KrF激光泵浦H2受激拉曼放大

利用KrF激光泵浦高压H_2,在同轴前向的受激拉曼散射(SRS)作用下,产生受激拉曼放大,1阶Stokes光对泵浦光的转换效率为17.2％,并对影响放大过程和转换效率的若干因素作了分析。     

利用飞秒受激拉曼光谱技术研究Pyranine分子激发态质子传递过程

本文利用共振增强的飞秒受激拉曼光谱技术结合瞬态吸收光谱技术研究了光致产酸剂Pyranine发色团分子在水溶液中与醋酸根离子之间的光致激发态质子传递过程.实验中观测到了Pyranine发色团在400—1700 cm^–1频率范围内去质子化状态下的激发态拉曼振动光谱.同时在920 cm^–1处也观测到了质子化醋酸根离子中激发态碳-碳单键伸缩拉曼振动信号.通过对激发态质子传递中给体和受体的动力学的分析得到了在该条件下的激发态质子传递的速率.     

泵浦光束质量对受激拉曼散射的影响

主要讨论泵浦光束质量对低气压拉曼种子源特性的影响。文中给出了一阶斯托克斯光泵浦阈值、输出能量和光束质量的实验数据。用Ｍ＾２因子分析了泵浦光和一阶斯托克斯光的光束质量。根据考虑泵浦聚焦和泵浦光束质量影响的近似拉曼散射理论计算了泵浦阈值的理论曲线，并与实验数据和有关文献进行了比较。     

碘激光的H2振动受激拉曼阈值研究

首次实现了脉冲光解碘激光作为基频光的氢气振动受激拉曼变频,对碘激光的波长转换有着重要意义。在碘激光单脉冲能量100~130 mJ(脉宽100 ns)的条件下, 采用双次聚焦技术降低了高压氢气的振动受激拉曼变频的阈值,获得了波长为2900 nm中红外激光,光子转化效率最高达到8.7%。实验发现当拉曼介质氢气气压大于1 MPa后,一级斯托克斯光的拉曼转化效率不再随气压变化,并对这一现象进行了理论分析和归属。     

用U(4)群研究氘代乙炔分子的振动激发态能谱

氘代乙炔分子的动力学对称群是三个U(4)群的直积群,找到一个适当群链,其中各子群的卡塞米尔算子组成分子的哈密顿,组合系数由该分子的实验光谱数据确定.利用这个代数哈密顿计算的能谱与实验值相符.实验上尚未观测的光谱也可以计算出来.     

用U（4）群研究氘代乙炔分子的振动激发态能谱

氘代乙炔分子的动力学对称群是三个U(4)群的直积群，找到一个适当群链，其中各子群的卡塞米尔算子组成分子的哈密顿，组合系数由该分子的实验光谱数据确定。利用这个代数哈密顿计算的能谱与实验值相符。实验上尚未观测的光谱也可以计算出来。     

YVO4晶体的高效受激拉曼散射

报道了YVO4晶体在532 nm、30 ps脉冲下的的高效受激拉曼散射。采用腔外单次通过方式测量了不同长度YVO4晶体1阶斯托克斯受激拉曼散射的阈值,并得到该晶体的稳态增益系数为16.0±0.5 cm/GW。实验中观察到2阶斯托克斯线(558.6 nm5、87.8 nm)和1阶反斯托克斯线(508.0 nm),受激拉曼散射的整体转换效率高于50%。     

非线性拉曼激光雷达系统检测CO2气体的受激拉曼过程

 利用气体的受激拉曼散射增益效应的非线性雷达技术是探测大气中的CO₂气体的重要方法，用Nd:YAG固体激光器（1 064 nm）的三倍频光（354.7 nm）注入装有CO₂和N₂高压气体的拉曼管中，气体的受激拉曼散射（SRS）过程产生两种气体的一阶斯托克斯光，用来作为拉曼雷达的发射种子光源。介绍了产生光源的实验装置，论述了SRS中气体气压变化与一阶斯托克斯光能量输出变化的定量关系，得到最佳能量输出的优化条件，并对SRS中一阶斯托克斯光产生过程的物理机制进行了讨论。并根据光源的试验结果，设计了非线性受激拉曼雷达系统，对前期的普通拉曼雷达进行了实验，得到了初步的实验结果。     

