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

• DOI: 10.1039/c6fd00130k
• Publication Date: 2016-09-26T10:00:18Z
• Authors: 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
• Keywords: Attosecond

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 response also opens multiple quantum pathways for multielectron molecules, resulting complex process of rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG used to detect follow core sub-laser cycle scales. We signatures laser-driven hole upon ionization reconstruct relative phases amplitudes relevant channels CO₂ molecule sub-cycle Reconstruction channel-resolved scales been long-standing goal spectroscopy. Our study brings us one step closer fulfilling this initial promise developing robust schemes sub-femtosecond imaging molecular systems.