Optical phonons in millerite (NiS) from single‐crystal polarized Raman spectroscopy

Although several fundamental physico‐chemical aspects of nickel sulfides have been studied in detail, particularly for millerite (nickel(II) monosulfide), the most common nickel sulfide mineral, no satisfactory investigation of optical vibrational modes has been reported previously. In this paper, we provide a definitive assignment of the optical phonons in millerite, investigated by polarized Raman spectroscopy on an oriented single crystal. The impact of the power of the incident laser beam on the spectra has also been investigated, revealing evidence for degradation in the quality of the spectra at sufficiently high laser power. Copyright © 2008 John Wiley & Sons, Ltd.     

喇曼感生克尔效应光谱的琼斯矩阵分析

介绍喇曼感生克尔效应光谱(RIKES)的琼斯(Jones)矩阵分析方法.探测光束的传输强度不仅由所经过的每一个光学器件的琼斯矩阵所决定,而且还受到强的泵波在非线性介质样品中感生依赖于强度的二向色性和双折射(克尔效应)对琼斯矩阵的影响.同时计及样品和光学器件由强泵波作用下感生应力和其他外部产生的线双折射对喇曼感生克尔效应光谱观察的不利影响,导出测量系统的功率传输函数的完整表达式和喇曼感生克尔效应光谱的实现观察条件,最后简述以甲笨(C_7H_8)液体为试样的喇曼感生克尔效应光谱实验结果分析.     

Kerr介质中双原子与相干态光场Raman过程的腔场谱

为探讨Kerr介质和原子间的耦合作用对两个等同二能级原子与双模光场Raman相互作用过程腔场谱的影响,通过求解本征方程导出了双模相干态光场处于任意强度时腔场谱的计算公式,给出了数值计算结果.发现在两模初始场均为弱场时,Kerr介质和原子间的耦合作用对谱结构的影响较小;在双模初始场均为强场时,有Kerr介质加入后两模的中心主峰迅速下降,但随Kerr效应的增强,产生出越来越多的边峰,且在两模主峰的两侧产生出拱形的梳状边峰群,并伴随着峰位的向右偏移.     

Coherent coupling between vibrational modes of C-H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering(fs-CARS) measurements on liquid toluene and PVK film.For both samples,we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals.The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes,which demonstrates that a coherent coupling between the vibrational modes of the C-H chemical bonds exists at the different positions of the molecules.The dephasing times of the excited modes are obtained simultaneously.     

Coherent coupling between vibrational modes of Cben H bonds at different positions studied by femtosecond time-resolved coherent anti-Stokes Raman scattering

We performed femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) measurements on liquid toluene and PVK film. For both samples, we selectively excited the CH stretching vibrational modes and observed the expected quantum beat signals. The frequency of the well-defined beats is in good agreement with the energy difference between the two simultaneously excited modes, which demonstrates that a coherent coupling between the vibrational modes of the C-H chemical bonds exists at the different positions of the molecules. The dephasing times of the excited modes are obtained simultaneously.     

Kerr缺陷一维耦合腔光波导的双稳态方向性

本文提出一种只在一层高折射率介质层中掺杂Kerr介质的一维耦合腔光波导.利用一维传输矩阵理论和非线性传输矩阵方法研究了此结构的光学双稳态.根据一维传输矩阵理论分析了此结构的线性特性,包括低频带边模的偏移及场分布的特点,讨论了此结构实现双稳态的原理.研究发现:由于缺陷层中场分布与入射光方向密切相关,而缺陷层光场的局域,将激发Kerr介质的三阶非线性效应,从而改变了缺陷层的折射率,所以不同方向的入射光具有不同的双稳态阈值.利用非线性传输矩阵方法研究了光学双稳态特性.结果表明:由于缺陷层的位置导致缺陷模正方向（由左到右）入射的场分布大于反方向（由右到左）入射的场分布,正方向的阈值低于反方向的阈值,相差一倍.     

Ultrafast optical switching in Kerr nonlinear photonic crystals

Nonlinear photonic crystals made from polystyrene materials that have Kerr nonlinearity can exhibit ultrafast optical switching when the samples are pumped by ultrashort optical pulses with high intensity due to the change of the refractive index of polystyrene and subsequent shift of the band gap edge or defect state resonant frequency. Polystyrene has a large Kerr nonlinear susceptibility and almost instantaneous response to pump light, making it suitable for the realization of ultrafast optical switching with a response time as short as a few femtoseconds. In this paper, we review our experimental progress on the continual improvement of all-optical switching speed in two-dimensional and three-dimensional polystyrene nonlinear photonic crystals in the past years. Several relevant issues are discussed and analyzed, including different mechanisms for all-optical switching, preparation of nonlinear photonic crystal samples by means of microfabrication and self-assembly techniques, characterization of optical switching performance by means of femtosecond pump-probe technique, and different ways to lower the pump power of optical switching to facilitate practical applications in optical information processing. Finally, a brief summary and a perspective of future work are provided.     

