仅是这些器件设计中不可缺少的参数,而且是开发新型光电材料的一个重要依据。文章运用太赫兹差分时域光谱技术对超薄金属铬、镍和钛膜的光学特性研究,获得其在太赫兹波段的折射率和消光系数,并根据菲涅尔公式计算入射介质为高阻GaAs时,GaAs/Metal界面的反射谱,三种金属在0.3～1.5THz的波段范围内的平均反射率均超过80%。研究超薄金属膜在太赫兹波段的反射特性,为设计性能优良的太赫兹辐射源、探测器及太赫兹光学元件奠定基础。     

太赫兹时域光谱技术对化学混合物的成分分析研究

不同化合物在太赫兹波段的吸收谱差别很大,所以存在用太赫兹光谱对化合物及混合物进行含量分析的可能。利用太赫兹时域光谱技术(THz-TDS)技术测量VC和VB1各纯化合物吸收谱,基于化合物的吸收谱,采用线性回归技术,对VC和VB1混合物的太赫兹吸收谱进行分析,得到样品中各个混合成分的相对含量。通过以VC和VB1混合物的THz吸收谱的研究为例,证实了利用整个测量波段的频谱作为化合物的指纹特征来分析化学混合物的成分和相对含量是可行的。     

表面粗糙样品的太赫兹光谱参数提取方法研究

很多物质在太赫兹波段内的光谱参数具有指纹特征,这是太赫兹技术在安检等众多领域有所应用的基础.但是,目前常用的太赫兹时域光谱(THz-TDS)技术提取物质光学参数的Duvillaret算法,要求样品上下表面平行且充分光滑.然而在很多有潜力的实际应用场合中,尤其是对于固体样品,表面粗糙度不可避免,并且不能使用模具压片等实验...     

几种塑料的太赫兹光谱检测

利用太赫兹时域光谱技术测量了聚乙烯、聚丙烯、聚氯乙烯、聚四氟乙烯和丙烯腈-丁二烯-苯乙烯的太赫兹透射谱,研究其在0.2～2.6THz频段的光谱特性,得到了在室温氮气环境下这些材料的太赫兹吸收谱和折射率色散特性.发现这五种塑料在太赫兹波段的折射率和吸收系数差异显著,折射率分别在1.35～1.85之间,聚乙烯、聚丙烯、聚四氟乙烯吸收很小,相比之下聚氯乙烯、丙烯腈-丁二烯-苯乙烯吸收很大,这为塑料种类的鉴别及高太赫兹透过率塑料衬底选择提供了依据.     

太赫兹波频域的GaAs材料特性

利用返波振荡器(BWO)系统对不同电阻率的GaAs在太赫兹波段的透射谱进行了测试,并对太赫兹波透射谱进行了计算和分析,得到不同电阻率的GaAs材料在太赫兹波0.23～0.375 THz波段范围的折射率、吸收系数和介电常数实部和虚部等光学特性参数。实验结果表明,不同电阻率的GaAs在整个测试太赫兹波频段内的折射率,吸收系数,介电常数实部和虚部均随着电阻率的增加而增加。高电阻率的GaAs材料对太赫兹波的吸收很小,其最小吸收系数可达到3.87×10-4 cm-1。同时也表明采用返波振荡器系统研究分析GaAs在太赫兹波段特性是可行的。研究不同电阻率的GaAs在太赫兹波段的光学特性,对设计高效率太赫兹波天线具有重要意义。     

Impact of post-injection strategy on the physicochemical properties and reactivity of diesel in-cylinder soot

Post injection has significant benefit in the reduction of diesel soot emissions. Therefore, there is a need to understand the effect of post-injection strategy on soot physicochemical properties and reactivity because they play an important role in soot oxidation process that governs the final soot emissions. This work focuses on the impact of post injection on the physicochemical properties and reactivity of diesel in-cylinder soot using a main plus post injection (M*P) and a single injection (M) strategy. The soot was sampled by a developed total cylinder sampling system, and the dividing points of soot formation-dominant and oxidation-dominant phases were used for studying the impacts of post injection on the characteristics of in-cylinder soot. The physicochemical properties of the soot samples, including primary particle size, nanostructure, carbon chemical state and surface functional groups, were characterized. The soot reactivity was evaluated in terms of peak temperature, burnout temperature and apparent activation energy. In the oxidation-dominant phase, the M*P soot initially possesses smaller primary particle size, shorter fringe length, larger tortuosity, lower sp²/sp³ hybridization ratio of carbon atoms and higher content of aliphatic CH groups than the M soot. The beneficial influence of physicochemical properties on soot reactivity when using post injection is validated by the thermogravimetric data, which shows that the M*P soot is more reactive than the M soot at the onset of the oxidation-dominant phase. In the M*P case, the soot generated from the main-injection combustion has lower reactivity than the soot from the post-injection combustion after they experience the soot formation-dominant phase. The results indicate that the use of post injection leads to in-cylinder soot with physicochemical properties that favor reactivity. The enhancement of reactivity means that the soot will be more readily oxidized in the subsequent combustion process, and consequently contributes to a reduction in final soot emissions.     