H_2、D_2及H_2/D_2混合气体受激拉曼特性研究

受激拉曼散射是扩展激光波长的重要方法,但是气体中非线性光学过程对受激拉曼光的影响非常复杂,实验研究受激拉曼光与气体气压及拉曼池耦合透镜焦距的关系是实际应用受激拉曼光的重要手段。设计了受激拉曼实验装置及其测量系统,采用Nd:YAG激光器的四倍频激光266 nm作为抽运源,活性气体(H2、D2及H2/D2混合气体)分别被密封在长为100 cm的拉曼管中,输出的拉曼激光由棱镜分光后用能量计采集保存用以研究拉曼散射特性。给出了H2、D2及H2/D2混合气体的各级Stokes和反Stokes受激拉曼激光能量与气体气压及透镜焦距的关系。获得了217.84~447.15 nm之间的12条激光谱线,有效地扩展了拉曼激光的应用范围。研究结果对气体受激拉曼光的实际应用具有十分重要的价值。     

皮秒激光抽运高压H2的受激拉曼散射研究

利用NdYAG锁模序列脉冲激光(1064nm)抽运充有高压H2的拉曼池,输出光束经棱镜分光后投射在屏上,在可见光及近紫外光区用彩色胶卷摄得15个受激拉曼散射光斑;经1m光栅摄谱仪摄谱,在365-605nm波长范围内得到65条受激拉曼谱线.通过实验结果与理论计算值的比较,证明除了H2的振动拉曼频移量4154.6cm-1外,还有多个振动及转动拉曼频移量共同参与作用,从而产生了从紫外到红外众多波长的受激拉曼散射光.     

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.     

交叉分子束实验研究F+D2(v=1, j=0)反应

本文使用交叉分子束方法研究了氟原子和振动激发态氘分子D₂(v=1, j=0)的反应. 使用受激拉曼抽运的方法制备了振动激发的D₂分子. 实验中未观测到来自于旋轨耦合激发态氟原子F^*(²P_1/2)与振动激发态D₂分子的贡献. 观测到来自于旋轨耦合基态氟原子F(²P_3/2)和振动激发态D₂的反应信号,相应的产物DF分子布居于v''=2,3,4,5振动态上. 与振动基态反应F+D₂(v=1,j=0)相比,振动激发态反应F+D₂(v=1,j=0)生成的DF产物转动分布更“热”. 获得了振动激发反应的四个碰撞能在0.32至2.62 kcal/mol范围内的微分反应截面. 在最低的碰撞能0.32 kcal/mol下,所有振动态的DF产物都以后向散射为主. 随着碰撞能的增加,DF产物的角分布逐渐从后向转移到侧向. 测量了DF(v''=5)产物的前向微分散射截面随碰撞能变化的曲线. 前向散射的DF(v''=5)信号出现于1.0 kcal/mol. 在2.62 kcal/mol碰撞能下DF(v''=5)主要为前向散射.     

Analysis of the CIA spectra of the first overtone band of D2 in D2-N2

Enhancement spectra of the collision-induced absorption (CIA) in the first overtone region 5000-7000 cm⁻¹ of D₂ in D₂-N₂ were studied at 298 K for a base density of D₂ of 73 amagat and for partial densities of N₂ in the range 150-370 amagat. The observed spectra were modeled with a total of 1176 components of double vibrational transitions. Binary and ternary absorption coefficients were determined from the integrated absorption of the band. Profile analysis of the spectra was carried out using the Birnbaum-Cohen line-shape function for the individual components of the band, and characteristic line-shape parameters were determined from the analysis. Good agreement was obtained between the experimental and calculated spectral profiles.     

The Raman spectra and cross-sections of the ν2 band of H2O, D2O, and HDO

We report the experimental Raman spectra of the ν₂ band of H₂O, D₂O, and HDO in the vapor phase at room temperature. A complete interpretation of the Raman intensities is carried out employing the variational rovibrational wavefunctions obtained from a Hamiltonian in Radau coordinates and an ab initio polarizability surface at 514.5 nm. We show the importance of the rotation-vibration coupling to obtain the correct line intensities. Several tables with the assignments of the individual rotational-vibrational transitions and their Raman scattering strengths are reported. From these tables, the ν₂ Raman spectra can be simulated up to 2000 K for H₂O, and up to 300 K for D₂O and HDO.     

