Time-resolved photoelectron diffraction imaging of methanol photodissociation involving molecular hydrogen ejection

Kazuki Yoshikawa, Manabu Kanno*, Hao Xue, Naoki Kishimoto*, Soki Goto, Fukiko Ota, Yoshiaki Tamura, Florian Trinter*, Kilian Fehre, Leon Kaiser, Jonathan Stindl, Dimitrios Tsitsonis, Markus Schöffler, Reinhard Dörner, Rebecca Boll, Benjamin Erk, Tommaso Mazza, Terence Mullins, Daniel E. Rivas, Philipp SchmidtSergey Usenko, Michael Meyer, Enliang Wang, Daniel Rolles, Artem Rudenko, Edwin Kukk, Till Jahnke, Sergio Díaz-Tendero*, Fernando Martín, Keisuke Hatada*, Kiyoshi Ueda*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Imaging ultrafast atomic and molecular hydrogen motion with femtosecond time resolution is a challenge for ultrafast spectroscopy due to the low mass and small scattering cross section of the moving neutral hydrogen atoms and molecules. Here, we propose time- and momentum-resolved photoelectron diffraction (TMR-PED) as a way to overcome limitations of existing methodologies and illustrate its performance using a prototype molecular dissociation process involving the sequential ejection of a neutral hydrogen molecule and a proton from the methanol dication. By combining state-of-the-art molecular dynamics and electron-scattering methods, we show that TMR-PED allows for direct imaging of hydrogen atoms in action. More specifically, the fingerprint of hydrogen dynamics reflects the time evolution of polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) as would be recorded in X-ray pump/X-ray probe experiments with few-femtosecond resolution. We present the results of two precursor experiments that support the feasibility of this approach.

Original languageEnglish
Pages (from-to)25118-25130
Number of pages13
JournalPhysical Chemistry Chemical Physics
Volume26
Issue number38
DOIs
StatePublished - 2024/08/23

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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