分子对飞秒激光场响应的含时密度泛函理论研究

采用含时密度泛函理论方法研究线性分子碳化锂(Li2C2)对飞秒激光场响应的电子-离子动力学行为.在典型的近共振和非共振的激光频率作用下,分别对比分析了分子的共振和非共振电离过程.研究发现:分子在共振频率激光场的作用下发生更强的电离过程,并倾向于发生库伦爆炸,键长的振荡断裂与电离相互促进影响,而分子在较弱的激光场作用下发生单光子电离过程;随着双脉冲时间间隔的增加,离化电子数在一定范围内呈振荡上升趋势,随后趋于常数.     

分子结构对非顺序双电离微观动力学的影响

本刊讯强场非顺序双电离包含了丰富的物理过程,最重要的是为研究电子关联效应提供了一个简单清晰的模型,因而成为当前强场物理领域研究的热点。在分子与强场的相互作用过程中,电离和解离会同时发生。实验和理论研究表明核间距的变化会对分子电离产生重要影响。     

分子对飞秒激光场响应的含时密度泛函理论研究

采用含时密度泛函理论方法研究线性分子碳化锂（Li2C2）对飞秒激光场响应的电子-离子动力学行为。在典型的近共振和非共振的激光频率作用下,分别对比分析了分子的共振和非共振电离过程。研究发现：分子在共振频率激光场的作用下发生更强的电离过程,并倾向于发生库伦爆炸,键长的振荡断裂与电离相互促进影响,而分子在较弱的激光场作用下发生单光子电离过程;随着双脉冲时间间隔的增加,离化电子数在一定范围内呈振荡上升趋势,随后趋于常数。     

分子核间距对非时序双电离的影响

利用半经典再散射模型研究了激光强度在一定范围内时分子核间距对非时序双电离过程的影响.分别计算了非时序双电离率、两电子的电离能、两电子的动量相关、Coulomb和激光场的复合势随分子核间距的变化关系.研究表明,分子核间距在1.0—6.0 a.u.范围内时,非时序双电离率和两电子动量和为零的双电离事件数随着分子核间距的增大而增大.当分子核间距继续增大(大于6.0 a.u.)时,非时序双电离率和两电子动量和为零的双电离事件数却减小.     

双波长圆偏振光场中分子电离动力学的研究新进展

超短激光脉冲的出现为人们研究原子分子内电子的超快动力学过程提供了重要的技术手段。强激光诱导原子分子的光电离过程是光诱导物理过程的基石,也是目前强场物理领域的前沿热点之一。本文重点综述了双波长圆偏振光场中分子电离动力学的研究进展。首先,介绍了研究强场分子电离动力学的半经典模型,给出了电离电子波包的相位和振幅分布。然后,介绍了利用双波长圆偏振光场测量H2分子和CO分子的电离动力学的研究,发现电离电子的振幅结构以及隧穿后电子受到的长程库仑势都会影响电子的动力学过程。此外,电子波包的相位结构也会包含在光电子的发射角中,这个初始相位编码了电子吸收光子而电离过程中的时域信息。最后,对新型阿秒钟在分子光电离过程中的应用进行了总结,并展望了未来复杂分子体系的应用前景。     

分子双电离对激光偏振性的依赖关系

利用经典系综模型研究了氢分子双电离对激光场椭圆率的依赖性.研究发现,氢分子双电离机制对激光的椭偏性有强烈的依赖关系.随着激光场椭圆率的增加,双电离机制由非次序双电离转变为次序双电离.在大椭圆率情况的次序双电离中,电子关联动量分布随椭圆率的灵敏变化显示了电子出射时间对椭圆率的强烈依赖关系.     

低于再碰撞阈值下强激光场原子非序列双电离

在最近的实验和理论研究中,我们探讨了氩原子和氖原子在红外强激光场中低于再碰撞阈值的非序列双电离问题。在研究中,我们发现在非序列双电离过程中,氖原子的电子关联表现为在激光偏振面内肩并肩出射,而对于氩原子的电子关联行为表现为在激光偏振面内的背对背出射,我们采用三维半经典模型（考虑电子隧道电离）很好地解释了实验结果。在阈值附近,我们发现电子在激光场中的多次散射以及电子再碰撞激发后电子隧道电离是氩原子反关联行为的主要原因,而电子在激光场作用下的单次碰撞是电子关联行为的主要原因。通过测量双电离过程中产生电子的横向电子动量分布,观察到了库伦聚焦效应,我们认为这是非经典的关联行为。最后,我们给出了氩原子和氖原子在激光场中阈值的解析模型,并给出了原子的关联和反关联激光强度区域.     

