Effects of aligning pulse duration on the degree and the slope of nitrogen field-free alignment

Through theoretical analysis,we show how aligning pulse durations affect the degree and the time-rate slope of nitrogen field-free alignment at a fixed pulse intensity.It is found that both the degree and the slope first increase,then saturate,and finally decrease with the increasing pump duration.The optimal durations for the maximum degree and the maximum slope of the alignment are found to be different.Additionally,they are found to mainly depend on the molecular rotational period,and are affected by the temperature and the aligning pump intensities.The mechanism of molecular alignment is also discussed.     

SF_6分子最高占据轨道对称性的判断

量化计算是理论研究分子的重要手段,对于具有高对称群的分子,采用子群计算是常用的方法.分子的电子态或分子轨道等的对称性在子群的表示中会出现重迭,从而不能从子群的结果直接给出电子态或分子轨道对称性的归属.本文以如何判断SF6基态1 A_(1g)的电子组态中最高占据轨道的对称性为例来解决这个问题.针对某些文献中的SF6基态1 A1g的电子组态中,最高占据轨道对称性是T_(1g)却写成T_(2g)的问题,采用Molpro量化计算软件,对SF6基态的平衡结构,进行了HF/6-311G*计算,得到了能量三重简并的最高占据轨道的函数表达式,进而运用O_h群的对称操作作用在三个轨道函数上,得到各操作的矩阵表示,于是得到特征标,最后确定了最高占据轨道为T_(1g)对称性.     

Angular distributions of CH3I fragment ions under the irradiation of a single pulse and trains of ultrashort laser pulses

The angular distribution of CH3I is investigated experimentally using a single Fourier transform-limited laser pulse and a pulse train, where a 90-fs 800-nm linearly polarized laser field with a moderate intensity of 2.8×1013 W/cm2 is used. The dynamic alignment is demonstrated in a single pulse experiment. Moreover, a pulse train is used to optimize the molecular alignment, and the alignment degree is almost identical to that with the single pulse. The results are analysed by using chirped femtosecond laser pulses, and it demonstrates that the structure of pulse train rather than its effective duration is crucial to the molecular alignment.     

Angular distributions of CH3I fragment ions under the irradiation of single pulse and trains of ultrashort laser pulses

The angular distribution of CH₃I is investigated experimentally using a single Fourier transform-limited laser pulse and a pulse train, where a 90-fs 800-nm linearly polarized laser field with a moderate intensity of 2.8×10¹³ W/cm² is used. The dynamic alignment is demonstrated in a single pulse experiment. Moreover, a pulse train is used to optimize the molecular alignment, and the alignment degree is almost identical to that with the single pulse. The results are analysed by using chirped femtosecond laser pulses, and it demonstrates that the structure of pulse train rather than its effective duration is crucial to the molecular alignment.     

Dynamics of molecular alignment steered by a few-cycle terahertz laser pulse

The field-free alignment of molecule ClCN is investigated by using a terahertz few-cycle pulse (THz FCP) based on the time-dependent density matrix theory. It is shown that a high degree of molecular alignment can be obtained by changing the matching number of the THz FCPs in the adiabatic regime and the non-adiabatic regime. The matching number can affect both the maximum value of the alignment and the time at which it is achieved. It is also found that a higher degree of alignment can be achieved by using the THz FCP at lower intensity and there exists an optimal threshold of molecular alignment with the increase of the field amplitude. Also found is the frequency sensitive region in which the degree of maximum alignment can be enhanced greatly by modulating the center frequencies of different THz FCPs. The investigation demonstrates that comparing with a THz single-cycle pulse, a better result of the field-free alignment can be created by a THz FCP at a constant rotational temperature of molecule.     

Low temperature enhancement of alignment-induced spectral broadening of femtosecond laser pulses

The propagation of femtosecond laser pulses in N2-filled hollow fibers is studied both theoretically and experimentally. The laser pulse aligns the N2 molecules and changes the refractive index, which meanwhile modulates the spectrum of the pulse in turn. The dependence of the spectral modulation on the gas temperature is investigated. We find that both spectral broadening and frequency red-shift are enhanced at low temperature. The degree of enhancement is found to be dependent on the pulse duration. Based on our findings, we propose a method for femtosecond pulse spectral broadening and few-cycle pulse generation via the molecular alignment.     

