期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 21, 期 19, 页码 10038-10051出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cp00649d
关键词
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资金
- ERC Advanced Grant within the Seventh Framework Program of the European Union [290853 - XCHEM]
- MINECO [FIS2016-77889-R]
- 'Severo Ochoa' Programme for Centres of Excellence in RD (MINECO) [SEV-2016-0686]
- Maria de Maeztu'' Programme for Units of Excellence in RD [MDM-2014-0377]
- DFG [HA 8252/2-1]
Time-resolving and controlling coupled electronic and nuclear dynamics at conical intersections on the sub-femtosecond to few-femtosecond time scale is among the challenging goals of attosecond physics. Here we present numerical simulations of time-resolved photoelectron spectroscopy of such dynamics in NO2, where the coupled electron-nuclear motion at the (2)A(1)/B-2(2) conical intersection is steered on the sub-laser-cycle time scale by a nearly single-cycle, waveform controlled mid-infrared laser pulse. For a rigorous description of the photoionization dynamics, we employ ab initio energy-and geometryresolved photoionization matrix elements obtained with the multichannel R-matrix method, using a multiconfigurational description of the molecule and a newly developed algorithm to generate photoionization dipoles that are phase consistent on the level of both the neutral and the ionic states. We find that for sufficient molecular alignment, the time- and energy-resolved anisotropy parameters of the photoelectron angular distributions provide a particularly clear picture of both the ultrafast natural molecular dynamics at the conical intersection and its modifications by the control pulse. In particular, changes in the electronic and nuclear configurations induced by the control pulse lead to the appearance of non-vanishing odd anisotropy parameters in the photoelectron spectra. These are absent in the spectra obtained without the control pulse and therefore provide sensitive, background-free diagnostic of the control.
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