基于偏振探测的CARS非共振背景抑制与分离

为消除非共振背景干扰,提高相干反斯托克斯拉曼散射测量精度,研究了基于偏振探测的相干反斯托克斯拉曼散射非共振背景抑制与分离.首先,从理论上证明了相干反斯托克斯拉曼散射信号强度只取决于三阶非线性极化率共振部分,而与非共振部分无关,并且三阶极化率共振部分与非共振部分偏振方向不一致,为偏振相干反斯托克斯拉曼散射提供了理论支撑;然后,以平面火焰炉温度场为研究对象,设计了偏振相干反斯托克斯拉曼散射探测系统实施方案,并与热电偶、常规相干反斯托克斯拉曼散射两种方法在相同条件下开展了温度测量对比实验.实验结果表明:常规相干反斯托克斯拉曼散射方法的测量相对误差优于7%,测量相对不确定度优于7%;偏振相干反斯托克斯拉曼散射方法的测量相对误差优于4%,测量相对不确定度优于5%;相同工况条件下与常规相干反斯托克斯拉曼散射相比,偏振相干反斯托克斯拉曼散射最接近均值的拟合光谱更加平滑.偏振相干反斯托克斯拉曼散射具有更小的拟合误差,是一种更为有效的相干反斯托克斯拉曼散射诊断方法.     

亚乙基硫脲的表面增强拉曼极化率研究：电磁和电荷转移机制

测量了吸附在银电极表面的亚乙基硫脲分子在不同电位下的表面增强拉曼光谱，对光谱强度变化进行了分析.从拉曼光谱强度计算出分子的键极化率数值，分析极化率大小和变化情况，提出了分子在不同电位下表面增强效应的增强机制. 关键词： 亚乙基硫脲 表面增强拉曼极化率 电磁增强 电荷转移增强     

以Y/Ni为催化剂制备的单壁碳纳米管的拉曼光谱研究

采用电弧放电法以Y/Ni为催化制备了单壁碳纳米管（SWNTs），对样品进行了扫描电镜、透射电镜和拉曼光谱的研究。所制备的样品中单壁碳纳米管的含量较高。对单壁碳纳米管的共振拉曼散射增强效应进行了观察，随激光波长的不同，单壁碳纳米管的拉曼光谱也随之变化，尤其是低频区径向呼吸模的变化比较明显。利用布里渊区折叠法计算了单壁碳纳米管的电子态密度曲线，根据SWNTs电子态密度尖峰之间的能量差、管子的直径和呼吸模频率建立了一个图表，并对SWNTs的呼吸模进行了归属。分析结果表明：样品中单壁碳纳米管的直径分布在0.79-1.76nm范围，金属管和半导体管均存在，并且直径在1.45nm附近的碳管居多。     

单壁碳纳米管吸附对三联苯的研究

利用对三联苯对单壁碳纳米管进行了化学修饰,并利用透射电镜、紫外可见吸收光谱、拉曼光谱对修饰后的单壁碳纳米管进行了表征分析.通过对比吸附前后的紫外可见吸收光谱发现,吸附后的光谱强度大约下降63.1%,说明单壁碳纳米管吸附上了对三联苯.通过拉曼光谱分析发现,吸附后单壁碳纳米管的拉曼光谱中主要峰的位置向长波方向移动了6～7 cm-1,认为拉曼光谱发生移动的原因是单壁碳纳米管吸附对三联苯前后状态的改变导致的.     

碳纳米管应变传感测量与偏振拉曼控制方法研究

面向微尺度平面变形的精细测量对碳纳米管应变传感测量方法进行了理论与实验研究。利用碳纳米管的拉曼应变敏感性及其偏振选择性,针对各种典型的拉曼光谱系统偏振构型,推导建立了适于各种偏振拉曼构型的碳纳米管平面应变传感解析关系式。从测量学角度出发,对不同偏振构型下的应变传感进行了对比分析,得出入射与散射光偏振方向皆能够连续控制且始终保持平行的双偏协同构型最适合于平面应变传感,并进一步提出易于实现的双偏协同构型光路配置方式与控制方法。通过实验应用证明,所提出的方法能够有效的实现基于偏振拉曼的碳纳米管平面应变传感测量。     

采用圆偏振啁啾飞秒激光脉冲操控CS2分子的相干拉曼散射过程

采用两束圆偏振啁啾飞秒激光脉冲,非共线相干激发三原子分子CS₂液体. 在相位匹配的方向上,探测到由CS₂频率为397 cm^-1的振动模式产生的强度对称分布的相干反斯托克斯拉曼散射(CARS)信号和相干斯托克斯拉曼散射(CSRS)信号. 当调整两束激发光的圆偏振状态时,CARS,CSRS信号的强度、偏振、波长均发生规律性的改变:CARS,CSRS信号的强度分布反映了CS₂ 在不同极化状态下的受激拉曼散射截面大小;信号光的 关键词： 啁啾脉冲 相干反斯托克斯拉曼散射(CARS) 相干斯托克斯拉曼散射(CSRS) 2')" href="#">CS₂     

