A1 Refereed original research article in a scientific journal
Time-resolved photoelectron diffraction imaging of methanol photodissociation involving molecular hydrogen ejection
Authors: Yoshikawa, Kazuki; Kanno, Manabu; Xue, Hao; Kishimoto, Naoki; Goto, Soki; Ota, Fukiko; Tamura, Yoshiaki; Trinter, Florian; Fehre, Kilian; Kaiser, Leon; Stindl, Jonathan; Tsitsonis, Dimitrios; Schoeffler, Markus; Doerner, Reinhard; Boll, Rebecca; Erk, Benjamin; Mazza, Tommaso; Mullins, Terence; Rivas, Daniel E.; Schmidt, Philipp; Usenko, Sergey; Meyer, Michael; Wang, Enliang; Rolles, Daniel; Rudenko, Artem; Kukk, Edwin; Jahnke, Till; Diaz-Tendero, Sergio; Martin, Fernando; Hatada, Keisuke; Ueda, Kiyoshi
Publisher: ROYAL SOCIETY OF CHEMISTRY
Publishing place: CAMBRIDGE
Publication year: 2024
Journal: Physical Chemistry Chemical Physics
Journal name in source: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Journal acronym: PHYS CHEM CHEM PHYS
Volume: 26
Issue: 38
First page : 25118
Last page: 25130
Number of pages: 13
ISSN: 1463-9076
eISSN: 1463-9084
DOI: https://doi.org/10.1039/d4cp01015a
Web address : https://doi.org/10.1039/D4CP01015A
Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/458531307
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.We explore time- and momentum-resolved photoelectron diffraction imaging (TMR-PED) to visualize hydrogen dynamics during methanol dication dissociation. Our approach allows real-time tracking of hydrogen migration and molecular fragmentation.
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Funding information in the publication:
This work was partially performed under the Cooperative Research Program of “Network Joint Research Center for Materials and Devices” and partially funded by the Spanish Ministry of Science and Innovation – Ministerio Español de Ciencia e Innovación MICINN – projects PID2022-138288NB-C31 and PID2022-138470NB-I00, the Severo Ochoa Programme for Centres of Excellence in R & D (CEX2020-001039-S) and the María de Maeztu Programme for Units of Excellence in R & D (CEX2023-001316-M). K. Y. acknowledges that this work was supported by JST, the establishment of university fellowships towards the creation of science technology innovation, Grant Number JPMJFS2115. N. K. and K. U. acknowledge research funding from the Institute for Quantum Chemical Exploration (IQCE). F. T. acknowledges funding from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – Project 509471550, Emmy Noether Programme. E. W., D. R., and A. R. were supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract No. DE-FG02-86ER13491. K. H. acknowledges funding from JSPS KAKENHI under Grant No. 18K05027 and 17K04980. This article is based upon work from COST actions CA18212 – Molecular Dynamics in the GAS phase (MD-GAS) and CA18222 – Attosecond Chemistry (AttoChem), supported by COST (European Cooperation in Science and Technology). We acknowledge the generous allocation of computer time at the Centro de Computación Científica at the Universidad Autónoma de Madrid (CCC-UAM). We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III and we would like to thank the P04 team for assistance in using the beamline. Beamtime was allocated for proposal I-20180746 EC. We acknowledge the European XFEL in Schenefeld, Germany, for the provision of XFEL beamtime at the SQS instrument and would like to thank the staff for their assistance. The experimental work was supported by the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)-EXC 2056-project ID 390715994, by BMBF, and in part by the Deutsche Forschungsgemeinschaft (DFG) Project No. 328961117-SFB 1319 ELCH (extreme light for sensing and driving molecular chirality, subproject B1). Open Access funding provided by the Max Planck Society.
