Correlated electronic and nuclear motion in molecules

分子中相关的电子和核运动

• 批准号: 233471155
• 负责人: Dr. Claus-Peter Schulz
• 金额: --
• 依托单位: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2018-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/233471155?language=en
• 关键词: Correlated; electronic; nuclear; motion; molecules

In this project we will investigate time-resolved electronic and nuclear dynamics in molecules. In particular, we want to study the coupling of electronic degrees of freedom and the coupling of electronic and nuclear degrees of freedom, in small diatomic to mid-size polyatomic molecules, and on timescales ranging from attoseconds to a few femtoseconds. In the initial phase of the project strong field ionization (SFI) will be utilized to probe the induced adiabatic and non-adiabatic multi-electron dynamics. To this end, we aim to measure the fragment ion and electron momentum in coincidence and with full angular resolution, thereby allowing us to study the breakdown of the single active electron (SAE) approximation in the molecular frame. In a later stage of the project two-colour XUV+IR pump-probe spectroscopy will be used to study purely electronic dynamics and coupled electronic and nuclear dynamics induced in molecules. Two different scenarios will be investigated. After SFI the breakdown of the SAE approximation leads to the production of a coherent superposition of electronic states in the molecular ion, and hence to electronic dynamics on the attosecond to few-femtosecond timescale, which may couple to nuclear dynamics as well. In this scenario we will use attosecond pulses to probe this coupled electronic and nuclear dynamics. In the second scenario we will study purely electronic dynamics and coupled electronic and nuclear dynamics induced in molecules by an ionizing attosecond pulse. The ensuing dynamics will be probed by the field of an IR pulse, which coherently couples different excited ionic states.These experiments will be enabled by bringing together three forefront technologies: (i) a high repetition rate (400 kHz) few-cycle laser based on Optical Parametric Chirped Pulse Amplification (OPCPA) technology, (ii) attosecond pulse generation by high harmonic generation in a tight-focussing geometry, and (iii) the use of a reaction microscope that allows simultaneous and coincident determination of the full 3D momentum vectors of several charged reaction fragments (electrons, ions), and thereby to follow in real time the evolution of the electronic and nuclear structure of the molecules.

在这个项目中，我们将研究分子中的时间分辨电子和核动力学。特别是，我们想要研究小型双原子到中型多原子分子中电子自由度的耦合以及电子和核自由度的耦合，时间尺度从阿秒到几飞秒。在该项目的初始阶段，将利用强场电离（SFI）来探测诱导绝热和非绝热多电子动力学。为此，我们的目标是同时以全角分辨率测量碎片离子和电子动量，从而使我们能够研究分子框架中单个活性电子（SAE）近似的分解。在该项目的后期阶段，双色 XUV+IR 泵浦探针光谱将用于研究纯电子动力学以及分子中诱导的电子和核耦合动力学。将研究两种不同的情况。 SFI 后，SAE 近似的崩溃导致分子离子中电子态的相干叠加的产生，从而导致阿秒到几飞秒时间尺度上的电子动力学，这也可能与核动力学耦合。在这种情况下，我们将使用阿秒脉冲来探测这种耦合的电子和核动力学。在第二种情况下，我们将研究纯电子动力学以及电离阿秒脉冲在分子中引起的耦合电子和核动力学。随后的动力学将通过红外脉冲场进行探测，该脉冲场相干地耦合不同的激发离子态。这些实验将通过汇集三种前沿技术来实现：(i) 基于光学参量啁啾脉冲放大 (OPCPA) 技术的高重复率 (400 kHz) 少周期激光器，(ii) 通过在紧聚焦中产生高谐波来产生阿秒脉冲 (iii) 使用反应显微镜，可以同时一致地确定多个带电反应片段（电子、离子）的完整 3D 动量矢量，从而实时跟踪分子电子和核结构的演变。

项目成果

Sequential and direct ionic excitation in the strong-field ionization of 1-butene molecules.

• DOI: 10.1039/c7cp08195b
• 发表时间: 2018-05
• 期刊: Physical chemistry chemical physics : PCCP
• 作者: F. Schell;A. Boguslavskiy;C. Schulz;S. Patchkovskii;M. Vrakking;A. Stolow;J. Mikosch