B-X and C-X Band Systems of CuCl Revisited: Laser-induced Fluorescence Study in 465−490 nm

通过20400～21800 cm^-1的激光诱导荧光激发谱,重新研究了CuCl的B～X和C～X带系,洪特情形(a)的转动分析揭示出明显的单重态到单重态的跃迁特征. 测量的寿命(分别为4.670和4.667 μs)对于纯的单重态明显太长, 表明CuCl的B态和C态应该位于单重态(¹П和¹∑⁺)和三重态(³П_0,1,2)的混合区,光谱所观测到的这两个激发态可能是被临近三重态严重微扰的单重态.     

OCS在217 nm的光解动力学研究

The S(¹D₂)+CO(X¹Σ⁺) product channel from photodissociation of OCS at 217 nm has been measured using the DC slice velocity map imaging (VMI) technique in combination with resonance enhanced multiphoton ionization (REMPI). Two diflerent REMPI intermediate states (¹F₃ and ¹P₁) and several pump-probe laser polarization geometries are used to detect the angular momentum polarization of the photofragmented S(¹D₂). The molecular- frame polarization parameters, as well as the laboratory-frame anisotropy parameters, for individual rotational states of co-fragment CO, are determined using two diflerent full quantum theories. The measured total kinetic energy release spectrum from photodissociation of OCS indicates two dissociation channels, corresponding to the fast and slow recoiling velocities of S(¹D₂), respectively. The slow channel is concluded to originate from an initial photoexcitation to the A(¹A'') state, followed by a non-adiabatic transition to the ground state. The fast channel is found to follow a coherent excitation to A(¹A'') and B(¹A'') states, where contributions of the two states are almost equal at 217 nm. The determined alignment and anisotropy parameters further indicate that the slow channel follows an incoherent excitation, while the fast channel follows a coherent excitation to A(¹A'') and B(¹A'') states with a phase di erence of π/2.     

使用时间切片离子速度成像技术研究CF_2Cl_2光解动力学（英文）

本文使用时间切片离子速度成像技术结合共振增强多光子电离技术研究了CF_2Cl_2分子在235 nm附近的光解动力学.通过测量CF_2Cl_2分子在235 nm附近单光子解离产生的氯原子影像,直接得到了解离产物的速度分布和角分布.激发态氯原子的速度分布包含高动能组分和低动能组分,分别对应~3Q_0电子态的直接解离和由于内转换引起的基态预解离.基态氯原子的速度分布也包含高动能组分和低动能组分,分别对应~3Q_0与~1Q_1电子态的预解离和由于内转换引起的基态预解离.自由基解离通道被确认,二次解离通道和三体解离通道被排除.     

超声射流冷却S2自由基激光诱导荧光激发谱

在超声射流条件下.采用SF6/Ar(～10%)混合气束脉冲直流放电方法产生S2自由基,观测了32S2自由基在30000～35500 cm-1波段的激光诱导荧光激发谱.通过对所观测到的40多个振动谱带的归属,确定其中28个谱带为s2自由基B3∑μ一X3∑-g跃迁的(v'=1-9,0),(v'=1-8,1),(v'=1-7,2)和(v'=2-5,3)四个谱带序列.通过对所获谱带的转动分析,得到更为丰富的S2自由基B3∑-μ-X3∑-g跃迁谱带的转动光谱常数和更为精确的B3∑-μ电子态的平衡分子常数:Te,щe,щXe,Be,ae和Re.另外,还测得所有观测到的谱带的寿命,进一步丰富了S2自由基学∑-μ-X2∑-g跃迁谱带的光谱信息.     

Resonance-Enhanced Photon Excitation Spectroscopy of the Even-Parity Autoionizing Rydberg States of Xe

用脉冲直流放电产生Xe原子亚稳态5p56s[3/2]2和5p56s′[1/2]0.在单光子28000－42000cm-1能量范围内,结合飞行时间质谱技术获得Xe原子共振增强激发光谱.光谱分析表明,所有谱线来源于Xe原子5p56s[3/2]2和5p56s′[1/2]0两个亚稳态吸收单个光子向偶宇称np′、nf′自电离Rydberg态序列的跃迁.实验观测到许多新的自电离能级,并获得更精确和系统的能级位置和量子亏损值数据.     

