期刊
CHEMICAL PHYSICS
卷 414, 期 -, 页码 184-191出版社
ELSEVIER
DOI: 10.1016/j.chemphys.2012.12.022
关键词
Attosecond spectroscopy; Molecular high-order harmonic generation; Intra-cation nuclear dynamics; Intra-cation electronic dynamics; Field coupling inducing intra-cation hole migration; High harmonics quantum path interferences; Short and long trajectories in high-harmonics; Ultrafast charge migration after ionisation
资金
- UK EPSRC [EP/J002348/1, EP/I0325174/1, EP/E028063/1]
- British Council Alliance [10026]
- [ERC-2011-ADG-20110209]
- [290467]
- EPSRC [EP/E028063/1, EP/J002348/1, EP/E036112/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/J002348/1, EP/E028063/1, EP/E036112/1] Funding Source: researchfish
We investigate how short and long electron trajectory contributions to high harmonic emission and their interferences give access to information about intra-molecular dynamics. In the case of unaligned molecules, we show experimental evidence that the long trajectory contribution is more dependent upon the molecular species than the short one, providing a high sensitivity to cation nuclear dynamics from 100's of as to a few fs after ionisation. Using theoretical approaches based on the strong field approximation and numerical integration of the time dependent Schrodinger equation, we examine how quantum path interferences encode electronic motion when the molecules are aligned. We show that the interferences are dependent upon which ionisation channels are involved and any superposition between them. In particular, quantum path interferences can encode signatures of electron dynamics if the laser field drives a coupling between the channels. Hence, molecular quantum path interferences are a promising method for attosecond spectroscopy, allowing the resolution of ultra-fast charge migration in molecules after ionisation in a self-referenced manner. (c) 2012 Elsevier B.V. All rights reserved.
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