NaLi分子飞秒含时光电子能谱的理论研究

运用三态模型和含时波包方法,研究了NaLi分子处于强飞秒抽运-探测激光场中的波包动力学过程和时间分辨光电子能谱,并且揭示了飞秒激光脉冲参数与NaLi分子光电子能谱之间的关系.研究发现:对于不同的激光波长,波包的振动周期是不同的,而且随着抽运-探测脉冲延迟时间的不同,NaLi分子光电子能谱的谱峰高度和位置发生变化;当λ1=352 nm并且?t=400 fs时,外阱中相应的光电离信号(0.5 eV处)明显强于内阱中相应的光电离信号(1.35 eV处).计算结果表明,NaLi分子激发态41Σ+上波包动力学的一些信息能够通过其光电子能谱反映出来.这些结果可以为实验上实现分子的光控制以及量子操控过程提供一些有价值的参考信息,并为进一步的理论研究提供重要依据.     

钴、钛原子激发态光电离研究

本文报道紫外区钛和钴原子共振增强多光子电离(REMPI)谱和激发态绝对光电离截面。实验上通过激光烧蚀金属样品制备中性原子,由飞行时间质谱仪检测离子产物,在298-351nm范围扫描激光波长,得到钛原子和钴原子共振增强多光子电离谱;并根据共振离子信号强度与电离激光通量关系得到原子激发态的绝对光电离截面,这些激发态电离截面的实验值在0.5-4 Mb。     

钴、钛原子激发态光电离研究

本文报道紫外区钛和钴原子共振增强多光子电离(REMPI)谱和激发态绝对光电离截面。实验上通过激光烧蚀金属样品制备中性原子,由飞行时间质谱仪检测离子产物,在298-351nm范围扫描激光波长,得到钛原子和钴原子共振增强多光子电离谱;并根据共振离子信号强度与电离激光通量关系得到原子激发态的绝对光电离截面,这些激发态电离截面的实验值在0.5-4 Mb。     

飞秒时间分辨质谱和光电子影像对分子激发态动力学的研究

分子量子态的研究,特别是分子激发态演化过程的研究不仅可以了解分子量子态的基本特性和量子态之间的相互作用,而且可以了解化学反应过程和反应通道间的相互作用.飞秒时间分辨质谱和光电子影像是将飞秒抽运-探测分别与飞行时间质谱和光电子影像相结合的超快谱学方法,为实现分子内部量子态探测,研究分子量子态相互作用及超快动力学过程提供了强有力的工具,可以在飞秒时间尺度下研究单分子反应过程中的光物理或光化学机理.本文详细介绍了飞秒时间分辨质谱和光电子影像的技术原理,并结合本课题组的工作,展示了这两种方法在量子态探测及相互作用研究领域,特别是激发态电子退相、波包演化、能量转移、分子光解动力学以及分子激发态结构动力学研究中的广泛应用.最后,对该技术的发展前景以及进一步的研究工作和方向进行了展望.     

铝原子激发态近阈限光电离截面测量

本文利用激光烧蚀、激光泵浦-探测、共振增强多光子电离和飞行时间质谱相结合的实验技术,根据离子产额和电离激光能量的关系,获取铝原子激发态的光电离截面;并研究了光电离截面与电离富余能的依赖关系.电离富余能0-2.98 e V内光电离截面值范围为15.6±1.7 Mb-2.3±0.9 Mb,激发态的寿命为17.6±1.8,16.9±1.7 ns.在光电离截面的测量中,总的均方根误差上限约为17%.     

水溶性TGA-CdTe量子点的超快弛豫动力学过程探究

本文以三个不同粒径(1^#:2.3 nm, 2^#:2.8 nm和3^#:3.5 nm)的巯基乙酸包覆的CdTe量子点(thioglycolic acid capped CdTe quantum dots, TGA-CdTe QDs)样品为研究对象, 其时间相关单光子计数(time-correlated single photon counting, TCSPC)实验得到的时间分辨光谱显示, 三个量子点的荧光平均寿命依次是～6 ns, ～10 ns和～12 ns, 其动力学过程包括慢过程和快过程两部分. 随其粒径尺寸的增加, 其慢过程延长, 快过程在变短. 然后, 通过瞬态吸收和荧光上转换两种基于飞秒的时间分辨光谱技术, 对TGA-CdTe量子点的带间弛豫过程做了探究. 实验结果显示, 三个TGA-CdTe量子点样品, 随其粒径增大, 最高激发态和最低激发态填充速率减慢, 其中, 最高激发态从0.33 ps增加至0.79 ps; 最低激发态从0.53 ps增至～1 ps. 另外, 由瞬态吸收和荧光上转换两种时间分辨手段相结合, 可得到CdTe量子点带间弛豫的完整图像, 结果显示了TGA-CdTe 量子点的一个本征特征:即在基态漂白恢复过程中的初始上升阶段, 荧光上转换信号要慢于瞬态吸收信号. 这可以为量子点在光电转换应用上提供帮助.     