Quantum interference in laser-assisted photo-ionization excited by a femtosecond x-ray pulse

The photoelectron energy spectra （PESs） excited by monochromatic femtosecond x-ray pulses in the presence of a femtosecond laser are investigated. APES is composed of a set of separate peaks, showing interesting comb-like structures. These structures result from the quantum interferences between photoelectron wave packets generated at different times. The width and the localization of each peak as well as the number of peaks are determined by all the laser and x-ray parameters. Most of peak heights of the PES are higher than the classical predictions.     

S-matrix study on alignment dependence of single ionization of molecular ions with different active orbitals

The orientation-dependent single ionization rate of the diatomic molecular ion H_2^+ with different active orbitals in an intense field is studied by using S-matrix theory. Our results show that the orientation-dependent single ionization probability of H_2^+ is greatly dependent on the symmetry and the electron density distribution of its initial states, and it can be used to identify the excited state of the molecular ion in the dissociation process.     

液晶空间光调制器在飞秒脉冲色散补偿中的应用

关键词：     

Conformation effects on the molecular orbitals of serine

This paper calculates the five most stable conformers of serine with Hartree--Fock theory, density functional theory (B3LYP), Moller--Plesset perturbation theory (MP4(SDQ)) and electron propagation theory with the 6-311++G(2d,2p) basis set. The calculated vertical ionization energies for the valence molecular orbitals of each conformer are in agreement with the experimental data, indicating that a range of molecular conformations would coexist in an equilibrium sample. Information of the five outer valence molecular orbitals for each conformer is explored in coordinate and momentum spaces using dual space analysis to investigate the conformational processes, which are generated from the global minimum conformer Ser1 by rotation of C₂--C₃ (Ser4), C₁--C₂ (Ser5) and C₁--O₂ (Ser2 and Ser3). Orbitals 28a, 27a and 26a are identified as the fingerprint orbitals for all the conformational processes.     

控制双激光脉冲的宽度提高N2分子的取向

提出了通过控制双激光脉冲宽度的方法来提高N₂分子取向程度. 利用数值方法求解了N₂分子刚性转子模型在双激光脉冲作用下的薛定谔方程,计算了双原子分子N₂在总强度固定的两束激光脉冲作用下,不同脉冲宽度对于N₂分子取向的影响. 研究结果表明,通过调整两束激光脉冲的宽度,选择合适的延迟时间能够有效提高N₂分子的取向程度. 关键词： 双激光脉冲 分子取向 脉冲宽度     

The photoluminescence of ZnSe bulk single crystals excited by femtosecond pulse

This paper reports on the photoluminescence spectra of ZnSe single crystal with trace chlorine excited by the femtosecond laser pulse. Three emission bands, including second-harmonic-generation, two-photon-excited peak and a broad band at 500--700nm, were detected. The thermal strain induced by femtosecond pulse strongly influences the photoluminescence of ZnSe crystal. The corresponding strain \va in ZnSe crystal is estimated to be about 8.8 \ti10^-3 at room temperature. The zinc-vacancy, as the main point defect induced by femtosecond pulse, is successfully used to interpret the broad emission at 500--700nm. The research shows that self-activated luminescence possesses the recombination mechanism of donor--vacancy pair, and it is also influenced by a few selenium defects and the temperature. The rapid decrease in photoluminescence intensity of two-photon-excited fluorescence and second-harmonic generation emission at lower temperature is attributed to the fact that more point defects result in the thermal activation of the two-photo-absorption energy converting to the stronger recombination emission of chlorine--zinc vacancy in 500--700nm. The experimental results indicate that the femtosecond exciting photoluminescence shows a completely different emission mechanism to that of He--Cd exciting luminescence in ZnSe single crystal. The femtosecond laser exhibits a higher sensitive to the impurity in crystal materials, which can be recommended as an efficient way to estimate the trace impurity in high quality crystals.     

具有几个光振荡周期长度的飞秒激光脉冲在线性色散介质中的传输

给出了描写具有几个光振荡周期长度的飞秒激光脉冲在线性色散介质中传输方程的解。对脉冲的传输特性进行了数值摸拟 ,分别考察了来源于电子和晶格的正常和反常群速色散对脉冲展宽和脉冲形状畸变的影响。     

