Simultaneous measurements of global vibrational spectra and dephasing times of molecular vibrational modes by broadband time-resolved coherent anti-Stokes Raman scattering spectrography

In broadband coherent anti-Stokes Raman scattering （CARS） spectroscopy with supercontinuum （SC）, the simultaneously detectable spectral coverage is limited by the spectral continuity and the simultaneity of various spectral components of SC in an enough bandwidth. By numerical simulations, the optimal experimental conditions for improving the SC are obtained. The broadband time-resolved CARS spectrography based on the SC with required temporal and spectral distributions is realised. The global molecular vibrational spectrum with well suppressed nonresonant background noise can be obtained in a single measurement. At the same time, the measurements of dephasing times of various molecular vibrational modes can be conveniently achieved from intensities of a sequence of time-resolved CARS signals. It will be more helpful to provide a complete picture of molecular vibrations, and to exhibit a potential to understand not only both the solvent dynamics and the solute-solvent interactions, but also the mechanisms of chemical reactions in the fields of biology, chemistry and material science.

Dynamical correlation between quantum entanglement and intramolecular energy in molecular vibrations:An algebraic approach

The dynamical correlation between quantum entanglement and intramolecular energy in realistic molecular vibrations is explored using the Lie algebraic approach. The explicit expression of entanglement measurement can be achieved using algebraic operations. The common and different characteristics of dynamical entanglement in different molecular vibrations are also provided. The dynamical study of quantum entanglement and intramolecular energy in small molecular vibrations can be helpful for controlling the entanglement and further understanding the intramolecular dynamics.

MOLECULAR DYNAMICS SIMULATION OF POLISHING PROCESS BASED ON COUPLING VIBRATIONS OF LIQUID

Molecular dynamics method is applied to study the machining mechanisms of polishing based on coupling vibrations of liquid. The physical phenomena of abrasive particles bombarding on silicon monocrystal surface are simulated using Tersoff potentials. The effects of vibration parameters, particle size, incident angle and particle material are analyzed and discussed. Material removal mechanisms are studied. Deformation and embedment phenomena are found in the simulations, Bombardment will destroy the crystal structures near the impact point, and adhesion effect is responsible for final removal of material.

Ab Initio Studies of Radicals HBX(X=H, F, Cl, Br): Molecular Structure,Vibrational Frequencies and Potential Energy

We describe high-level ab initio calculations on the BH_2, HBF, HBCl and HBBr radicals. Molecular structure,vibrational frequencies and potential energy curves of the ground state and the first excited state, which are two Renner-Teller components for a^2Π state at linearity, are studied using the basis sets aug-cc-pVTZ and icMRCI＋Q technique. On the basis of the potential energy curves, a reliable potential energy barrier to dissociation HB＋X（X=F, Cl, Br） fragments and to linearity are given. The ab initio results will add some understanding on the spectrum and the photo-dissociation dynamics of the series of radicals.

Research on the characteristics of atmospheric air dielectric barrier discharge under different square wave pulse polarities

Energy efficiency limits the application of atmospheric pressure dielectric barrier discharge(DBD),such as air purification,water treatment and material surface modification.This article focuses on the electrical and optical effects of the DBD under three square wave pulses polarities-positive,negative and bipolar.The result shows that under the same voltage with the quartz glass medium,the discharge efficiency of bipolar polarity pulse is the highest due to the influence of deposited charge.With the increase of air gap distance from 0.5 to 1.5 mm,average power consumed by the discharge air gap and discharge efficiency decrease obviously under alumina,and increase,and then decrease under quartz glass and polymethyl methacrylate(PMMA).Through spectrum diagnosis,in the quartz glass medium,the vibration temperature is the highest under negative polarity pulse excitation.Under bipolar pulse,the vibration temperature does not change significantly with the change of air gap distance.For the three dielectric materials of quartz glass,alumina and PMMA,the molecular vibration temperature is the highest under the quartz glass medium with the same voltage.When the gap spacing,pulse polarity or dielectric material are changed,the rotational temperature does not change significantly.

交叉分子束方法研究H＋CH4和H＋CD4反应：CH3／CD3的振动激发态产物通道

本文利用时间切片离子成像技术较为系统地研究了H＋CH4／CD4-H2／HD＋CH3／CD3这一反应．通过（2＋1）共振增强多光子电离技术探测了产物CH3／CD3的影像，从中发现该反应在0．72和1．06eV碰撞能下，除了基态产物外，还生成了激发态产物．这一现象并未在前人的实验中观测到．由激发态产物的图像可知，随着碰撞能的增大，产物的角分布逐渐从后向往侧向转移．通过对比产物CH3／CD3的基态与激发态的角分布，可知振动激发态产物更倾向于分布在侧向．由于散射产物的角分布主要受反应碰撞参数的影响，这一实验结果意味着碰撞参数对振动激发态产物通道有着重要的影响．

Effect of the ratio of transition dipole moments on few-cycle pulse propagation

Propagation of a few-cycle laser pulses in a dense V-type three-level atomic medium is investigated based on full-wave Maxwell-Bloch equations by taking the near dipole-dipole （NDD） interaction into account. We find that the ratio, γ of the transition dipole moments has strong influence on the time evolution and split of the pulse： when γ≤ 1, the NDD interaction delays propagation and split of the pulse, and this phenomenon is more obvious when the value of γ is smaller; when γ =√2, the NDD interaction accelerates propagation and split of the pulse.

Photo-acoustic spectrum and detection of nitrogen dioxide

The photo-acoustic （PA） spectrum of nitrogen dioxide （NO2） in the range of 420 - 520 nm with a Nd：YAG pumped optical parametric generator and amplifier as radiation source is presented. The spectrum has a characteristic of banded structure superimposed on continuum. The banded structure of the spectrum can be assigned to NO2 B2B1← X^2A1 transition. While the continual one comes from the chaos states of the first excited state A^2B2 and the high vibration levels of the ground state X^2A1. The relationship of PA signal with buffer gas pressure and NO2 concentration is measured. The PA signal intensity increases with buffer gas pressure and almost is invariable when the buffer gas pressure is more than 3.00 × 10^4 Pa. The PA signal intensity has linearity with NO2 concentration. The detection limit is about 2×10^-5 on the basis of SNR = 1, however lower value of the detection limit can be expected by improving the apparatus properties.

A procedure of determining potential energy surfaces of triatomic molecules from inversion of spectroscopic data

In this paper, we have suggested an iterative procedure of optimization of the linear parameters in an analytic potential energy function for a triatomic molecule, by combining both variational and second order perturbation methods. The most important feature of this procedure is that the objective function is an analytical expression which can be optimized easily. The application to the water molecule is presented.