光腔衰荡光谱研究PH2自由基在465-555nm的光谱

Absorption spectra of jet-cooled PH₂ radicals were recorded in the wavelength range of 465-555 nm using cavity ringdown spectroscopy. The PH₂ radicals were produced in a supersonic jet by pulsed direct current discharge of a mixture of PH₃ and SF₆ in argon. Seven vibronic bands with fine rotational structures have been observed and assigned as 0⁰₀、2ⁿ₀、2ⁿ₁(n=1-3) bands of the ?²A₁- Χ²B₁ electronic transition. Rotational assignments and rotational term values for each band were re-identified, and the molecular parameters including rotational constants, centrifugal distortion constants, and spin-rotation interaction constants were also improved with reasonably high precision. In addition, large perturbations observed in each quantum number of total angular momentum of the a axis level of the excited vibronic stateswere briefly discussed.     

荧光色散谱对FeS(X5△)振动常数的实验确认

Based on previous laser-induced fluorescence excitation spectroscopy work, the vibrational constants of neutral FeS in the X⁵△ electronic state were obtained by directly mapping the ground-state vibrational levels up to v″=3 using conventional laser-induced dispersed fluorescence spectroscopy. The vibrational frequency of FeS(X⁵△) (518±5 cm-1) agrees well with that reported in a recent PES measurement (520±30 cm-1) [J. Phys. Chem. A 107, 2821 (2003)] which is the only one prior experimental vibrational frequency value for the ⁵△ state of FeS. Careful comparisons of our experimental results and those documented in the literature (mainly from theoretical predictions) suggest that the ground state of FeS is ⁵△ state.     

CS分子在207 nm的光解动力学研究：S(1D2)+CO(X1Σ+)产物通道

利用直流时间切片离子成像技术对OCS分子在紫外波段207 nm的光解产物S(¹D₂)进行了偏振实验研究. 通过在两种不同的共振增强多光子电离中间态，¹F₃和¹P₁, 以及四种不同的泵浦-探测激光偏振几何构型下探测了光碎片S(¹D₂)的角动量极化特性. 使用分子坐标系极化模型和实验室坐标系各向异性模型提取和分析出对应产物CO(X¹Σ⁺)的角分布.观测到的总平动能释放谱表明解离过程存在三种解离通道，分别对应于低、中、高平动能解离通道. 低、中平动能通道的来源与光解波长在较长波长下得到的双峰分布来源一致. 高平动能通道是一种新的解离通道，它来自于单重排斥态A(2¹A'')的直接解离.     

钙钛矿晶体的电荷复合动力学研究

本文利用紫外吸收光谱和稳态荧光光谱技术结合理论模型，研究了钙钛矿材料CH₃NH₃PbI₃晶体在光激发过程中的电荷复合动力学行为，进而获得晶体的扩散长度. 电荷载体的扩散长度是判断光电材料的重要参数. 研究通过合成两种不同缺陷态浓度的CH₃NH₃PbI₃晶体，测量这两种晶体在0.019∽4.268 μJ/cm²的激光激发下的时间分辨荧光光谱，利用动力学模型对光谱进行拟合，可以获得每个晶体的掺杂浓度，空穴浓度以及电荷复合参数. 将这些参数结合已有公式，最终可获得每个晶体的电荷载体的扩散长度.     

硫化镍激光诱导荧光光谱：一个新的低激发态

采用激光诱导荧光技术在12200～13550 cm^-1能量范围内研究了超声射流冷却下的硫化镍光谱. 获得了4个具有转动结构的振转带,并被归属为基态至低激发态[12.4]³∑₀^- 的跃迁. 通过转动分析,确定了该低激发态的转动常数、同位素位移以及分子(平衡)常数. 此外,还测量了这些振转带的寿命.