关联电子体系中电子和磁的拉曼散射

周期结构的晶格振动和分子的振动或转动谱,可以看作材料的特征指纹,拉曼散射正是探测这些振动的非常灵敏和有效的技术,因此它已经被广泛地应用到基础研究和工业生产的各个方面.而原则上,通过固体中的自由载流子或自旋与光的非弹性散射过程,人们也可以获得关于电子和磁激发的重要信息.文章对电子和磁的拉曼散射基本概念作了简要介绍,并对一些关联电子体系中的拉曼实验作了简要综述.特别是在非常规超导中,拉曼散射在确定超导能隙的大小和各向异性以及配对对称性等方面发挥了独特的作用.     

铜氧化物超导体两能隙问题的电子拉曼散射理论研究

电子拉曼实验表明在空穴型掺杂的铜氧化物超导体中存在两能隙行为,即在欠掺杂区,随着掺杂浓度的降低,一个能隙逐渐增大而且在超导转变温度以上仍然存在,而另一个能隙逐渐减小且在DDW态依然存在.解释两能隙行为非常重要因为它与赝能隙的机理密切相关.本文计算了超导序和d-density-wave(DDW)序竞争机理下相图上不同区域的电子拉曼谱,发现欠掺杂区能隙表现出两能隙行为,与实验一致.特别地,本文发现B_1g峰对应能量由超导和DDW序共同决定,且随着掺杂浓度的降低而增大,在D 关键词： 两能隙 电子拉曼散射 竞争序     

线性多烯分子的π电子能隙对原子振动的调制

β胡萝卜素是典型的线性多稀分子,重要的光电材料,在医学上也有重要的作用,研究它在外场作用下分子结构和性能的变化及机理有很重要的理论和应用价值。分别测量了β胡萝卜素在二甲基亚砜中温度为81～25 ℃范围和β胡萝卜素在二硫化碳中压力为0.04～0.60 GPa范围的紫外-可见吸收和共振拉曼光谱。发现了两种不同的的光谱现象,随温度降低,二甲基亚砜中的β胡萝卜素分子的紫外-可见吸收、拉曼光谱都红移,拉曼散射截面增大;而随压强增加二硫化碳中β胡萝卜素分子的紫外-可见吸收峰也红移,但拉曼散射峰却蓝移,拉曼散射截面减小。两种实验现象不能同时用线性多烯分子的“有效共轭长度”“弱阻尼相干振动”等理论模型给予明了解释。电子—声子耦合常数,可以表征分子中的原子和电子在外界环境作用下的相互振动耦合程度的强弱。该研究依据电子—振动相互作用规律,通过分析和计算得出结论：二种实验现象都是π电子与碳碳键振动相互作用产生的,即由于温度、压力作用对β胡萝卜素分子结构及电子—振动耦合影响不同, 引起电子-声子耦合常数不同,是电子能隙对碳碳振动的调制作用而产生的两种实验结果。     

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。     

铁基超导体系基于电子关联强度的统一相图

铁基超导和铜基超导具有诸多相似性,这为建立统一的高温超导机理图像提供了可能性.然而,对铁基超导体系中无论是进行电荷掺杂、还是等价掺杂来改变化学压力,都能产生定性上类似、而细节上纷繁复杂的相图,这对建立统一的图像造成了困难.研究化学掺杂效应如何在微观上影响电子结构和超导电性,区分主导超导电性演化的主要因素和次要因素,对建立统一图像和揭示高温超导机理至关重要.本文综述了对铁基超导体系中化学掺杂效应的一系列角分辨光电子能谱研究,涵盖了基于FeAs和FeSe面的多种代表性铁基超导体系,包括异价掺杂、等价掺杂、在元胞不同位置的化学掺杂,及其对电子体系在费米面结构、杂质散射、电子关联强度等方面的影响.实验结果表明：电子关联性或能带宽度是多个铁基超导相图背后的普适参数,不同的晶格和杂质散射效应导致了并不重要的复杂细节,而费米面拓扑结构与超导电性的关联并不强.这些结果对弱耦合机理图像提出了挑战,并促使人们通过局域反铁磁交换作用配对图像在带宽演化层面上统一地理解铁基超导.     