Measurement of Photoionization Cross Sections of the Excited States of Titanium

实验研究了钛原子在293～321 nm波段的共振增强多光子电离. 采用激光烧蚀和超声射流相结合的实验技术来制备自由原子,由飞行时间质谱仪实现对钛原子光电离产物的检测. 从离子信号强度对和激光强度的依赖关系导出了钛原子价电子激发态的光电离截面. 实验测量的一些激发态光电离截面在0.2～6.0 Mb. 通过对⁴⁶Ti、⁴⁷Ti、⁴⁸Ti的光电离截面测量研究,没有发现明显的同位素依赖性.     

类锂离子C3+激发态(1s22p)2P光电离的计算

文中首次运用R-矩阵方法,在三态密耦近似下计算了类锂离子C3+激发态(1s22p)2P光电离截面,主要给出了不同过程和不同分波的光电离截面.计算结果显示了光电离过程中非常丰富的Rydberg系列共振结构.     

用光电离技术探测钐原子的奇宇称束缚激发态的光谱

采用光电离探测方法,对钐原子奇宇称束缚激发态进行了系统研究.通过设计三条不同的激发路径, 采用共振激发方式,先将钐原子分三步从基态激发到不同的束缚激发态,然后采用光电离手段对其进行探测. 通过对第三步激发光的波长进行大范围的扫描,在同一能域内获得了三组不同的光谱. 通过比对三条路径所得到的三组光谱,不仅精确确定了大量奇宇称束缚激发态的能级位置, 而且还获得了相应跃迁的相对强度的信息.最后,通过运用三条不同的激发路径的选择定则, 还确定了上述能级的总角动量. 关键词： 钐原子 束缚激发态 奇宇称 光电离探测     

铝原子激发态近阈限光电离截面测量

本文利用激光烧蚀、激光泵浦-探测、共振增强多光子电离和飞行时间质谱相结合的实验技术,根据离子产额和电离激光能量的关系,获取铝原子激发态的光电离截面;并研究了光电离截面与电离富余能的依赖关系.电离富余能0-2.98 eV内光电离截面值范围为15.6±1.7 Mb-2.3±0.9 Mb,激发态的寿命为17.6±1.8,16.9±1.7ns.在光电离截面的测量中,总的均方根误差上限约为17%.     

Ultrafast dissociation processes in the NO dimer studied with time-resolved photoelectron imaging

Ultraviolet photodissociation of the NO dimer is studied with femtosecond time-resolved photoelectron imaging (TR-PEI) spectroscopy. Pump pulses in the range 200–235 nm are employed, while probe pulses are kept at 300 nm. The time dependencies of the observed photoelectron kinetic energies and photoelectron angular distributions support a picture in which valence state optically excited in the dimer evolves on a time scale of <1 ps to the dimer 3s Rydberg state. This dimer Rydberg state then undergoes fragmentation on a time scale of a few ps. In this study we focus on dissociation into an NO ground state fragment and an NO fragment in its 3s Rydberg A²Σ⁺ state. Every stage of this continuous process, viz. the dimer valence state, the dimer 3s Rydberg state, the separating NO(X) + NO(A) fragments, and the isolated NO(A) fragment is interrogated with TR-PEI.     

The dynamics of a THz Rydberg wavepacket

An optically excited Rydberg wavepacket can be generated by exciting the electron from a low-lying state to a coherent superposition of high-lying states with a short broadband optical pulse. A special kind of Rydberg wavepacket is generated in the case of a interaction of a weak THz half cycle pulse with a stationary Rydberg state, called the THz wavepacket. This THz wavepacket is a coherent superposition of the initial Rydberg state and its neighbouring states. We have investigated the time evolution of THz wavepackets by measuring the impact of two in time delayed half cycle pulses ( ≈ 200 V cm^-1) on the population of a stationary (n = 40) Rydberg state in rubidium. The first half cycle pulse creates the THz wavepacket and the second half cycle pulse probes the dynamics of the THz wavepacket. We support our experimental data by numerically solving the Schr?dinger equation and with a semi-classical picture. Whereas an optically excited wavepacket is initially localized, a THz wavepacket is initially delocalized and becomes localized after half a revival time. Received 23 August 2000 and Received in final form 27 March 2001     

Theoretical study of the time-resolved photoelectron spectrum of Na 2F: effects of thermal initial conditions

