期刊
SCIENCE
卷 350, 期 6262, 页码 790-795出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aab2160
关键词
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资金
- ERC [307270-ATTOSCOPE, 277767-TDMET]
- Swiss National Science Foundation via National Centre of Competence in Research Molecular Ultrafast Science and Technology
- Fonds National de la Recherche Scientifique of Belgium
- Fonds de la Recherche Fondamentale Collective [2.4545.12]
- Belgian American Education Foundation
- Wallonie-Bruxelles International
- Ministry of Education and Science of Russia [3.679.2014/K]
- VKR Centre of Excellence QUSCOPE
- Villum Fonden [00007335] Funding Source: researchfish
The ultrafast motion of electrons and holes after light-matter interaction is fundamental to a broad range of chemical and biophysical processes. We advanced high-harmonic, spectroscopy to resolve spatially and temporally the migration of an electron hole immediately after ionization of iodoacetylene while simultaneously demonstrating extensive control over the process. A multidimensional approach, based on the measurement and accurate theoretical description of both even and odd harmonic orders, enabled us to reconstruct both quantum amplitudes and phases of the electronic states with a resolution of 100 attoseconds. We separately reconstructed quasi field-free and laser-controlled charge migration as a function of the spatial orientation of the molecule and determined the shape of the hole created by ionization. Our technique opens the prospect of laser control over electronic primary processes.
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