压强对β胡萝卜素分子的电子-声子耦合常数的影响

电子-声子耦合常数不仅可以反映出分子中π电子离域程度的强弱, 有效共轭长度的大小, 同时也可以表征分子中的原子和电子在外界环境作用下的相互振动耦合程度的强弱。在一些研究中电子-声子耦合常数被定义为无量纲的系数。应用R.Tubino等引用的一种有量纲的电子-声子耦合常数, 建立其与黄昆因子的关系式, 进而可以计算出共轭键中单个振动模的数值。压强对多烯分子吸收光谱、拉曼光谱频移影响的研究已有报道, 但对拉曼散射截面、黄昆因子、电子-声子耦合常数的研究还没有报道。测量了β胡萝卜素分子在二硫化碳溶液中0.04～0.60 GPa的压强范围内的紫外-可见吸收光谱和共振拉曼光谱。实验结果表明, 随着压强的增加, CS₂溶液中的β胡萝卜素分子的紫外-可见吸收光谱的吸收带发生明显的红移现象, 而拉曼光谱的特征谱线却发生蓝移的现象, 拉曼散射截面减小, 电子-声子耦合常数增加。其机理是随着压强的增加, β胡萝卜素分子被压缩又结构有序性下降, 导致电子能隙变窄, 有效共轭长度变短, π电子离域范围减小, 拉曼散射截面减小, 黄昆因子、电子-声子耦合常数增加。     

用激光拉曼散射法测量电子线路板中元件的温度

本文针对电子学中电子线路板上元器件通电后要精确测量其温度的问题引入了激光拉曼散射光谱技术,介绍了该方法在无损伤探测电子元器件(通各种电流后)表面温度方面的应用,为设计电子线路板散热问题提供了可参考的数据。并开拓了激光拉曼散射光谱技术在电子学中的应用,也同时为测量复杂结构物体表面温度提供了较好的方法。     

低能电子与N2分子碰撞的振动共振激发散射截面的密耦合研究

使用经孙卫国教授改进后的振动密耦合散射方法和基于量子力学从头计算得到的静电、交换与极化散射作用势,研究了低能电子与N2分子的振动激发散射截面.研究表明在振动密耦合计算中使用18个振动波函数和12个分波数目,可以得到收敛的0→5,1→5等高激发散射的积分和微分截面.     

p型掺杂Si/Ge量子点的电子拉曼散射(英文)

在本文中我们首次报道了p型掺杂的自组织Si/Ge量子点中空穴能级子带间的电子拉曼散射,此电子跃迁的能量为105meV。Si/Ge量子点Ge Ge模的共振拉曼散射表明此空穴能级间的电子拉曼散射与Γ点附近的E0(≈2.52eV)发生了共振,而E1的能量小于2.3eV.变温实验和偏振实验进一步证实了我们的指认。所有观测的实验数据与6 bandk·p能带结构理论的计算结果吻合得很好。     

新型高分辨率电子能量损失谱仪与表面元激发研究

高分辨率电子能量损失谱仪利用单色平行电子束入射样品表面,与表面吸附基团的化学键振动、表面声子、电子及其集体激发模式等相互作用而被散射,通过分析散射电子的能量和动量,可以测量表面化学键、晶格动力学、电子态占据以及表面等离激元等的精确信息,是表面科学研究的有力工具.最近,能够对电子能量、动量做二维成像探测分析的半球形电子能量分析器被引入电子能量损失谱仪,实现了高能量、动量分辨率的高效率测量.在对FeSe/SrTiO_3界面超导增强物理机制的研究中,不同厚度的FeSe膜表面的电子能量损失谱表明衬底光学声子产生的偶极电场能够穿透到薄膜内部,诱导较强的电子-声子耦合作用,从而增强薄膜中电子的配对作用,进而使超导转变温度显著提高.三维拓扑绝缘体Bi_2Se_3表面大动量范围的电子能量损失谱还显示出一支奇异的电子集体激发模式,其色散特征不受晶格周期性的限制,而且其寿命和强度几乎不随动量的增加而衰减.这说明在拓扑绝缘体表面,不仅是狄拉克电子态本身,其集体激发也受到拓扑保护.充分发挥新型电子能量损失谱仪观测表面元激发分辨率高、动态范围大的优势,将有力地推动表面界面凝聚态物理问题研究的深入和发展.     

Raman scattering for weakened bonds in the intermediate state: enhancement of low-frequency vibrations

A multimode theory of the Raman scattering in resonance with an electronic transition causing a strong weakening of atomic bonds is proposed. Simple analytical relations between the Fourier transforms of the first- and second-order Raman amplitudes and the absorption are derived. It is predicted that the Raman scattering on low-frequency vibrations will be strongly enhanced. Besides the second-order Raman scattering is also enhanced as compared to the first-order scattering. The Raman excitation profiles show a structure caused by the Airy oscillations. The shapes of the profiles of all vibrations contributing to the weakening bond are the same as a consequence of the strong mode mixing under the virtual vibronic transition.     

