Journal
FARADAY DISCUSSIONS
Volume 194, Issue -, Pages 369-405Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6fd00130k
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Funding
- Deutsche Forschungsgemeinschaft [Sm292/5-1, IV152/7-1]
- EU ITN MEDEA [AMD-641789-17]
- EPSRC/DSTL MURI grant [EP/N018680/1]
- European Cooperation in Science and Technology (COST) [CM1204 XLIC]
- Minerva Foundation
- Israeli Science Foundation
- European Research Council Starting Research Grant MIDAS
- Crown Photonics Center
- I-Core Center
- European Union [641272]
- EPSRC [EP/N018680/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/N018680/1] Funding Source: researchfish
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High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multidimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
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