Multidimensional high harmonic spectroscopy of polyatomic molecules: Detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields

Barry D. Bruner, Zdeněk Mašín, Matteo Negro, Felipe Morales, Danilo Brambila, Michele Devetta, Davide Faccialà, Alex G. Harvey, Misha Ivanov, Yann Mairesse, Serguei Patchkovskii, Valeria Serbinenko, Hadas Soifer, Salvatore Stagira, Caterina Vozzi, Nirit Dudovich, Olga Smirnova

Research output: Contribution to journalArticlepeer-review

Abstract

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 multi-dimensional 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.

Original languageEnglish
Pages (from-to)369-405
Number of pages37
JournalFaraday Discussions
Volume194
DOIs
StatePublished - 2016
Externally publishedYes

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