Neutron Scattering and Vibrational Spectra of Molecular Crystals

Infrared and Raman spectra of a number of molecular crystals have been measured for studying molecular vibrations and the intermolecular and intramolecular force fields. The infrared absorption bands arise from interaction of the electric wave with the oscillating dipole moment of the crystal. Raman scattering covers inelastic photon scattering processes and accordingly Raman lines arise from the oscillating polarizability of the crystal. Thus, the vibrational modes observed in infrared absorption or Raman scattering spectra are k = 0 modes, for which translationally equivalent molecules vibrate in phase.     

Surface plasmon polariton contributions to strokes emission from molecular monolayers on periodic Ag surfaces

Surface enhanced Raman scattering from molecular monolayers adsorbed on a holographic grating and covered by Ag has been studied. The coupling of surface plasmon polaritons to light through the grating produces emission similar to the continuum observed in other surface Raman experiments. The angular dependence of the surface Raman scattering shows that enhanced Raman cross-sections can arise from scattering of surface plasmon polaritons into light by the localized molecular vibrations.     

Background-free coherent Raman spectroscopy by detecting the spectral phase of molecular vibrations

We propose and demonstrate a new approach to subtracting high nonresonant background in coherent anti-Stokes Raman scattering spectroscopy. The method is based on the retrieval of the spectral phase of molecular vibrations using the technique of frequency-resolved optical gating of Raman scattering. In the presence of high nonresonant background the retrieved phase corresponds directly to the background-free spectrum of the coherent Raman response.     

Picosecond stimulated Raman scattering in crystals

The comparative values of the peak and integral cross sections of spontaneous Raman scattering and the optical dephasing time of molecular vibrations were determined for several oxide crystals by spontaneous Raman spectroscopy. The spectral, time, and energy parameters of stimulated Raman scattering (SRS) were measured for ten crystals using picosecond YLF: Nd laser pumping with a radiation wavelength of 1047 nm. An analysis of the experimental dependence of the threshold energy of pumping SRS on the integral and peak cross sections of spontaneous Raman scattering showed that the SRS gain increment explicitly depended on the integral cross section and was independent of the peak cross section of spontaneous Raman scattering as the ratio between the pumping pulse width (11 ps) and the time of optical dephasing of molecular vibrations changed from 0.42 to 9.3. The gain coefficients of steady-state stimulated Raman scattering under threshold stimulated Raman scattering conditions were determined for all the crystals studied on the basis of the measured threshold SRS pumping energies, the duration and width of the spectrum of pulses, the nonlinear interaction length, the intensity of pumping, and the theoretical dependences that relate the steady-state and transient SRS gain increments. The steady-state SRS gain coefficients obtained in this work fitted well a linear dependence on the peak cross sections of spontaneous Raman scattering, which substantiated the correctness of our analysis and measurements.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed. The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together. Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

Applications of stimulated Raman scattering

The applications of stimulated Raman scattering reviewed in this paper include: determination of spontaneous Raman parameters and nonlinear susceptibilities by gain measurements and coherent anti-Stokes Raman spectroscopy, excitation of molecular vibrations and lattice waves and measurement of their relaxation times, generation of intense tunable light in the infrared region of the spectrum. The main results of the theory of stimulated Raman scattering relevant to the understanding of these applications are discussed.     

Theoretical Treatment of Nonstationary Scattering by Phonons and Polaritons Part II. Transient Raman Scattering by Polaritons and Dipole Active Phonons

The stimulated Raman scattering by polaritons and phonons generated by the fluctuations of the crystal vibrations is investigated for the transient regime. The transient gain and the scattering energy is given for the case of retarded or advanced Stokes and polariton pulses in relation to the laser pulse. Moreover, the influence of phase modulation of the laser pulse on the transient SRS by polaritons is discussed.     

Quantum confinement effect in the vibrational spectrum of CdSxSe1−x quantum dots in a fluorophosphate glass matrix

The vibrational spectra of mixed cadmium sulfoselenide nanocrystals in a fluorophosphate glass matrix are investigated by Raman spectroscopy. The asymmetry of the lines of the fundamental modes of nanocrystals is experimentally observed in the region of lattice vibrations, which is interpreted as a quantum confinement effect. In the framework of the model of confined phonons, the contribution of the band states to the Raman scattering spectrum is calculated and the size of nanocrystalline regions is estimated. The results obtained are in good agreement with the data on the low-frequency Raman scattering in these objects.