黑磷的多声子共振拉曼散射

黑磷由于具有独特的各向异性而受到广泛的关注.声子色散和电子能带结构的研究对于理解黑磷的性质及其在下一代各向异性纳米光电子器件中的应用有促进作用.拉曼光谱作为材料的指纹谱,可提供材料声子色散以及电子能带结构等信息.根据拉曼选择定则,多声子(两个或两个以上的声子)拉曼散射光谱可以探测整个布里渊区内的声子态密度.然而,一般来说,相比于一阶拉曼散射,高阶拉曼散射具有极低的强度.为了克服这种限制,本文通过多个激光波长来激发黑磷的拉曼光谱,观测到了丰富的二阶和三阶拉曼模.同时,采用特定的偏振配置避免了黑磷光学各向异性所导致的双折射效应对拉曼强度的影响,结合声子色散及其对称性对680—930 cm~(–1)范围内的多声子拉曼峰进行了指认,这表明非布里渊区中心的声子对黑磷的二阶和三阶拉曼散射有重要贡献.本文所提出的研究高阶拉曼散射的方法对研究其他各向异性材料中的共振拉曼光谱具有借鉴作用.     

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。     

MgB2超导薄膜的变温拉曼光谱研究

MgB₂作为迄今为止超导转变温度最高的合金超导体,由于其具有结构简单、相干长度长、晶界间不存在弱连接、上临界场很高、电-声散射时间短等特点,MgB₂超导薄膜在电子学领域有着广阔的的应用前景。拉曼光谱是研究电-声子相互作用和超导能带的一种有效方法,且已广泛用于分析MgB₂材料的电子、声子特征以及超导体能带结构,研究表明,样品质量、晶粒尺寸以及测试条件对MgB₂拉曼峰的峰位和峰形影响很大,其中拉曼光谱随温度的变化也是一个研究重点,但目前关于MgB₂变温拉曼光谱的研究,测试的温度范围相对较小,局限在83 K到室温区域或是转变温度附近。研究了大范围温度区间内MgB₂薄膜的拉曼光谱变化,采用混合物理化学沉积法在(0001)SiC衬底上制备了MgB₂多晶薄膜,薄膜的晶粒尺寸约为300 nm,超导转变温度为39.3 K,对其在10～293 K之间的拉曼光谱进行了测试,测量的波数范围为20～1 200 cm-1。变温拉曼光谱的测试结果显示,在高频620 cm-1附近以及低频80和110 cm-1附近存在MgB₂的拉曼峰。经分析,低频区域出现的两个拉曼峰的频率与超导能隙宽度相对应,表明MgB₂的双能隙特性。考虑到MgB₂中四种声子模式的拉曼活性,高频620 cm-1附近的拉曼峰应是由E_2g振动模所贡献的,且随着测试温度的降低,该拉曼峰的峰位未发生明显的偏移,但半高宽显著变小,从293 K时的380.7 cm-1减小到10 K时的155 .7 cm-1,分析表明E_2g声子与电子系统的非线性耦合所引起的非简谐效应可能是拉曼峰半高宽线性变小的主要原因。     

硅纳米线拉曼光谱的研究

声子限制效应会引起本征硅纳米线拉曼光谱红移及不对称宽化,但研究发现其并非引起硅纳米线拉曼光谱改变的主要因素。研究表明,由于在拉曼光谱测量中,通常使用的入射激光功率都在5 mW以上,激光加热会导致很高的局部温度,从而引起拉曼光谱大幅度红移并对称宽化,这是硅纳米线拉曼光谱红移的主要影响因素。另外,激光功率很高时,由激光激发的载流子会与声子发生Fano型干涉,从而使硅纳米线拉曼光谱发生Fano型红移和不对称宽化。除此之外,对小直径本征硅纳米线,声子限制效应导致波矢选择定弛则弛豫,使不在布里渊区中心的声子也可以参与拉曼散射,因而其拉曼光谱中除常见的几个拉曼峰外还会出现新拉曼峰。     

