title: Multidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields.
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 CO2molecule 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.
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel. nirit.dudovich@weizmann.ac.il.
authors.forename: Barry D
authors.initials: BD
authors.lastname: Bruner
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Zdeněk
authors.initials: Z
authors.lastname: Mašín
authors.affiliation: Istituto di Fotonica e Nanotecnologie-CNR, Milan 20133, Italy.
authors.forename: Matteo
authors.initials: M
authors.lastname: Negro
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Felipe
authors.initials: F
authors.lastname: Morales
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Danilo
authors.initials: D
authors.lastname: Brambila
authors.affiliation: Istituto di Fotonica e Nanotecnologie-CNR, Milan 20133, Italy.
authors.forename: Michele
authors.identifier: 0000-0002-3806-3475
authors.initials: M
authors.lastname: Devetta
authors.affiliation: Dipartimento di Fisica, Politecnico di Milano, Milan 20133, Italy.
authors.forename: Davide
authors.initials: D
authors.lastname: Faccialà
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Alex G
authors.initials: AG
authors.lastname: Harvey
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Misha
authors.initials: M
authors.lastname: Ivanov
authors.affiliation: CELIA, Université de Bordeaux-CNRS-CEA, UMR5107, F33405 Talence, France.
authors.forename: Yann
authors.initials: Y
authors.lastname: Mairesse
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Serguei
authors.initials: S
authors.lastname: Patchkovskii
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Valeria
authors.initials: V
authors.lastname: Serbinenko
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel. nirit.dudovich@weizmann.ac.il and Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors.forename: Hadas
authors.initials: H
authors.lastname: Soifer
authors.affiliation: Dipartimento di Fisica, Politecnico di Milano, Milan 20133, Italy.
authors.forename: Salvatore
authors.initials: S
authors.lastname: Stagira
authors.affiliation: Istituto di Fotonica e Nanotecnologie-CNR, Milan 20133, Italy.
authors.forename: Caterina
authors.initials: C
authors.lastname: Vozzi
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel. nirit.dudovich@weizmann.ac.il.
authors.forename: Nirit
authors.initials: N
authors.lastname: Dudovich
authors.affiliation: Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Max-Born-Strasse 2 A, 12489 Berlin, Germany.
authors.forename: Olga
authors.initials: O
authors.lastname: Smirnova