Raman tensor of AlN bulk single crystal

The angle dependence of optical phonon modes of an AlN bulk single crystal from the m-plane（1100） and c-plane（0001） surfaces, respectively, is investigated by polarized Raman spectroscopy in a backscattering configuration at room temperature. Corresponding Raman selection rules are derived according to measured scattering geometries to illustrate the angle dependence. The angle-dependent intensities of phonon modes are discussed and compared to theoretical scattering intensities, yielding the Raman tensor elements of A1（TO）, E22, E1（TO）, and A1（LO） phonon modes and the relative phase difference between the two complex elements of A1（TO）. Furthermore, the Raman tensor of wurtzite AlN is compared with that of wurtzite ZnO reported in previous work, revealing the intrinsic differences of lattice vibration dynamics between AlN and ZnO.

Polarization-resolved Raman spectra of α-PtO_(2)

Using density functional theory,we investigate the vibrational properties and polarization-resolved Raman spectra ofα-PtO_(2) and obtain the Raman tensor and angle-dependent Raman intensity of α-PtO_(2).It is found that the polar plot of A_(1g)mode in parallel polarization configuration is useful in identifying the orientation of the crystal.The Raman intensity of the E_(g) mode is about five times stronger than that of the A_(1g) mode.The Raman intensity is about three times stronger when the wave vector of the incident light is in x or y direction than in z direction.Our work will help the material scientists to characterize the α-PtO_(2) and to identify its orientation by comparing the experimental spectra with our result.

二十面体群C-G系数计算

本文简要介绍了计算ＣＧ系数的生群元矩阵方程法，给出计算二十面体群ＣＧ系数时采用的简化计算方法，并给出了Ⅰ群ＣＧ系数的计算结果。

基于键极化加和模型及其实验修正方法的超拉曼微观极化率张量元微分的简化方案-C_(2v)对称性

相干反斯托克斯拉曼光谱(CARS)和相干反斯托克斯超拉曼光谱(CAHRS)等高阶非线性光谱技术已经应用在动力学过程、基因表达谱筛选、高分辨率光谱分析等诸多领域。但因其涉及到的高阶微观极化率张量元数量众多,对其光谱信号进行定量分析非常困难。文献通过理论分析将CARS和CAHRS的微观极化率张量元分解为拉曼微观极化率张量元微分α′i′j′和超拉曼微观极化率张量元微分β′i′j′k′的乘积,将高阶光谱定量分析的困难简化为对低阶光谱的分析。该研究处理了具有C_(2v)对称性分子基团,提出一种利用键极化加和模型及其实验修正的方法简化超拉曼微观极化率张量元微分β′i′j′k′比值的方案。首先利用键极化加和模型方法,在对C_(2v)分子基团局域模式假设的基础上,进行单键的局域模式假设,通过对单键伸缩振动进行简正振动模式的分析,并与单键的偶极矩表达式进行比较,得到单键的超拉曼微观极化率张量元微分β′i′j′k′。在单键β′i′j′k′结果的基础上利用键极化加和模型,对C_(2v)分子基团进行对称性分析,将基团中两个单键伸缩振动的β′i′j′k′耦合,得到C_(2v)分子基团对称振动和反对称振动两种简正振动模式的超拉曼微观极化率张量元微分β′i′j′k′的表达式。在此基础上对C_(2v)分子基团对称振动和反对称振动的β′i′j′k′表达式进行理论推导,结合对应振动模式下不同偏振组合的超拉曼退偏率ρHR-SS和ρHR-AS及HV偏振组合时实验测量的超拉曼光谱强度比,得到超拉曼实验修正的C_(2v)分子基团β′i′j′k′之间的比值。再结合文献中拉曼实验修正的拉曼微观极化率张量元微分α′i′j′之间的比值,即可得到C_(2v)分子基团CARS和CAHRS的微观极化率张量元之间的比例关系,为定量分析高阶非线性光谱信息提供理论基础。

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。

含有五度旋转轴点群的超拉曼张量的计算

超拉曼散射涉及晶格振动,因此它需要由动态张量来描述。根据坐标积与张量元在对称操作下的变换形式相同的原理,通过C语言编程,计算了属于不同不可约表示的动态张量,并列出了含有五度旋转轴点群的三阶超拉曼张量。