基于群论的PAHs分子偏振拉曼去噪

利用群论理论研究16种多环芳烃(polycyclic aromatic hydrocarbons,PAHs)分子振动规律,并对PAHs指纹区特征拉曼峰进行偏振去噪,减少非特征拉曼峰对特征拉曼峰的干扰,增强16种PAHs之间的拉曼辨识度。群论分析发现16种PAHs分别属于C_s,C_2v,C_2h,D_2h点群,四个点群中的A′,A₁,A_g,A_g类对称振动属于全对称振动,其余对称振动为非全对称振动,其中全对称振动均具有拉曼活性。Gaussian 09杂化密度泛函理论计算与群论分析相结合,发现16种PAHs全对称振动分布拉曼位移全区域,涵盖16种PAHs基团振动模式;全对称振动产生的波动性小,具有一定的抗外部环境干扰能力,稳定性相对较高,并且其产生的拉曼峰更强。根据全对称振动具有代表性、稳定性、显著性的特征,本文将16种PAHs的全对称振动作为特征拉曼振动。此外,研究发现,拉曼偏振效应与振动模对称性直接相关,拉曼光谱的偏振效应具有增强PAHs特征拉曼峰、降低PAHs非特征峰强度的作用。16种PAHs通过拉曼光谱的偏振效应选择性调节作用后,PAHs特征拉曼峰信噪比可提高6.52%~182%,说明利用拉曼偏振效应去除非特征拉曼峰的作用显著,可有效降低特征峰的噪声干扰。因此,所建立的基于群论的PAHs分子拉曼偏振去噪方法可以改善其拉曼光谱信号质量,提高PAHs同步拉曼光谱分析效率,为实现16种PAHs同步拉曼光谱检测提供了理论依据。     

二维材料及其异质结的声子物理研究

声子是固体最重要的元激发之一,是理解材料摩尔热容、德拜温度以及热膨胀系数等热力学性质的基础,同时电声子相互作用也决定了固体的电导和超导等特性。拉曼光谱是表征固体声子物理的重要实验手段,不仅能表征材料的结构和质量,还能提供材料声子性质、电子能带结构、电声耦合等信息。文章将拉曼光谱应用于二维材料及其范德瓦尔斯异质结的声子物理研究。先简单介绍二维材料的层间振动声子模式和层内振动声子模式,其中层间振动声子模式的频率可用线性链模型来计算,而强度则可用层间键极化率模型来解释;同类层内振动声子模式的Davydov劈裂峰之间的频率差异可用范德瓦尔斯模型拟合。随后,将这些模型推广到二维范德瓦尔斯异质结中,以转角多层石墨烯、MoS_2/石墨烯和hBN/WS_2为例介绍了范德瓦尔斯异质结的声子谱,阐述如何应用线性链模型和经典键极化率模型计算层间振动模的频率和强度,并由此给出二维范德瓦尔斯异质结的界面耦合强度和各层间呼吸模的电声耦合强度等重要参数。     

CdSe和ZnO量子点的拉曼光谱研究

本文介绍了用拉曼光谱研究CdSe和ZnO两种Ⅱ Ⅳ族量子点材料的结果,对拉曼峰进行了指认。观察到的光学声子峰位的移动被认为是由量子限制效应引起。     

不同晶粒尺寸SnO2纳米粒子的拉曼光谱研究

对晶粒尺寸在4-80 nm范围的纯SnO2纳米颗粒进行了拉曼散射研究.除了SnO2 本征拉曼振动峰外,还有几个新的拉曼振动峰和波长在700 nm左右的一个发光很强而且峰宽很大的荧光峰被观察到.结果所示,当纳米颗粒尺寸减小时,纳米SnO2 颗粒的体相特征拉曼峰变弱,而由缺陷,表面和颗粒尺寸引起的相关效应呈强势.晶粒尺寸在20 nm左右是引起体相拉曼光谱变化的临界尺寸. 晶粒尺寸在20 nm以下,其体相拉曼峰的发生宽化和峰位移动, 以及分别出现在位于571 cm-1 的表面振动峰,位于351 cm-1 处的界面峰和与表面吸附水分子及氢氧基团的N系列拉曼峰是纳米SnO颗粒的主要特征.这些结果反映了纳米颗粒的微结构变化与颗粒尺寸和表面效应以及它们之间相互作用的信息.     

非共振条件下单壁碳纳米管拉曼散射强度的计算

利用非共振情况下的键极化模型理论，对单壁碳纳米管的拉曼光谱强度进行了研究.考察了碳纳米管结构、入射光和散射光的偏振方向以及管轴的取向对散射光强度的影响.计算结果表明，光的偏振方向对拉曼散射强度影响较大，而手性对拉曼光谱的影响较小.针对碳管样品的实际情况，给出了无规取向碳管的拉曼散射光谱. 关键词： 碳纳米管 拉曼散射 声子 键极化     

不同晶粒尺寸SnO2纳米粒子的拉曼光谱研究

对晶粒尺寸在4—80nm范围的纯SnO₂纳米颗粒进行了拉曼散射研究.除了SnO₂本征拉曼振动峰外，还有几个新的拉曼振动峰和波长在700nm左右的一个发光很强而且峰宽很大的荧光峰被观察到.结果所示，当纳米颗粒尺寸减小时，纳米SnO₂颗粒的体相 特征拉曼峰变弱，而由缺陷，表面和颗粒尺寸引起的相关效应呈强势.晶粒尺寸在20nm左右是引起体相拉曼光谱变化的临界尺寸.晶粒尺寸在20nm以下，其体相拉曼峰的发生宽化和峰位移动，以及分别出现在位于571cm^-1 的表面振动峰，位于351cm-1 处的界面峰和与表面吸附水分子及氢氧基团的N系列拉曼峰是纳米SnO颗粒的主要特征.这些结果反映了纳米颗粒的微结构变化与颗粒尺寸和表面效应以及它们之间相互作用的信息. 关键词： ２')" href="#">纳米SnO_２ 拉曼光谱 荧光光谱 水分子的吸附     

Microscopic theory on the Raman spectra of transition metal dichalcogenides in CDW state

Microscopic mechanisms are clarified for Raman scattering of collective modes, i.e., amplitude and phase modes in the charge density wave (CDW) state of transition metal dichalcogenides. We study three phonon process in triple CDW state and effects of $\text{partial}$ destruction of the Fermi surface due to the phase transition. It has then been understood how both phase and amplitude modes are given Raman activity and how A-E splittings of both modes and the commensurability pinning of the phase mode are related to the three phonon process. We can also explain change of Raman intensity of the originally Raman active A_1g phonon mode at phase transition as interference between paramagnetic and diamagnetic contributions for 2HTaSe₂ as well as other materials.     

Direct observation of melted Mott state evidenced from Raman scattering in 1T-TaS_2 single crystal

The evolution of electron correlation and charge density wave(CDW)in 1T-TaS_2 single crystal has been investigated by temperature-dependent Raman scattering,which undergoes two obvious peaks of A_(1g) modes about 70.8 cm~(-1) and 78.7 cm~(-1) at 80 K,respectively.The former peak at 70.8 cm~(-1) is accordant with the lower Hubbard band,resulting in the electron-correlation-driven Mott transition.Strikingly,the latter peak at 78.7 cm~(-1) shifts toward low energy with increasing the temperature,demonstrating the occurrence of nearly commensurate CDW phase(melted Mott phase).In this case,phonon transmission could be strongly coupled to commensurate CDW lattice via Coulomb interaction,which likely induces appearance of hexagonal domains suspended in an interdomain phase,composing the melted Mott phase characterized by a shallow electron pocket.Combining electronic structure,atomic structure,transport properties with Raman scattering,these findings provide a novel dimension in understanding the relationship between electronic correlation,charge order,and phonon dynamics.     

Y_（1－x）Nd_xSr_2Cu_（2．7）Mo_（0．3）O_（7－δ）体系的拉曼和红外光谱研究

利用拉曼散射和红外吸收光谱研究了Ｙ１－ｘＮｄｘＳｒ２Ｃｕ２．７Ｍｏ０．３Ｏ７－δ（ｘ＝０，０．２，０．５，０．８，１．０）系列样品的声子振动性质。实验结果表明，对ｘ＝０的样品，在拉曼光谱中主要出现３２３，４４３，５２２和５７８ｃｍ－１几个特征峰，在中红外吸收光谱中出现５２２，５８０和６４６ｃｍ－１特征峰。随着样品中Ｎｄ组分的增加，３２３ｃｍ－１峰向低波数发生位移，而５２２和６４６ｃｍ－１峰则向高波数发生位移。本文对这些振动模进行了指认，并对其随不同样品组分的变化行为进行了讨论     

Raman spectroscopy of collective modes in charge‐density‐wave systems: the mean‐field microscopic theory

The electron‐mediated coupling of external electromagnetic fields and Raman‐active oscillations is derived for a general electronic model with multiple bands using the adiabatic approach and the explicit diagrammatic approach. The theory is illustrated on the quasi‐one‐dimensional (Q1D) quarter‐filled charge‐density‐wave (CDW) model. It is shown how the long‐range Coulomb forces and the single‐electron relaxation processes affect the Raman spectroscopy of the amplitude‐oscillation mode in clean CDW systems. It is also argued that the adiabatic treatment of the photon‐phonon coupling functions can be safely used in this case. Copyright © 2008 John Wiley & Sons, Ltd.     