An analysis of the in-cylinder soots generated from the main- and post-injection combustion in diesel engines

In modern diesel engines, the exhaust soot primarily comes from the main-injection combustion and post-injection combustion. Therefore, to reduce the diesel soot emissions, it is essential to better understand the soots generated from the main-injection combustion (main-soot) and from the post-injection combustion (post-soot). This work focused on the properties of the main-soot and post-soot during the combustion process, including the primary particle size, nanostructure and soot mass. The in-cylinder soot samples were obtained using a self-developed total cylinder sampling system, and the primary particle size and nanostructure were determined using high-resolution transmission electron microscopy. The isolation of the post-soot was achieved by adding dimethyl ether to the intake gas instead of the real main-injection to create a simulated main-injection combustion environment for post-soot formation. Combustion analysis and numerical simulation results showed that the simulated combustion environment for post-soot formation generated by the DME combustion was very similar to that generated by the real main-injection combustion. During the combustion process, although the main-soot and post-soot exhibit similar variations in the primary particle size, the maximum primary particle size of the post-soot is smaller than that of the main-soot (23.38 nm for the main-soot and 20.51 nm for the post-soot). The main-soot and post-soot show almost the same trends in the nanostructure, as characterized by the fringe length, separation and tortuosity, throughout the combustion process. The introduction of the post-injection accelerates the reduction of the primary particle size of the main-soot and the increase in the structural order of the main-soot. Because a large number of the main-soot particles are oxidized during the post-injection combustion, the post-soot accounts for a considerable proportion in the engine-out soot (i.e., 42%).     

Characterization of the light scattering by ensembles of randomly distributed soot aggregates

Soot particles formed in combustion processes commonly exist in the form of ensembles of randomly distributed aggregates of small, nearly spherical monomers. In this paper, these randomly distributed aggregates are numerically generated using a combination of the cluster–cluster aggregation algorithm with the Monte Carlo method. Moreover, an efficient and accurate numerical method is presented for characterizing the light scattering by these complex soot particles illuminated by plane wave and Gaussian beam. This method exploits the unique features of the hybrid finite element-boundary integral method and, more importantly, the unique features of soot aggregates. It is designed in such a manner that it first decomposes the original problem into many sub-regions, where each primary particle is regarded as a sub-region, and then it employs the edge-based finite element method to deal with each sub-region. The sub-regions communicate through the near-field Green’s function. To reduce computational burdens, an iterative domain decomposition method in combination with parallel conjugate gradient method is adopted to solve the coupling system of equations. As an illustration, we present some of our preliminary numerical results. The results are expected to provide useful insights into the optical properties of soot particles formed in combustion processes.     

基于光谱诊断的烃类火焰碳烟形成机理研究综述

碳烟主要是烃类燃料不完全燃烧生成的产物,其对人类健康、空气质量以及燃烧装置的使用寿命都会产生有害影响。碳烟生成是一个复杂的物理化学过程,控制碳烟排放,需要克服碳烟生成和燃烧过程中物理和化学演化的巨大差异,这些差异表现为对碳烟纳观结构和表面官能团随碳烟氧化活性反应变化的深入探索研究。近些年,研究人员对碳烟的生成机理开展了系列研究,对碳烟生成各个物理化学反应阶段有了一定认识。结合光谱诊断技术可深入了解燃烧系统碳烟形成过程,确定碳烟颗粒分子组成、精细结构、浓度分布等特征,也可从碳烟结构变化、黑体辐射强度等方面详细了解碳烟形成过程。该文旨在阐述光谱诊断技术对烃类火焰碳烟表征的研究进展和发展趋势,探讨LIBS, LII和LIF等作为诊断工具在包含背景辐射的火焰中检测碳烟生成过程产生辐射强度准确性等问题。主要介绍了烃类火焰碳烟的形成机理(从前驱体产生、生长到颗粒生成、凝聚,最后进行颗粒氧化)。总结了探测碳烟性质光谱诊断方法的应用以及光谱诊断技术对燃烧过程中碳烟表征的研究现状,包括对碳烟体积分数、温度和基于图像处理的碳烟结构表征,反应碳烟前驱体(多环芳烃)、反应气氛、温度等对碳烟颗粒物生成的影响。最...     

Investigation of optical properties of aging soot

The optical properties of soot, in particular the propensity of soot to absorb and scatter light as a function of wavelength, are key parameters for the correct interpretation of soot optical diagnostics. An overview of the data available in the literature highlights the differences in the reported optical properties of aging soot. In many cases, the properties of mature soot are used when evaluating in-flame soot but this assumption might not be suitable for all conditions and should be checked. This need has been demonstrated by performed spectral resolved line-of-sight attenuation (Spec-LOSA) measurements on an ethylene/air premixed and non-premixed flame. Transmission electron microscopy of thermophoretically sampled soot was also performed to qualify the soot aging and to establish soot morphology in order to correct light extinction coefficients for the scattering contribution. The measured refractive index absorption function, E(m) _λ , showed a very strong spectral dependence which also varied with height above the burner for both flames. However, above 700 nm, the slope of the refractive index function was near zero for both flames and all measurement heights. The upper visible and near infrared wavelengths are therefore recommended for soot optical measurements.     