二十面体群拉曼和超拉曼张量的计算

本文简单介绍了计算张量的不变式－协变式方法，以及根据此原理所编程序的设计思想，并在附录中给出了二十面体群（Ⅰ群）的Ｒａｍａｎ、ＨｙｐｅｒＲａｍａｎ对称（α、β、γ）张量和非对称（α－、β－、γ－）［１］张量。

采用偏振喇曼光谱研究AlN晶体(110)面的各向异性

采用平行及垂直配置下的偏振散射装置,对物理气相传输(PVT)法同质籽晶生长的六方AlN晶体进行偏振喇曼研究,测量了激发光偏振方向与光轴成不同角度时各个振动模的偏振喇曼光谱,得到不同振动模式的喇曼信号强度变化。结果表明,对于A1(TO)和E1(TO)振动模,在平行及垂直偏振配置下,其喇曼强度曲线的变化周期均为π/2,相位差均为π/4;对于E■振动模,在平行和垂直偏振配置下,其喇曼强度曲线的变化周期分别为π及π/2。通过喇曼选择定则及实验数据拟合分析得到AlN晶体各个振动模的喇曼张量比,其中,A1(TO)、E1(TO)和E■振动模的喇曼张量比为ZnO的2~3倍。垂直偏振配置下,AlN晶体的喇曼张量比远大于4H-SiC材料,为4~7倍,表明AlN晶体具有更强的各向异性,为纤锌矿结构材料的各向异性研究提供依据。

二硫化钼薄片共振拉曼光谱的偏振相关性研究

研究采用传统的二维材料制备方法——机械剥离法制备了厚度约为60 nm的MoS_(2)纳米薄片,由光学显微镜和原子力显微镜观察MoS_(2)薄片的形貌和厚度分布,并搭建了偏振拉曼测试系统,根据MoS_(2)薄片1.8 eV的能带分别选择633 nm(1.96 eV)和458 nm(2.71 eV)激光来激发MoS_(2)的共振和非共振拉曼散射,拉曼散射光经过光纤耦合进频谱仪获得拉曼光谱,由洛伦兹拟合确定了共振拉曼光谱中的特征模式,通过与非共振拉曼对比,分析出MoS_(2)的拉曼光谱在共振状态下会激发出新的拉曼模式。通过观察0°到360°之间不同偏振角度下的共振拉曼光谱和极坐标图,发现共振拉曼光谱中的所有模式均具有偏振相关性,且偏振相关的方式相似,均呈现双极纺锤形,结合拉曼张量理论模型计算出的拉曼强度理论值与实验数据几乎完全重合。

Understanding angle-resolved polarized Raman scattering from black phosphorus at normal and oblique laser incidences

The selection rule for angle-resolved polarized Raman(ARPR)intensity of phonons from standard grouptheoretical method in isotropic materials would break down in anisotropic layered materials(ALMs)due to birefringence and linear dichroism effects.The two effects result in depth-dependent polarization and intensity of incident laser and scattered signal inside ALMs and thus make a challenge to predict ARPR intensity at any laser incidence direction.Herein,taking in-plane anisotropic black phosphorus as a prototype,we developed a so-called birefringence-linear-dichroism(BLD)model to quantitatively understand its ARPR intensity at both normal and oblique laser incidences by the same set of real Raman tensors for certain laser excitation.No fitting parameter is needed,once the birefringence and linear dichroism effects are considered with the complex refractive indexes.An approach was proposed to experimentally determine real Raman tensor and complex refractive indexes,respectively,from the relative Raman intensity along its principle axes and incident-angle resolved reflectivity by Fresnel’s law.The results suggest that the previously reported ARPR intensity of ultrathin ALM flakes deposited on a multilayered substrate at normal laser incidence can be also understood based on the BLD model by considering the depth-dependent polarization and intensity of incident laser and scattered Raman signal induced by both birefringence and linear dichroism effects within ALM flakes and the interference effects in the multilayered structures,which are dependent on the excitation wavelength,thickness of ALM flakes and dielectric layers of the substrate.This work can be generally applicable to any opaque anisotropic crystals,offering a promising route to predict and manipulate the polarized behaviors of related phonons.