The excited state dynamics of the Na₂F cluster initiated by a femtosecond laser pulse is studied considering a thermally excited initial sample. Within a pump-probe set-up, the time-dependent photoelectron spectrum is calculated, which is shown to be a sensitive tool to study intramolecular motion of the cluster. Temperature effects are taken into account through thermal averaging over the time-dependent spectra obtained from different initial vibrational states of the cluster. The nuclear motion upon laser excitation is described by full-dimensional quantum wavepacket propagation using explicit, realistic pump and probe pulses. The characteristic features of the time-resolved photoelectron spectra of the Na₂F cluster, identified as due to periodic bending motion of the cluster as well as to the excitation of the stretching mode, are found to be robust against increasing vibrational temperature of the cluster beam. This finding is important for possible future experiments.     

Femtosecond pump-probe experiments on non-stoichiometric sodium-fluoride clusters

In this paper we present two-color pump and probe spectroscopy on Na₂F, the smallest of the non-stoichiometric sodium-fluoride clusters (Na_nF_n-1), in molecular beams by employing femtosecond laser pulses. The molecules were pumped into the first excited state by one photonic transition and consecutively ionized from there by the second photon. We resolved the wavepacket oscillatory motion involving periodical structural rearrangements in the first excited state of Na₂F with a period of 185 fs. The time-resolved experiments show that sodium fluoride clusters provide interesting features which can be manipulated in optimal control experiments.     

Influence of radiation cross section uncertainties on shock wave structure

This numerical study investigates the sensitivity of non-equilibrium shockwave structure to uncertainties in (a) the ground and excited state continuum radiative cross section and (b) the bound-bound radiative cross section in a three level (ground, excited, and free electronic states considered) argon-like gas at Mach 18 and a pressure of 1 cm Hg. Changing the values of the radiative cross sections by an order of magnitude does not significantly influence the relaxation region; however, a large change occurs in not only the magnitude but also the extent of both the electron and excited state precursors. Increasing either the ground state continuum or the bound-bound cross section decreases the number of free electrons in front of the shock wave. These cross sections also influence the extent of the electron precursor through their influence on the ratio of the electrons produced by ground state photoionization to those produced by ground state photoexcitation followed by excited state photoionization. The bound-bound cross section also controls the excited state precursor, because the production of excited states is entirely due to line radiation. Increasing the excited state photoionization cross section increases both the magnitude and extent of the electron precursor, because the cross section influences the ratio of the two processes that compete to produce free electrons, and at the same time it influences the magnitude of the excited state precursor.     

Photoionization of the 4d state of the sodium atom in the field of a nanosecond pulse of a Nd:YAG laser

Results of experiments on photoionization of excited sodium atoms in the 4d state in the field of nanosecond pulses of a Nd:YAG laser are reported. The dependence of the photoionization signal for the given atomic state on the ionizing pulse energy was obtained. The experimental results are compared with the model calculations of the saturation curve for the photoionization signal.     

迭加态原子高次谐波发射的选频提高

本文研究了由体系的基态和较高激发态迭加形成的原子在强激光场作用下的高次谐波发射.观察电离波包的演化过程,阐明了谐波发射效率提高的原因.在给定入射激光条件下,通过选择不同的激发态,可以实现对谐波发射的控制.     

Ultrafast time-resolved coherent degenerate four-wave-mixing spectroscopy for investigating molecular dynamics in different states

In this paper, ultrafast time-resolved coherent degenerate four-wave-mixing (DFWM) spectroscopy is performed to investigate molecular dynamics in the gaseous phase. Laser pulses lasting for 40 fs are used to create and monitor different vibrational eigenstates of iodine at room temperature (corresponding to a low saturation pressure of about 35 Pa). Using an internal time delay in the DFWM process resonant with the transition between the ground X-state and the excited B-state, the vibrational states of both the electronically excited and the ground states are detected as oscillations in the DFWM transient signal. The dynamics of either the electronically excited or ground state of iodine molecules obtained are consistent with the previous high temperature studies on the femtosecond time-resolved DWFM spectroscopy.     

ATOMIC COHERENT POPULATION TRAPPING AND ITS APPLICATION IN A RAMAN-TYPE PHOTOIONIZATION SYSTEM WITH THREE BOUND STATES

We have studied the atomic coherent population trapping in a Raman-type, photoionization system with three bound states. The conditions for the system having two or one stable eigenstate are given. The influences of Fano asymmetric factors on the coberent population transfer are also analyzed.It is found that the property of the system having on]y one population trapping state consisting of the ground state, and one excited state, can be utilized to transfer the atomic initial population into one excited state.