使用斯塔克诱导的绝热拉曼通道技术实现D2分子的高效相干布居转移

使用斯塔克诱导的绝热拉曼通道技术,成功地将分子束中的D₂分子从(v=0, J=0)转移至(v=1, J=0). 激发效率达到了75%.该技术将为交叉分子束和分子束-表面散射实验研究氢分子的振动激发对化学反应的影响提供一个独特的工具.     

光泵重水气体产生THz激光的半经典理论分析

从半经典密度矩阵理论出发，采用三能级系统模型对光泵重水气体产生太赫兹激光进行了理论分析，求解得到了脉冲光泵重水气体分子产生太赫兹激光过程中激光信号增益系数G_s和抽运光信号被吸收系数G_p的表达式，通过迭代法对太赫兹激光信号的输出光强进行了数值计算，理论计算得到的频谱特性曲线完全符合受激Raman辐射的频谱特性，即频谱宽度较大、输出光强随抽运失谐量的改变而变化明显等特征.在脉冲激光抽运受激Raman辐射过程中，工作介质D₂O气体分子的偶极矩由于受到抽运脉冲光场的扰动发生变化，在频谱特性曲线中表现为受激辐射THz信号的谱线发生了分裂.理论计算结果与已报道的实验结果能较好地相符.     

A novel demonstration of photoacoustic Raman spectroscopy with combined stimulated Raman pumping in H2 molecule

We present the experimental demonstration of a novel, efficient, and vibrational selective technique to prepare population in vibrational level v″ = 1 using the stimulated Raman pumping. Photoacoustic Raman signal has been studied in non-radiative transitions in the molecule H₂ (v″ = 0) and (v″ = 1). The population fraction in the v″ = 1 level can be estimated by using combined photoacoustic Raman spectroscopy with stimulated Raman pumping for the first time.     

Stimulated raman pumping to H2 (v″=1, J″=1) and resonance-enhanced multiphoton ionization from it using a single laser

Light pulses from one ArF laser are used both a) to produce H₂ in v=1, J=1 of the X-state by means of stimulated Raman pumping (SRP) and b) to analyze for that state via (2+1) resonance-enhanced multiphoton ionization (REMPI). Both SRP and REMPI have been previously measured in H₂, but with a different laser for each process. Some of our laser light is Raman shifted in H₂. The resulting mixture of fundamental (193 nm) and first Stokes (210 nm) light is focused into low-pressure H₂ where the SRP and REMPI both occur. The SRP is efficient and it produces only v=1, J=1. As the laser is tuned, a REMPI spectrum occurs from excitation by two photons of 193 nm, by two photons of 210 nm, or by one photon each of 210 and 193 nm. The features of this approach are a) that the necessary temporal and spatial overlaps are automatically achieved, b) that the frequency difference generated in the Raman shifter is precisely that needed for SRP, c) that large pulse energies are available for the REMPI, and d) that only one laser is needed.     

Global fit of the high-resolution infrared spectrum of D2S

High-resolution Fourier-transform spectra of the D₂S molecule in the regions of polyads of interacting vibrational states v = 3/2, 2, 5/2, 3 and 7/2 (v = v₁ + v₂/2 + v₃) were recorded for the first time with a Bruker IFS 120 Fourier-transform interferometer and analysed. A global fit of all currently available rotation-vibration energies has been made for 22 vibrational states of the D₂S molecule. The resulting set of 231 parameters reproduces all the initial experimental data (about 3670 vibration-rotation energies which correspond to more than 9700 ro-vibrational transitions with J^max = 25) with accuracies close to the experimental uncertainties.     

Vibrational and rotational excitation effects of the N(2D) + D2(X1Σg +) → ND(X3Σ+) + D(2S) reaction

The effects of the rovibrational excitation of reactants in the N(²D) + D₂(X¹Σ_g⁺) → ND(X³Σ⁺) + D(²S) reaction are calculated in a collision energy range from the threshold to 1.0 eV using the time-dependent wave packet approach and a second-order split operator. The reaction probability, integral cross-section, differential cross-section and rate constant of the title reaction are calculated. The integral cross-section and rate constant of the initial states v = 0, j = 0, 1, are in good agreement with experimental data available in the literature. The rotational excitation of the D₂ molecule has little effect on reaction probability, integral cross-section and the rate constant, but it increased the sideways and forward scattering signals. The vibrational excitation of the D₂ molecule reduced the threshold and broke up the forward–backward symmetry of the differential cross-section; it also increased the forward scattering signals. This may be because the vibrational excitation of the D₂ molecule reduced the lifetime of the intermediate complex.     