电子-声子相互作用对柱形量子线中光学克尔效应的影响

本文利用密度矩阵方法研究了柱形量子线中的光学克尔效应, 重点讨论了电子-声子相互作用对其的影响,并以GaAs量子线为例进行了数值计算。结果显示,随着量子线半径R0的减小,光学克尔效应会逐渐增强;考虑了电子-声子相互作用时的光学克尔效应比未考虑电子-声子相互作用时的大20%多;量子线半径R0越小,峰越尖锐,峰值越强;当量子线半径R0大〖WTBZ〗于40 nm时,峰会逐渐消失.     

Partial compensation of Kerr nonlinearities by optical phase conjugation in optical fiber transmission systems without power symmetry

We investigate the suppression of Kerr nonlinearities by optical phase conjugation (OPC) in a fiber transmission system without power symmetry by including all the manifestations of the Kerr nonlinearities. We found that OPC cannot completely compensate for all Kerr nonlinearities in absence of power symmetry, and some nonlinearities may become even worse if one of the nonlinearities is fully compensated. Therefore, it is necessary to optimize the compensation system to eliminate the most dominating nonlinearity. Simulation results are presented to demonstrate the interplay of various kinds of nonlinearities. The need of proper design for transmission systems to suppress the dominating nonlinear effect is shown when all manifestations of Kerr nonlinearity are not compensated simultaneously.     

Kinetics of irreversible transformations in a glassy crystal studied by infrared spectroscopy

The kinetics of the transformation between phases I, II and III of solid cyclohexanol was studied by Fourier transform infrared spectroscopy. Special attention was paid to the dependence of the time evolution on the thermal history of the sample. We observed drastic change of the kinetics after 48 hours of aging in the glassy state. The time evolution of the spectra was described by a power low rather than an exponential one.     

Coherent molecular vibrational dynamics of CH2 stretching modes in polyethylene studied by femtosecond‐CARS

We have studied the coherent molecular vibrational dynamics of CH₂ stretching modes in polyethylene by time‐resolved femtosecond coherent anti‐Stokes Raman spectroscopy. We observed that the coherent vibrational relaxation of symmetric CH₂ stretching modes in polyethylene at room temperature is much faster than that previously measured in polyvinyl alcohol. In addition, it was detected that, at low temperature, the coherent vibrational relaxation of the symmetric stretching modes evidently becomes slower compared with that at room temperature. These temperature‐dependent measurements enable us to discriminate the contribution of pure dephasing mechanism, due to phonons and two‐level systems in polymer, from the contribution of lifetime of the vibrational excited state to the coherent vibrational relaxation of CH₂ stretching modes. We conclude that the coherent vibrational relaxation of symmetric CH₂ stretching modes at room temperature consists of the contribution of lifetime and approximately 1.5 times larger contribution of pure dephasing. Copyright © 2015 John Wiley & Sons, Ltd.     

极化子效应对核壳量子点中光学克尔效应的影响

在有效质量近似下利用量子力学的密度矩阵理论,采用无限深势阱模型解三维薛定谔方程得到电子的本征能量和波函数.从理论上计算了考虑极化子效应后,在导带子带间跃迁时ZnS/CdSe柱型核壳结构量子点光学克尔效应的三阶极化率.通过数值计算,分析了电子-LO声子和电子-IO声子相互作用对ZnS/CdSe柱型核壳结构量子点光学克尔效应的三阶极化率的影响.结果表明：极化子效应对光学克尔效应的三阶极化率 有很大影响,并且影响的大小与量子点的尺寸大小有关.       

Superconducting gap in iron pnictides studied by optical spectroscopy

We investigated the in-plane optical spectrum of a Co-doped Ba(Fe_0.94Co_0.06)₂As₂ single crystal showing superconductivity below . In the normal state, the low-energy optical conductivity spectrum can be decomposed into a sharp Drude term and a broad “incoherent” term. Below T_c, an s-wave-like superconducting gap appears in both components. We also investigated a magnetic or spin-density-wave gap in the detwinned parent compound.     

Characteristics of solid aerosols produced by optical catapulting studied by laser-induced breakdown spectroscopy

Optical catapulting (OC) constitutes an effective method to transport small amounts of different materials in the form of a solid aerosol. In this report, laser-induced breakdown spectroscopy (LIBS) is used for the analysis of those aerosols produced by OC. For this purpose, materials were catapulted using a Q-switch Nd:YAG laser. A second Q-switch Nd:YAG laser was used for LIBS analysis of the ejected particles. Data processing of aerosols was conducted using conditional data analysis. Also, the standard deviation method was used for the qualitative identification of the ejected particles. Two modes of interaction in OC (OC with focused or defocused pulses) have been evaluated and discussed. LIBS demonstrates that the distribution (spreading) of the ejected particles along the propagation axis increased as a function of the interpulse delay time. The mass density and the thickness of the target also play an important role in OC-LIBS.     

