Issue 38, 2024

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

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.

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

Supplementary files

Article information

Article type
Paper
Submitted
07 Mar 2024
Accepted
22 Aug 2024
First published
23 Aug 2024
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2024,26, 25118-25130

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

K. Yoshikawa, M. Kanno, H. Xue, N. Kishimoto, S. Goto, F. Ota, Y. Tamura, F. Trinter, K. Fehre, L. Kaiser, J. Stindl, D. Tsitsonis, M. Schöffler, R. Dörner, R. Boll, B. Erk, T. Mazza, T. Mullins, D. E. Rivas, P. Schmidt, S. Usenko, M. Meyer, E. Wang, D. Rolles, A. Rudenko, E. Kukk, T. Jahnke, S. Díaz-Tendero, F. Martín, K. Hatada and K. Ueda, Phys. Chem. Chem. Phys., 2024, 26, 25118 DOI: 10.1039/D4CP01015A

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements