固体的光散射讲座第五讲 共振喇曼散射

共振喇曼散射能够提供的信息和普通喇曼散射很不相同.在普通喇曼散射里,入射光频率和散射光频率并不重要,重要的是散射光对入射光的频移、光的波矢和偏振态等,人们正是根据这些信息,来研究分子、液体和固体中的激发态,这些激发态的能量最多比基态大约只高出5 ×10-2eV.在共振喇曼散射里,除了上述这些信息外,入射光和散射光的频率也上升到重要的地位,只有当入射光子能量与材料体系的某个激发态能量很接近时,才能出现共振喇曼散射.在可见光区域内,光子能量范围大约是1-3eV.因此,利用共振喇曼散射,人们能够有选择地去研究特定激发态的性质.共…     

Hg1—xCdxTe的共振拉曼散射

当入射光的光子能量接近Hg1-xCdxTe的Eo △o时,发现了Hg1-xCdxTe的共振拉曼散射,观察到了“禁戒”共振增强拉曼散射,同时也观察到了二级共振拉曼散射。分析了非共振条件下能在样品的（100）面观察到微弱的“禁戒”TO2模拟及在共振条件下“禁戒”TO2模大大增强的原因。通过分析,发现由双LO声子引起的二级共振拉曼散射主要由带内的Froehlich相互作用造成的。     

利用径向呼吸模及其倍频模的共振特性精确测定单壁碳纳米管的电子跃迁能量

提出一个根据拉曼基频模及其倍频模的斯托克斯和反斯托克斯拉曼成分的不同共振行为来探测样品与激光共振的系统能级的方法.此方法被应用到不均匀单壁碳纳米管束样品中某一径向呼吸模频率为219波数的金属型碳纳米管.通过分析呼吸模及其倍频模和切向模的共振行为,获得了该碳纳米管的电子跃迁能量,并获得纳米管C-C最近邻重叠积分因子为2.80 eV.此数值可以很好的解释单壁碳纳米管径向呼吸模的共振行为. 关键词： 单壁碳纳米管 呼吸模 共振拉曼散射 电子跃迁能     

分子费米共振拉曼光谱强度分析

测量了CCl₄和CS₂分子的Raman光谱。用Bertran理论和群论等相关理论对其光谱强度进行了分析,获得了发生费米共振分子的拉曼光谱强度的特殊规律： (1)发生费米共振的基频和倍频(和频)间发生能量转移,两光谱强度大小相互接近,当发生费米共振的基频和倍频(和频)间距离很小时,两发生费米共振的光谱强度相等(R=1);(2)能出现倍频光谱强度高于其基频光谱强度;(3)也会观测到费米共振光谱,而观测不到参与费米共振的和频中的基频光谱。此研究对化学、材料科学中的分子结构、材料成分等研究中的谱线认证、归属有很好的参考价值。     

1,4-苯二硫醇分子的表面增强共振拉曼散射的化学增强

利用密度泛函和含时密度泛函理论方法研究了1,4-苯二硫醇分子在两个金团簇之间的表面增强拉曼散射及表面增强共振拉曼散射光谱. 采用对应四种不同形式的电荷转移激发态能量的入射光,计算了表面增强共振拉曼光谱. 结果显示,光谱增强的效果与电荷转移的形式密切相关. 不同的电荷转移形式对增强因子的贡献是有差异的.     

多光子非线性Compton散射的能量转换

研究了多光子非线性Compton散射中电子与光子的能量转换及其转换效率.结果表明:散射光子频率随电子吸收光子数n的增大而增大,随碰撞非弹性成分ξ的增大而迅速减小.在超强激光场中,当极端相对论性电子与光子发生多光子非线性Compton散射且被光场俘获时,能量转换效率趋于无限大,即电子可以从超强激光场中获得巨大的加速能量.用高速电子束入射并与光子发生多光子非线性Compton散射,是提高非线性Compton散射能量转换效率的重要途径.     

球型量子点中的电子拉曼散射

研究了球型半导体量子点中的电子拉曼散射.讨论了初态为导带全满,价带全空时的电子跃迁过程,给出了电子拉曼散射的跃迁选择定则。通过计算GaAs和CdS材料球型量子点中电子及空穴参与拉曼散射的微分散射截面,分别比较了电子和空穴的不同影响,发现电子对拉曼散射的贡献要远大于空穴的贡献;当选取不同量子点半径时,拉曼散射微分散射截面变化也非常明显;量子点尺寸不变的条件下,改变入射光子能量,可以发现,微分散射截面随入射光子能量增大而减小。     

共振拉曼效应和电子-声子耦合对线性多烯分子共振拉曼光谱的影响

线性多烯分子具有高强度且信息丰富的共振拉曼光谱,在生物学、光电材料和医学等方面都有一定应用。而含有共轭双键的短链β胡萝卜素分子是多烯分子中极具有代表性的分子。在激发光作用下π电子与CC键振动相互作用影响着吸收光谱和拉曼光谱,而共振拉曼效应和电子-声子耦合影响着共振拉曼光谱的强度、频率和线型。测量了β胡罗卜素分子在二氯乙烷中283～223 K温度范围内的紫外-可见吸收和共振拉曼光谱。研究了共振效应和电子-声子耦合对吸收光谱和拉曼光谱的变化所起的作用。获得随着温度的降低,黄昆因子减小,表明CC键的振动减弱,分子体系能量减小,吸收峰红移;随着温度的降低,分子有序性提高,电子-声子耦合强度增加,增强了电子能隙对CC键振动的调制作用,拉曼模频率向低波数方向移动,即拉曼光谱红移;同时,经过计算发现随着温度的降低,β胡萝卜素分子C-C和C═C的拉曼散射截面增加,线宽变窄,倍频与基频强度比增加。对比和分析了共振效应和电子-声子耦合作用对拉曼光谱的拉曼散射截面、线宽和倍频与基频强度比的影响。虽然共振效应和电子-声子耦合作用在不同温度下对拉曼光谱都有一定影响,但研究发现不同温度下共振效应对拉曼光谱的影响要大于电子-声子耦合,且电子-声子耦合对谐波的影响更小。这是由于随着温度的降低,发生红移的紫外可见吸收光谱,使拉曼光谱中514.5 nm激发光更接近00吸收峰,明显的增强了分子的共振效应,使其拉曼散射截面,线宽,倍频与基频强度比随温度有很大变化。该研究对共振效应和电子-声子耦合的研究为研究温度对胡萝卜素等线性多烯分子性质的影响提供一定实验和理论依据。     

激光场作用下钠原子的近共振散射和碰撞感生荧光

一、引 言 关于原子共振和近共振吸收和散射的研究,对于认识等离子体和中性气体的辐射能量转移过程以及原子之间相互作用的特性是非常重要的; 特别是近共振散射能量再分布的研究对于了解星际和星际系介质中辐射能量转移过.程是很关键的.但目前,关于近共振散射再分布函数的直接测量进行得很少.Carlsten等人利用脉冲染料调频激光器,将其频率调到Sr原子4607A0(1p01-1s0)共振线附近,测量了近共振散射光谱的再分布,得到了瑞利散射与△-2(△表示入射激光频率ωl与原子共振频率ω。之差)成比例,得到了感生的共振荧光随△的变化曲线及其随△符号变…     

共振拉曼光谱技术应用综述

拉曼光谱是提供物质结信息的强有力工具。但由于拉曼散射信号弱,灵敏度低,因此应用范围受到限制。而在共振拉曼光谱(RRS)中,由于激发光源频率落在分子的某一电子吸收带内,分子吸收光子向电子激发态的跃迁变成了共振吸收,因此对入射光的吸收强度大大增加。与常规拉曼光谱相比,RRS能够提高信号强度的106倍。因此,RRS检测技术以其更高的灵敏度和选择性而具有更广的应用,特别是在生物学及医学等领域。如：(1)生物基质中的类胡萝卜素和叶绿素等色素分析;(2)细胞、蛋白质和DNA等有机物研究以及一些临床疾病诊断。RRS可以得到在常规拉曼光谱中隐藏的、更为重要的分子结构信息。RRS总是在很低的浓度下测试,且共振拉曼增强的谱线是属于产生电子吸收的基团,这对于有色物和生物样品尤为重要。因为很多这类样品的活性部位接近于生色基团,且研究对象往往是生物大分子的某一部分,所以在研究生物物质的结构和功能的关系时,RRS起着重要作用。近年来,由于光谱技术的发展使得RRS检测技术得到创新与延伸,如液芯光纤共振拉曼光谱和透射共振拉曼光谱等新技术的应用。通过对近几年有关RRS技术应用的原始论文、数据和主要观点进行归纳整理与分析提炼,介绍了RRS这一专题的历史背景和研究现状,分别对共振拉曼光谱的色素检测、生物检测和爆炸物检测等应用领域展开详细的综述,并介绍了相关新技术的发展应用。随着光谱技术的快速发展,RRS必将在科研领域拥有其他光谱技术不可取代的重要地位。     

Der Resonanz-Raman-Effekt bei Erregung im Absorptionskontinuum

When the frequency used for excitation of Raman spectra of gases is high enough to reach the region of continuous absorption typical resonance Raman spectra may be observed. It is shown theoretically that the scattering formula for this case leads to selection rules at variance with the normal Raman effect, allowing an enhanced appearance of overtones. Also this resonance Raman effect has to be understood as a single quantum process.     

Orbital ordering in LaMnO3 investigated by resonance Raman spectroscopy

Orbital ordering leads to an unconventional excitation spectrum that we investigate by resonance Raman scattering using incident photon energies between 1.7 and 5.0 eV. We use spectral ellipsometry to determine the corresponding dielectric function. Our results show resonant behavior of the phonon Raman cross section when the laser frequency is close to the orbiton-excitation energy of 2 eV in LaMnO3. We show an excellent agreement between theoretical calculations based on the Franck-Condon mechanism activating multiphonon Raman scattering in first order of the electron-phonon coupling and the experimental data of phonons with different symmetries.     

Excitation profiles of resonant coherent Raman scattering by impurity molecules

The amplitudes and the excitation profiles of coherent resonant Raman scattering (coherent anti‐Stokes and Stokes Raman scattering (CARS and CSRS)) by impurity centers in crystals and/or molecules in solutions are studied, taking into account the coherence of the excited mode and the inhomogeneity of the environment. The CARS and CSRS excitation profiles can directly be related to one‐photon absorption when using the transform theory known from spontaneous resonant Raman scattering. The enlargement of the amplitude of the active mode reveals itself in an enhancement of the vibrational overtones. At large amplitudes, a splitting in the profiles caused by the contribution of two turning points of a strong coherent vibration is observed. The inhomogeneous broadening is different in the excitation profiles of CARS and CSRS. The overlapping contributions to spectrally narrow and broad transitions lead to Fano peculiarities. The effects are illustrated by model calculations. Copyright © 2011 John Wiley & Sons, Ltd.     

Resonant enhancement of inelastic light scattering in strongly correlated materials

We use dynamical mean field theory to find an exact solution for inelastic light scattering in strongly correlated materials such as those near a quantum-critical metal-insulator transition. We evaluate the results for q=0 (Raman) scattering and find that resonant effects can be quite large, and yield a double resonance, a significant enhancement of nonresonant scattering peaks, a joint resonance of both peaks when the incident photon frequency is on the order of U, and the appearance of an isosbestic point in all symmetry channels for an intermediate range of incident photon frequencies.     

利用拉曼散射、共振拉曼散射及瑞利散射对ZnSe-ZnS多量子阱材料光谱的判定

利用拉曼散射、共振拉曼散射及瑞利散射对ＺｎＳｅ┐ＺｎＳ多量子阱材料光谱的判定赵福潭王淑梅苏锡安刘行仁（中国科学院激发态物理开放研究实验室长春１３００２１）ＤｉｓｔｉｎｇｕｉｓｈｉｎｇｏｆＬｕｍｉｎｅｓｃｅｎｃｅＳｐｅｃｔｒａｉｎＺｎＳｅ┐ＺｎＳＭＱＷ...     

Bistability in coherent two-photon processes

Using the coupled Maxwell-Bloch equations for coherent two photon processes, we show the existence of bistable behavior of systems undergoing coherent two photon resonant processes such as two photon absorption and Raman process. The system is taken to be contained in a ring cavity. The dependence of the bistable behavior on detuning parameter and the Stark shifts is also discussed.     

Resonant two-magnon Raman scattering and photoexcited States in two-dimensional mott insulators

We investigate the resonant two-magnon Raman scattering in two-dimensional (2D) Mott insulators by using a half-filled 2D Hubbard model in the strong coupling limit. By performing numerical diagonalization calculations for small clusters, we find that the Raman intensity is enhanced when the incoming photon energy is not near the optical absorption edge but well above it, being consistent with experimental data. The absence of resonance near the gap edge is associated with the presence of background spins, while photoexcited states for resonance are found to be characterized by the charge degree of freedom. The resonance mechanism is different from those proposed previously.     

Theoretical study of the continuous evolution of a resonance fluorescence spectrum towards a resonance Raman spectrum

A theoretical model is proposed to interpret the continuous transition from a resonance fluorescence spectrum to a resonance Raman spectrum, recently observed when the scattering molecule is progressively perturbed by its environment. An analytical expression for the resonant scattering tensor is given, which describes the evolution of the resonance fluorescence spectrum of a diatomic molecule perturbed by a foreign gas. The variations of the intensities and polarizations are quantitatively studied in the case of iodine, and it is shown how the resonance fluorescence spectrum is progressively transformed into a resonance Raman spectrum when the pressure of the perturbing gas is increased.     

Application of quantum mechanical method to analysis of the intensity distribution in spectra of resonant hyper-Raman scattering of low-symmetry molecules

The quantum-mechanical method of calculating the relative intensities of lines in the spectra of resonant hyper-Raman scattering of polyatomic molecules in the Herzberg-Teller approximation is tested with respect to low-symmetry molecules. The method makes it possible to describe resonant Raman and hyper-Raman scattering spectra, as well as vibronic absorption spectra, from the same viewpoint based on a common set of parameters. The particular features of the implementation of the method are discussed based on the calculation of the spectra of resonant hyper-Raman scattering of chlorobenzene and adenine, and the expedience of the application of the method is illustrated. Satisfactory agreement is obtained between calculation results and available experimental data.