Low‐noise,vibrational phase‐sensitive chemical imaging by balanced detection RIKE

We perform a back‐to‐back comparison between two nonlinear vibrational imaging techniques: stimulated Raman scattering (SRS) and balanced detection Raman‐induced Kerr effect (BD‐RIKE). Using a compact fiber‐based laser system for generation of pump and Stokes signals, we image polymer beads as well as human hepatocytes under the same experimental conditions. We show that BD‐RIKE, despite the slightly lower signal levels, consistently offers an improved signal‐to‐noise ratio with respect to SRS, resulting in significantly higher image quality. Importantly, we observe that such quality is not affected by the static birefringence of the sample, which makes BD‐RIKE a robust and attractive alternative to SRS. We also highlight a unique advantage of the technique, which is its capability to easily access both the real and imaginary parts of the nonlinear susceptibility, thus allowing for vibrational phase imaging. The phase information can be readily obtained from BD‐RIKE with minimal experimental effort and provides an additional chemical selectivity channel for coherent Raman microscopy. Copyright © 2014 John Wiley & Sons, Ltd.     

Optical spectroscopy study of damage evolution in 6H-SiC by H_2~+ implantation

Lattice defects induced by ion implantation into Si C have been widely investigated in the decades by various techniques. One of the non-destructive techniques suitable to study the lattice defects in Si C is the optical characterization. In this work, confocal Raman scattering spectroscopy and photoluminescence spectrum have been used to study the effects of 134-ke V H_2~+ implantation and thermal treatment in the microstructure of 6 H-Si C single crystal. The radiation-induced changes in the microstructure were assessed by integrating Raman-scattering peaks intensity and considering the asymmetry of Raman-scattering peaks. The integrated intensities of Raman scattering spectroscopy and photoluminescence spectrum decrease with increasing the fluence. The recovery of the optical intensities depends on the combination of the implantation temperature and the annealing temperature with the thermal treatment from 700℃ to 1100℃. The different characterizations of Raman scattering spectroscopy and photoluminescence spectrum are compared and discussed in this study.     

Hydrogen bonding in homochiral dimers of hydroxyesters studied by Raman optical activity spectroscopy

Spectroscopic analysis of homochiral dimerization is important for the understanding of the homochirality of life and enantioselective catalysis. In this paper, (S)‐methyl lactate and related molecules were studied to provide detailed structural information on hydrogen bonding in homochiral dimers of chiral α‐hydroxyesters through the experimental and theoretical study of Raman optical activity. Different homochiral dimers can be distinguished by comparing their simulated Raman optical activity spectra with the experimental results. Hydrogen bonding motions are decoded with the aid of vibrational motion analysis, which are apparently involved in vibrational motions below 800 cm^–1. A common feature related to the chain‐bending mode also indicates the absolute configuration of methyl lactate and related molecules. The differing behavior of electric dipole–electric quadrupole invariants (β(A)²) compared with the electric dipole–magnetic dipole invariant (β(G′)²), suggests that the intermolecular hydrogen bonding motion behaves differently from the intramolecular one in the asymmetric molecular electric and magnetic fields. These results may help understand hydrogen‐bonded self‐recognition and other dynamical features in chiral recognition. Copyright © 2011 John Wiley & Sons, Ltd.     

The structure of solvated halide ions in dimethyl sulfoxide studied by Raman spectroscopy and X-ray diffraction

The solvation structure of chloride, bromide, and iodide ions, X⁻, in dimethyl sulfoxide (DMSO) has been investigated by using Raman spectroscopy and large angle X-ray diffraction under ambient conditions. The positively charged sulfur atom in DMSO interacts with X⁻ and slightly positively charged methyl groups in the coordinating molecules also interact with X⁻. The X⁻---S, X⁻···C, and X⁻···O distances are determined as follows: Cl⁻---S: 416, Cl⁻···C: 363, Cl⁻···O: 543, Br⁻---S: 433, Br⁻···C: 372, Br⁻···O: 544, I⁻---S: 437, I⁻···C: 374 and I⁻···O: 520 pm. The coordination numbers of DMSO molecules around the anions are six, seven and eight for Cl⁻, Br⁻ and I⁻ ions, respectively, with the uncertainty of ±1. Rather large uncertainties in the measured solvation numbers suggest large fluctuations in the solvation structure of the anions.     

Selective excitation of molecular mode in a mixture by femtosecond resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy

Femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy is used to investigate gaseous molecular dynamics. Due to the spectrally broad laser pulses, usually poorly resolved spectra result from this broad spectroscopy. However, it can be demonstrated that by the electronic resonance enhancement optimization control a selective excitation of specific vibrational mode is possible. Using an electronically resonance-enhanced effect, iodine molecule specific CARS spectroscopy can be obtained from a mixture of iodine-air at room temperature and a pressure of 1 atm (corresponding to a saturation iodine vapour as low as about 35 Pa). The dynamics on either the electronically excited state or the ground state of iodine molecules obtained is consistent with previous studies (vacuum, heated and pure iodine) in the femtosecond time resolved CARS spectroscopy, showing that an effective method of suppressing the non-resonant CARS background and other interferences is demonstrated.