组态相互作用和相对论修正对类He离子双电子谱的影响

研究了组态相互作用和相对论修正对低Z(原子序数)及中等Z类He离子双电子谱的影响,使用准相对论及非相对论的Hartree-Fock自洽场方法计算了描写双电子伴线的原子参数。计算结果表明,(1)组态相互作用对类He离子双电子诺有显著影响;(2)对中等Z的类He离子,仅以能量微扰的形式计入相对论修正是不足够的,为了获得更加精确的计算结果,不仅要考虑相对论修正对单、双激发态能量的影响,而且要考虑该效应对径向波函数的影响。     

双原子分子多光子电离强场效应的含时波包动力学研究

强激光非线性条件下分子的多光子电离过程呈现出较为明显的强场效应.由于这种效应不能用传统的量子微扰论来处理,“缀饰态”模型方法提供了物理图象清晰的处理光与物质相互作用的方案.本文基于含时波包动力学的基本理论,将激光场看作经典场,利用“缀饰态”模型研究了强场下双原子分子(NO、RbI等)的多光子电离过程.研究表明,激光场的强度、泵浦-探测脉冲延迟时间等对多光子电离光电子能谱的形状有着重要的影响,而这种影响是由光诱导势引起的.另外,在研究具有两个连续态的RbI体系时,自电离现象的发生也与势能面的交叉密切相关,并受外场强度的影响.本文计算模拟外场中分子的光电子能谱时所得到的强场效应对理解和实现原子分子过程的激光操控具有重要的意义.     

双原子分子多光子电离强场效应的含时波包动力学研究

强激光非线性条件下分子的多光子电离过程呈现出较为明显的强场效应.由于这种效应不能用传统的量子微扰论来处理,"缀饰态"模型方法提供了物理图象清晰的处理光与物质相互作用的方案.本文基于含时波包动力学的基本理论,将激光场看作经典场,利用"缀饰态"模型研究了强场下双原子分子(NO、RbI等)的多光子电离过程.研究表明,激光场的强度、泵浦-探测脉冲延迟时间等对多光子电离光电子能谱的形状有着重要的影响,而这种影响是由光诱导势引起的.另外,在研究具有两个连续态的RbI体系时,自电离现象的发生也与势能面的交叉密切相关,并受外场强度的影响.本文计算模拟外场中分子的光电子能谱时所得到的强场效应对理解和实现原子分子过程的激光操控具有重要的意义.     

异核双原子和三原子分子在红外强激光场中的电离抑制

Ionization is the fundamental process in interaction of atoms/molecules with femtosecond strong laser fields. Comparing to atoms, molecules exhibit peculiar behaviors in strong-field ionization because of their diverse geometric structures, molecular electronic orbitals as well as extra nuclear degrees of freedom. In this study, we investigate strong field single and double ionization of carbon monoxide (CO) and carbon dioxide (CO₂) in linearly polarized 50-fs, 800-nm laser fields with peak intensity in the range of 2×10¹³ W/cm² to 2×10¹⁴ W/cm² using time-of-flight mass spectrometer. By comparing the ionization yields with that of the companion atom krypton (Kr), which has similar ionization potential to the molecules, we investigate the effect of molecular electronic orbitals on the strong-field ionization. The results show that comparing to Kr, no significant suppression is observed in single ionization of both molecules and in non-sequential double ionization (NSDI) of CO, while the NSDI probability of CO₂ is strongly suppressed. Based on our results and previous studies on homonuclear diatomic molecules (N₂ and O₂), the mechanism of different suppression effect is discussed. It is indicated that the different structure of the highest occupied molecular orbitals of CO and CO₂ leads to distinct behaviors in two-center interference by the electronic wave-packet and angular distributions of the ionized electrons, resulting in different suppression effect in strong-field ionization.     

Two-photon double ionization of helium by chirped few-cycle attosecond pulses:From nonsequential to sequential regime

The two-photon double ionization(TPDI) dynamics of helium by chirped attosecond pulses are theoretically studied by solving the two-electron time-dependent Schr o¨dinger equation in its full dimensions. We show that both the differential and the total double ionization probability can be significantly controlled by adjusting the chirp. The dependence of the TPDI on the chirp can be quite different for different photon energies, relying on the central photon energy being in the sequential region, nonsequential region, or translation region. The physics which lead to the chirp dependence for different photon energies are addressed. Present findings are well reproduced by a model based on the second-order time-dependent perturbation theory.     