基于氧化镁晶体中级联四波混频过程的紫外飞秒光脉冲产生

紫外波段飞秒激光脉冲是研究超快化学和超快物理相关过程的重要工具,实现波长可调谐的宽带紫外飞秒光脉冲将有助于推动超快动力学及相关领域的研究.本文报道了以两束400 nm的飞秒光脉冲作为级联四波混频的抽运源,在氧化镁晶体中产生9阶频率上转换和5阶频率下转换边带信号的实验结果.边带波长范围从350 nm到450 nm连续可调谐,这些边带信号的发散角和波长与级联四波混频理论预测结果吻合.紫外边带相对于入射光的整体转化效率约为1.2%.同时,高阶边带的光谱形状呈现高斯型,其谱宽理论上支持傅里叶转换极限脉宽为20—50 fs.本文展示了一种高效产生波长可连续调谐的紫外飞秒光脉冲的便捷方法,为基于紫外超短脉冲的相关研究提供了有效工具.     

飞秒脉冲在光子晶体光纤中的传输特性

基于广义非线性薛定谔方程,利用分步傅里叶法数值模拟了超高斯时间分布的飞秒脉冲在光子晶体光纤中的传输特性。结果表明：超高斯脉冲比高斯脉冲在更短距离内形成孤子衰变,而且出现比强孤子功率稍低的次峰,孤子自频移更显著;另外,三阶色散会导致脉冲波形及频谱不对称,出现精细结构,并且有形成孤子的趋势;脉冲内拉曼散射对脉冲有平滑作用;自陡改变了主峰与次峰之间的能量分配。     

具有几个光振荡周期的飞秒激光脉冲

从麦克斯韦方程组出发 ,推导出了具有几个光振荡周期的飞秒激光脉冲在非线性光纤中传输的方程和非线性光纤的折射率。给出了描述具有几个光振荡周期的飞秒激光脉冲在非线性光纤中传输方程的解。研究了在非线性光纤中自相位调制导致具有几个光振荡周期的飞秒激光脉冲频谱展宽 (脉宽压缩 )的详细物理过程。研究了非线性光纤中飞秒光孤子产生的条件     

Three-dimensional simulation on explosions of hydrogen atomic clusters irradiated by an intense femtosecond laser pulse

Using classic particle dynamics simulations, the interaction process between an intense femtosecond laser pulse and icosahedral hydrogen atomic clusters H_{13}, H_{55} and H_{147} has been studied. It is revealed that with increasing number of atoms in the cluster, the kinetic energy of ions generated in the Coulomb explosion of the ionized hydrogen clusters increases. The expansion process of the clusters after laser irradiation has also been examined, showing that the expansion scale decreases with increasing cluster size.     

飞秒啁啾Gauss型脉冲在稠密Λ型三能级原子介质中的传播

利用由预估校正(PC)- 时域有限差分(FDTD)法求得的不含慢变包络近似(SVEA)和旋转波近似(RWA)的全波Maxwell-Bloch方程的数值解, 研究了飞秒啁啾Gauss型激光脉冲(以下简称啁啾脉冲)在稠密Λ型三能级原子介质中的传播.研究表明,啁啾系数(C)的正负及大小的变化对脉冲传播特性有显著的影响,而且这个影响与脉冲面积的大小密切相关.面积小于4π的啁啾脉冲,在介质中传播时不发生分裂,且啁啾脉冲逐渐演化为一个近似的无啁啾(C=0)脉冲,这一特点不随啁啾系数的改变而     

飞秒激光脉冲作用下氢原子径向和角向波包的产生与演化

采用劈裂-伪谱方法求解激光场中的含时薛定谔方程,探讨飞秒激光脉冲中氢原子波包的演化过程.研究了氢原子激发态的径向分布,角向分布、各态布居和电子云密度随时间的变化关系.在用共振激光脉冲控制氢原子波包演化的过程中径向分布、角向分布、各态布居和电子云密度随时间发生变化,但发现径向分布和角向分布在变化的过程中始终经过一些特殊点,并从理论上分析了存在这些特殊点的原因.     

Spectral modulation of third-harmonic generation by molecular alignment and preformed plasma

We demonstrate spectral modulation of third-harmonic generation from molecular alignment effects. The third harmonic spectrum is broadened or narrowed under different influences of cross-phase modulations originating from various molecular alignment revivals. Furthermore, the spectrum and spatial distribution of the generated third harmonic pulse change dramatically in the presence of a preformed plasma. Under the influence of a preformed plasma, a narrower third harmonic spectrum is observed, and the conical third-harmonic pulse increases while the axial part decreases. The investigation provides an effective method to modulate the spectral characteristic and spatial distribution of third-harmonic generation from intense femtosecond filament.