The effect of surface temperature on H2/D2(v = 0, j = 0)–Ni(100) scattering processes

We carry out both four-dimensional (4D×2D) and six-dimensional (6D) quantum dynamics on a parametrically time- and temperature-dependent effective Hamiltonian for H₂/D₂(v = 0,j = 0)–Ni(100) collision process. Such an effective potential was derived within a theoretical framework of mean-field approximation by considering weakly correlated interaction between molecular degrees of freedom, phonon modes and electron– hole pair (elhp) coupling through a Hartree-product-type wave function, where the initial state distribution of the surface modes and elhp coupling were introduced through Bose– Einstein and Fermi– Dirac probability factor, respectively. The temperature-dependent dissociation and state-to-state transition probabilities for H₂/D₂(v = 0,j = 0)–Ni(100) system are depicted as a function of initial kinetic energ of the incoming diatom. Though such effect appears negligibly small for H₂(v = 0,j = 0)–Ni(100) system, it is prominent in the case of D₂(v = 0,j = 0)–Ni(100) collision. It appears that the change of dissociation and transition probabilities of D₂ with the increase of surface temperature is exclusively dictated by the phonon modes directed along Z-axis, but the effect of elhp coupling particularly for transition probabilities is insignificant.     

Spontaneous and stimulated red luminescence of Lu2O3: Eu nanocrystals

The spectra of spontaneous and stimulated luminescence of Lu₂O₃: Eu (7 at %) nanopowders at different optical pumping intensities have been investigated. The obtained results—changes in the shape of the red luminescence spectra and in the lifetime of the ⁵ D ₀ excited state of Eu³⁺ ions—indicate the onset of superluminescence with an increase in the excitation power. It has been found that an increase in the optical pumping intensity leads to a decrease in the luminescence decay time of the Lu₂O₃: Eu (7 at %) phosphor in the stimulated luminescence regime and to an increase in the quantum efficiency of red luminescence with a maximum at 611 nm.     

Theory of the evolution of 2D band in the Raman spectra of monolayer and bilayer graphene with laser excitation energy

A double‐resonance process gives rise to the 2D band in the Raman spectra of monolayer and bilayer graphene. Based on the electronic and vibrational dispersion energies of graphene, the wavenumbers of the 2D band were calculated under different laser excitation energies (from 1.0 to 4.4 eV). Calculated results are in good agreement with experimental data and reproduce the experimental dispersion slope of the 2D band very well. The calculated wavenumbers of the 2D band do not show a linear dependence on the laser excitation energies. Moreover, it is explained that the lowest wavenumber peak of the 2D band of the bilayer graphene, which is composed of four components, has the largest slope with laser excitation energy. Copyright © 2009 John Wiley & Sons, Ltd.     

Semirigid vibrating rotor target calculation for reaction O(<Superscript>3</Superscript>P)+CH<Subscript>4</Subscript>→CH<Subscript>3</Subscript>+OH

The time-dependent quantum dynamics calculation for reaction O(³P)+CH₄ →CH₃+OH is made, using of the semirigid vibrating rotor target (SVRT) model and the time-dependent wave packet (TDWP) method. The corresponding reaction probabilities of different initial states are provided. From the calculation of initial rovibrational statej=0,v=0, 1, we can see that the excitation of the H-CH₃ stretching vibration gives significant enhancement of reaction probability and the reaction threshold decreases dramatically with the enhancement of the vibrating excitation, which indicates that the vibrating energy of reagent molecules contributes a lot to the molecular collision. As for the calculation of reaction probability of statev=0,j=0,1,2,3, the results show that the reaction probability rises significantly with the enhancement of rotational quantum numberj while the reaction threshold has no changes. The spatial steric effect of the title reaction is studied and analyzed too after the calculation of reaction probability of statesj=5,k=0–2,n=0 andj=5,k=2,n=0–2 is made.