碳纳米管拉曼光谱研究新进展

本文介绍碳纳米管拉曼光谱研究的最新进展。重点介绍金属性和半导体性碳纳米管的共振拉曼效应、表面增强拉曼效应和偏振拉曼效应。同时也介绍了碳纳米管的温度效应、压力效应和杨氏模量的拉曼光谱研究     

基于偏振拉曼散射光谱的4H-SiC晶体各向异性特性研究

采用背向散射偏振配置,对半极性a面(1120)生长的4H-SiC晶体,测量了激发光偏振方向与光轴成不同角度时各声子振动的偏振拉曼散射光谱,研究了不同声子模式的偏振拉曼散射光的强度变化与性质。利用拉曼选择定则,对实验结果进行拟合分析得到了不同声子模式的拉曼散射矩阵张量元系数及其各向异性特征。研究结果为深入了解4H-SiC晶体的微观结构和各向异性性质提供依据。     

偏振拉曼实验技术研究

拉曼光谱技术作为常用的表征和测试分析手段,已被广泛的应用。本文设计搭建了基于激光显微共聚焦拉曼光谱仪的偏振拉曼光谱测试系统,将入射激光和拉曼散射的偏振引入拉曼光谱测试系统中。应用该实验平台,测试物理气相传输(PVT)法制备的4H-SiC样品,结果表明其拉曼光谱强度具有旋转偏振变化规律。本文所设计的系统将为偏振拉曼的研究提供实验基础,也为相关材料的分析提供技术保障。     

单壁碳纳米管吸附酞菁类有机物的研究

利用苯氧基酞菁修饰单壁碳纳米管,并利用透射电子显微镜、紫外可见吸收光谱、荧光光谱以及拉曼光谱进行了表征分析.在透射电镜下观察到结合物呈现糖葫芦状,吸附后吸收光谱以及荧光光谱中峰的强度明显下降说明单壁碳纳米管吸附了大量的苯氧基酞菁,通过拉曼光谱发现吸附后单壁碳纳米管的拉曼光谱中主要峰的位置向长波数方向移动,原因是单壁碳纳米管吸附苯氧基酞菁前后状态的改变导致的.     

High-resolution near-field Raman microscopy of single-walled carbon nanotubes

We present near-field Raman spectroscopy and imaging of single isolated single-walled carbon nanotubes with a spatial resolution of approximately 25 nm. The near-field origin of the image contrast is confirmed by the measured dependence of the Raman scattering signal on tip-sample distance and the unique polarization properties. The method is used to study local variations in the Raman spectrum along a single single-walled carbon nanotube.     

New features in the anti‐Stokes and Stokes Raman spectra of single‐walled carbon nanotubes that are highly separated into their semiconducting and metallic nanotube components

Surface‐enhanced Raman scattering studies were performed using nonresonant (514.5 nm) and resonant (676.4 nm) optical excitations on single‐walled carbon nanotubes thoroughly separated into semiconducting (pure 99%) and metallic (pure 98%) components. Regardless of the support (Au or Ag), the metallic nanotubes do not present an anomalous anti‐Stokes Raman emission. Regardless of whether an on‐resonant or off‐resonant optical excitation is used, only the semiconducting nanotubes produce an abnormal anti‐Stokes Raman emission that grows when increasing the excitation light intensity or temperature. The Raman studies under light polarized relative to the main nanotube axis demonstrate that only semiconducting nanotubes are sensitive toward changes in the polarization of the excitation light. Copyright © 2014 John Wiley & Sons, Ltd.     

Polarized raman study of aligned multiwalled carbon nanotubes

Polarized Raman spectra of high purity aligned arrays of multiwalled carbon nanotubes, prepared on silica substrates from the thermal decomposition of a ferrocene-xylene mixture, show a strong dependence of the graphitelike G band and the disorder-induced D band on the polarization geometry employed in the experiments. The experimental G-band intensity exhibits a minimum at straight theta(m) = 55 degrees in the VV configuration, in good agreement with theoretical predictions of a characteristic minimum at 54.7 degrees for A(1g) modes in single wall nanotubes, where straight theta(m) denotes the angle between the polarization direction and the nanotube axis.     

Dependence of the electrical properties of defective single-walled carbon nanotubes on the vacancy density

The relationship between the electric properties and the vacancy density in single-walled carbon nanotubes has been investigated from first principles as well as the dependence of the influencing range of a vacancy in the nanotube on the nanotube chirality.Compared with the long-range interaction of the vacancies in a single-walled carbon nanotube with non-zero chiral angle,a much shorter interaction was found between vacancies in a zigzag single-walled carbon nanotube.In this study,we investigated the bandstructure fluctuations caused by the nanotube strain,which depends on both the vacancy density and the tube chirality.These theoretical results provide new insight to understand the relationship between the local deformation of a defective single-walled carbon nanotube and its measurable electronic properties.     