Bohmian trajectory perspective on strong field atomic processes

The interaction of an atom with an intense laser field provides an important approach to explore the ultrafast electron dynamics and extract the information of the atomic and molecular structures with unprecedented attosecond temporal and angstrom spatial resolution. To well understand the strong field atomic processes, numerous theoretical methods have been developed, including solving the time-dependent Schr ?dinger equation(TDSE), classical and semiclassical trajectory method, quantum S-matrix theory within the strong-field approximation, etc. Recently, an alternative and complementary quantum approach, called Bohmian trajectory theory, has been successfully used in the strong-field atomic physics and an exciting progress has been achieved in the study of strong-field phenomena. In this paper, we provide an overview of the Bohmian trajectory method and its perspective on two strong field atomic processes, i.e., atomic and molecular ionization and high-order harmonic generation, respectively.     

Two-electron atoms in strong fields

Multiphoton excitation and ionization of two-electron atoms under strong laser pulses, with emphasis on double excitation, is reviewed. After an introduction to the basic concepts of traditional single-photon spectroscopy and methodology, the main phenomena and experimental observations under multiphoton excitation in the perturbative regime are summarized. That is followed by the discussion of the main ideas underlying various non-perturbative approaches, especially as they pertain to the two-electron problem. The present state of understanding non-perturbative time-dependent behavior, in that context and in relation to issues such as correlation, double excitation, sequential and direct double ionization, is then formulated and discussed. The article ends with a summary of effects relating to autoionizing states in strong fields and an outlook for future developments.     

Taking snapshots of a moving electron wave packet in molecules using photoelectron holography in strong-field tunneling ionization

Coherent superposition of electronic states induces attosecond electron motion in molecules. We theoretically investigate the strong-field ionization of this superposition state by numerically solving the time-dependent Schrödinger equation. In the obtained photoelectron momentum distribution, an intriguing bifurcation structure appears in the strong-field holographic interference pattern. We demonstrate that this bifurcation structure directly provides complete information about the status of the transient wave function of the superposition state:the horizontal location of the bifurcation in the momentum distribution reveals the relative phase of the involved components of the superposition state and the vertical position indicates the relative coefficient. Thus, this bifurcation structure takes a snapshot of the transient electron wave packet of the superposition state and provides an intuitive way to monitor electron motion in molecules.     

H$lt;sub$gt;2$lt;/sub$gt;$lt;sup$gt;+$lt;/sup$gt;在强激光场中的解离及其量子调控的理论研究

利用非波恩-奥本海默近似的三维含时量子波包法,理论研究了氢分子离子在强激光场中的解离动力学.通过分析H₂⁺在不同的初始振动态（ν=0–9）和激光场强度下的解离核动能谱,得到了H₂⁺的光解离机理及其随激光场的变化规律.研究结果表明：当激光场的强度I₁=5.0×10¹³ W/cm²时,分子的解离来源于高振动态ν=5–9,其解离机理主要是通过键软化、键硬化和阈下解离过程.当激光场的强度I₂=1.0×10¹⁴ W/cm² 时,H₂⁺在低振动态ν=3–4上的阈上解离起主导作用,而高振动态的键软化、键硬化和阈下解离所占的比重明显地下降了.研究结果为后续的量子调控的实验研究提供了科学的理论预测和指导. 关键词： 光解离 氢分子离子 含时波包法 核动能谱     

低于再碰撞阈值下强激光场原子非序列双电离(英文)

在最近的实验和理论研究中,我们探讨了氩原子和氖原子在红外强激光场中低于再碰撞阈值的非序列双电离问题。在研究中,我们发现在非序列双电离过程中,氖原子的电子关联表现为在激光偏振面内肩并肩出射,而对于氩原子的电子关联行为表现为在激光偏振面内的背对背出射,我们采用三维半经典模型(考虑电子隧道电离)很好地解释了实验结果。在阈值附近,我们发现电子在激光场中的多次散射以及电子再碰撞激发后电子隧道电离是氩原子反关联行为的主要原因,而电子在激光场作用下的单次碰撞是电子关联行为的主要原因。通过测量双电离过程中产生电子的横向电子动量分布,观察到了库伦聚焦效应,我们认为这是非经典的关联行为。最后,我们给出了氩原子和氖原子在激光场中阈值的解析模型,并给出了原子的关联和反关联激光强度区域。     

Double ionization of helium studied with the multi-configuration time-dependent Hartree–Fock method

The intensity dependence of double ionization probability of helium in a strong laser field is investigated by using the multi-configuration time-dependent Hartree–Fock (MCTDHF) method. The results agree with the previous theoretical report by directly solving the time-dependent Schrödinger equation. The time evolution of electronic population on the ground state, electronic energy and dipole moment are also presented and discussed.