Phason and amplitudon in the charge-density-wave phase of one-dimensional charge stripes in La(2-x)Sr(x)CuO4

The present systematic Raman scattering experiments reveal the phason and amplitudon of the charge density wave (CDW) mode in the charge stripes of La(2-x)Sr(x)CuO4. Only about 15% of the electronic density of states condenses into the CDW state. The symmetries of the CDW modes change by the rotation of the stripes at the insulator-metal transition. The energy of the phason is finite at 0.06 < or = x < or = 0.1 and zero at x = 0.035 and 0.115 < or = x < or = 0.135, which suggests that the CDW is commensurate at 0.06 < or = x < or = 0.1 and incommensurate otherwise. The zero-energy phason seems to reduce T(c) at x = 1/8.     

Raman scattering under extreme conditions

Raman scattering is a versatile and powerful technique and has been widely used in modern scientific research and vast industrial applications. It is one of the fundamental experimental techniques in condensed matter physics, since it can sensitively probe the basic elementary excitations in solids like electron, phonon, magnon, etc. The application of extreme conditions(low temperature, high magnetic field, high pressure, etc.) to Raman scattering, will push its capability up to an unprecedented level, because this enables us to look into new quantum phases driven by extreme conditions, trace the evolution of the excitations and their coupling, and hence uncover the underlying physics. This review contains two topics.In the first part, we will introduce the Raman facility under extreme conditions, belonging to the optical spectroscopy station of Synergetic Extreme Condition User Facilities(SECUF), with emphasis on the system design and the capability the facility can provide. Then in the second part we will focus on the applications of Raman scattering under extreme conditions to a variety of condensed matter systems such as superconductors, correlated electron systems, charge density waves(CDW) materials, etc. Finally, as a rapidly developing technique, time-resolved Raman scattering will be highlighted here.     

Sm atomic dynamics in a charge density wave compound SmNiC2

¹⁴⁹Sm nuclear resonant inelastic scattering was carried out in a charge density wave compound SmNiC₂. We have investigated temperature dependences of the Sm partial phonon density of states and recoil-free fraction at the Sm site and the average sound velocity estimated from the Sm partial density of states. The Sm partial density of states exhibits temperature dependence, suggesting that the phonon modes between 20 and 25 meV may correlate with the charge density wave. Temperature dependence of the recoil-free fraction is difficult to prove the correlation with either the charge density wave or ferromagnetic ordering. The average sound velocity obtained by the Sm partial phonon density of states exhibits temperature dependence, agreeing qualitatively with very recent elastic constant measurements.     

掺镱钒酸钇晶体的晶格振动光谱

掺镜钒酸钇晶体是一种很有应用前景的晶体材料,由于它适合于半导体激光器泵浦的全固态激光器的要求而受到人们的普遍关注。拉曼光谱是研究材料的声子能谱分布的方法。本文根据群论对称性分类,计算了掺镜钒酸钇晶体的拉曼和红外活性振动模。选择不同几何配置的拉曼光谱,获得了不同的晶格振动模并计算了不同晶格振动模的散射效率。实验证明最强的振动模来自钒氧四面体的振动。     

Semimetal-to-semimetal charge density wave transition in 1T-TiSe(2)

We report an infrared study on 1T-TiSe(2), the parent compound of the newly discovered superconductor Cu(x)TiSe(2). Previous studies of this compound have not conclusively resolved whether it is a semimetal or a semiconductor-information that is important in determining the origin of its unconventional charge density wave (CDW) transition. Here we present optical spectroscopy results that clearly reveal that the compound is metallic in both the high-temperature normal phase and the low-temperature CDW phase. The carrier scattering rate is dramatically different in the normal and CDW phases and the carrier density is found to change with temperature. We conclude that the observed properties can be explained within the scenario of an Overhauser-type CDW mechanism.     

GaAs/AlAs超晶格的近共振喇曼散射研究

本文介绍GaAs/AlAs超晶格的室温近共振喇曼散射测量结果。由于超晶格中Fr?hlich相互作用的共振增强效应,GaAs LO声子偶模的散射得到了很大的增强。和前人的结果一样,在偏振谱我们观察到了偶模。但和前人的结果不同,在退偏振谱中我们观察到的是奇模,而不是偶模。从而证明了在近共振条件下LO声子限制模仍遵从与非共振时一样的选择定则。二级喇曼散射实验结果表明,在偏振谱中二级谱是由两个偶模组合而成,而在退偏振谱中的二级谱与前人的结果不同,由一个奇模与一个偶模组合而成。上述结果与最近提出的黄朱模型的预言是一 关键词：