Structural ( n, m) determination of isolated single-wall carbon nanotubes by resonant Raman scattering

We show that the Raman scattering technique can give complete structural information for one-dimensional systems, such as carbon nanotubes. Resonant confocal micro-Raman spectroscopy of an (n,m) individual single-wall nanotube makes it possible to assign its chirality uniquely by measuring one radial breathing mode frequency omega(RBM) and using the theory of resonant transitions. A unique chirality assignment can be made for both metallic and semiconducting nanotubes of diameter d(t), using the parameters gamma(0) = 2.9 eV and omega(RBM) = 248/d(t). For example, the strong RBM intensity observed at 156 cm(-1) for 785 nm laser excitation is assigned to the (13,10) metallic chiral nanotube on a Si/SiO2 surface.     

Optical studies of carbon nanotubes and nanographites

Resonance Raman and photoluminescence excitation (PLE) spectroscopies are used to study the optical properties of different types of carbon nanostructures such as carbon nanotube, nanoribbons, nanographites and graphite edges. In the resonance Raman experiments of carbon nanotubes, the (n,m) assignment is obtained by comparing the experimental and theoretical diameter and chirality dependence of the optical transitions. The influence of the environment on the optical transitions of the nanotubes is also obtained in the Raman experiments. The PLE measurements in different samples of carbon nanotubes show both direct and phonon-assisted optical transitions, and the results give new evidences that the optical transitions in nanotubes have an excitonic character, which is very strong for the low energy transitions. We also analyze the Raman spectra of nanoribbons and nanographites, showing that this technique is an important tool for defect characterization in graphitic materials, and can be used to distinguish the atomic structure of the graphite edges.     

Phonon and thermal properties of achiral single wall carbon nanotubes

A detailed theoretical study of the phonon and thermal properties of achiral single wall carbon nanotubes has been carried out using force constant model considering up to third nearest-neighbor interactions. We have calculated the phonon dispersions, density of states, radial breathing modes (RBM) and the specific heats for various zigzag and armchair nanotubes, with radii ranging from 2.8 Å to 11.0 Å. A comparative study of phonon spectrum with measured Raman data reveals that the number of Raman active modes for a tube does not depend on the number of atoms present in the unit cell but on its chirality. Calculated phonon modes at the zone center more or less accurately predicted the Raman active modes. The radial breathing mode is of particular interest as for a specific radius of a nanotube it is found to be independent of its chirality. We have also calculated the variation of RBM and G-band modes for tubes of different radii. RBM shows an inverse dependence on the radius of the tube. Finally, the values of specific heat are calculated for various nanotubes at room temperature and it was found that the specific heat shows an exponential dependence on the diameter of the tube.     

Intrinsic and extrinsic effects in the temperature-dependent photoluminescence of semiconducting carbon nanotubes

The temperature dependence of the band gap of semiconducting carbon nanotubes was measured for ten different nanotube species. The unprecedented effectiveness in avoiding the effect of external strain, or any other effects originating from the surrounding environment, lead to an accurate measurement of the band gap temperature dependence, giving fundamental insight into the nanotube electron-phonon interaction. Small but reproducible energy shifts of the emission lines with temperature were observed, showing a moderate chirality dependence, well in agreement with recent theoretical calculations. In addition to the energy shift, a substantial narrowing of the emission lines was also observed. The removal of the temperature shift of the band gap allows the precise measurement of the effect of external strain on carbon nanotubes in different environments.     

Anisotropic optical properties of mechanically aligned single-walled carbon nanotubes in polymer

We have prepared aligned single-walled carbon nanotubes in polymer by mechanical stretching. The polarized absorption and Raman spectra of the aligned samples have been investigated. The optical transitions in nanotubes strongly depend on the angle between the polarization of the incident light and the nanotube axis: the absorbance measured at the peak energy shows a maximum at =0°, and they are suppressed at =90°. Raman spectra also show strong polarization dependence, which is mainly determined by the dependence of the oscillator strength of optical transitions in nanotubes. PACS 71.35.Cc; 78.30.-j; 78.67.Ch; 73.22.-f     

Anisotropy of the Raman spectra of nanographite ribbons

A polarized Raman study of nanographite ribbons on a highly oriented pyrolytic graphite substrate is reported. The Raman peak of the nanographite ribbons exhibits an intensity dependence on the light polarization direction relative to the nanographite ribbon axis. This result is due to the quantum confinement of the electrons in the 1D band structure of the nanographite ribbons, combined with the anisotropy of the light absorption in 2D graphite, in agreement with theoretical predictions.