乙醇柴油混合燃料碳烟特性可视化研究

在一台电控共轨光学发动机上,采用高速摄影法,对不同掺混比例的乙醇柴油混合燃料进行研究,获取了缸内燃烧火焰图像,通过双色法得到表征碳烟总体分布的KL因子,分析了乙醇这种含氧生物质燃料对缸内燃烧过程和碳烟生成特性的影响。研究结果表明,随着乙醇掺入比例的增加,滞燃期相对延长,燃烧持续期缩短,火焰的亮度和分布面积都随之下降。KL因子的最高浓度降低,碳烟浓区的分布区域减小,碳烟的氧化进程加快。     

Modeling soot formation in flames and reactors: Recent progress and current challenges

The study of soot has long been motivated by its adverse impacts on health and the environment. However, this combustion knowledge is also relevant to the production of carbon black and hydrogen via methane pyrolysis which are important commodities. Over the last decade, steady progress has been made in the development of detailed continuum models of soot formation in flames and reactors. Developing more comprehensive models has often been motivated by the need for predicting soot formation over a wider range of conditions (e.g., temperature, pressure, fuels). Measurements with novel experimental techniques have given us new insights into the chemistry, particle dynamics and optical properties of soot particles and even molecules and radicals forming them. Also, multi-scale modeling has enabled us to translate the detailed mechanisms of soot processes based on first principles into computationally efficient but accurate continuum models of soot formation in flames and reactors. However, important questions remain including (1) what is the mechanism of soot inception and surface growth, (2) which gas-phase species are involved in soot inception and surface growth (3) how surface growth and oxidation are affected by soot surface properties. Proposed models need to be evaluated against experimental data over a wide range of conditions to determine their predictive strength. These questions are critical for the accurate prediction of soot formation in flames and its emissions from engines. However, this knowledge can also be used to develop predictive process design and optimization tools for carbon black and other nanocarbon formation in reactors.     

The Formation of Carbon in Combustion and how to Quantify the Impact on Human Health

We summarize our current research on combustion aerosols. First, sampling devices for the analyses of flame gases are described. The flame gas samples are investigated by mass spectroscopy and by standard aerosol techniques. Time-of-flight mass spectroscopy is well suited to study formation and growth of soot precursor molecules. Fullerenes can also be seen in some mass spectra of flame gases. Presumably, the fullerenes are evaporated from small soot particles in the mass spectrometer by the ionizing laser. Size spectra of soot particles from the flame are presented. The flame is optionally seeded with palladium aerosol to demonstrate that the particle size distribution is not altered during the sampling procedure. It is found that soot particles are already present low in the flame where large molecules are absent.Photoemission is applied to study surface properties of soot particles from the flame. It is shown that the surface of the particles is covered with polycyclic aromatic hydrocarbons (PAH). The PAH can be removed by heating and the properties of the carbon core are revealed. One can thereby distinguish a soot growth from a soot burnout region in the flame. Time-resolved desorption experiments of perylene (a PAH) from model aerosol particles are presented. It is shown that they follow a first order rate law. The photoelectric PAH sensor is introduced as a personal air quality monitor. The danger from inhaling combustion aerosol can be expressed in units of standard cigarettes.     

柴油引燃天然气的双燃料燃烧机理的研究

本文介绍在一台光学发动机上,利用高速数字摄像和数据采集技术,对柴油引燃天然气双燃料发动机的着火、火焰传播、气缸内压力、压力升高率等变化规律进行的研究。结果表明,采用双燃料的燃烧方式具有明显的多点着火型的预混燃烧特点,与采用纯柴油的燃烧方式相比,燃烧持续期短、产生的碳烟少,但爆发压力高、压力升高率大。     

随机取向烟尘团簇粒子的光学截面的数值计算

采用蒙特卡罗方法根据团簇—团簇凝聚（CCA）模型对由球形原始微粒凝聚而成的烟尘团簇粒子进行了模拟,利用离散偶极子近似（DDA）方法数值计算了不同原始微粒粒径和数目组成的随机取向的烟尘团簇粒子的总消光截面、吸收截面及散射截面等光学特性参数,研究了原始微粒粒径及数目对随机取向烟尘团簇粒子光学特性的影响。结果表明：当入射波长一定时,随机取向烟尘団簇粒子的光学特性主要取决于原始微粒的粒径和数目;烟尘团簇粒子对不同波段激光的吸收和散射存在差别,这种差别随原始微粒粒径及数目变化而变化。这一工作为研究电磁波在烟尘中的传输特性提供重要参考数据。