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.     

Collision-induced first overtone band of D2 in binary mixtures D2-X where X is Ar, Kr, and Xe

Enhancement spectra of the collision-induced absorption in the first overtone region 5500-6750 cm⁻¹ of D₂ in the D₂-Ar, D₂-Kr, and D₂-Xe binary mixtures were studied at 298 K for base densities of D₂ in the range 55-251 amagat and for partial densities of Ar, Kr, and Xe in the range 46-384 amagat. The observed spectra consist of the following quadrupolar transitions: O₂(3), O₂(2), Q₂ (J), J = 1-5 and S₂ (J), J = 0-5 of D₂. Binary and ternary absorption coefficients were determined from the integrated absorption coefficients of the band. Profile analyses of the spectra were carried out using the Birnbaum-Cohen (BC) lineshape function and characteristic lineshape parameters were determined from the analyses.     

Atomic-potential parameters for H2 and D2: quantum corrections in the calculation of second-virial coefficients

First-order quantum corrections were introduced into the computation of the second-virial coefficients of H₂ and D₂. The quantum effects, for the studied two light molecules, are considerable even at the room temperature and become prominent at low temperatures. Atomic potentials, incorporating the quadrupole interactions, were employed in the calculations. Optimum atomic-potential parameters ε_H, σ_H, ε_D and σ_D were obtained from the nonlinear least-squares fit of the experimental second-virial coefficients. The fitted virial coefficients cover the temperature ranges of 173-423 and 153- for H₂ and D₂, respectively.     

The rotational Raman spectra and cross sections of H2O, D2O, and HDO

We report the experimental rotational Raman spectra of H₂O, and of a mixture of D₂O and HDO in the vapor phase at room temperature, and their interpretation in terms of rotational–vibrational energies, wavefunctions, and transition moments of the molecular polarizability. These transition moments are based on high-level ab initio calculations of the wavelength dependent polarizability surface, and on wavefunctions where the rotational–vibrational coupling is considered in detail. As a byproduct of this analysis several tables have been compiled including scattering strengths and assignments for individual rotational transitions of the three species. From these tables the rotational Raman spectra can be simulated over the range of temperatures up to 2000 K for H₂O, and up to 300 K for D₂O and HDO.     

The Raman spectra and cross-sections of H2O, D2O, and HDO in the OH/OD stretching regions

We report the OH and OD stretching regions of the vapor phase Raman spectra of H₂O, and of a D₂O/HDO mixture, at room temperature. Also, the corresponding spectrum of H₂O at ∼2000 K in a methane/air flame is reported. These spectra are interpreted in terms of transition moments of the molecular polarizability, based on high-level ab initio calculations of the polarizability surface, and on variational wavefunctions considering the rotational-vibrational coupling in full. As a byproduct of this analysis several tables have been compiled including scattering strengths and assignments for individual rotational transitions of the three species. From these tables the Raman spectra in the OH/OD stretching regions can be simulated over the range of temperatures up to 2000 K for H₂O, and up to 300 K for D₂O and HDO.     

Stimulated emission from trapped excitons in SnO2 nanowires

The pump fluence dependent photoluminescence (PL) spectra of SnO₂ nanowires were investigated, which were synthesized with a high-temperature chemical reduction method. The integrated intensity of the narrower peak at 3.2 eV experiences a strong superlinear dependence on the pump fluence, and the narrowest width of the sharp peak is only 19 meV. Moreover, under high excitation fluence, an ultrafast decay time (less than 20 ps) appears in the time-resolved PL spectra. The emission of these SnO₂ nanowires shows strong apparent stimulated emission behaviors although the SnO₂ is a dipole forbidden direct gap semiconductor. The stimulated emission should relate to the localized islands on the surface of nanowire, which was observed through the high resolution transmission electron microscopy (HRTEM) image. The giant-oscillator-strength effect of bound exciton generated from the localized islands was considered to induce the stimulated emission of SnO₂ nanowires.