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 language | English |
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Pages (from-to) | 25118-25130 |
Number of pages | 13 |
Journal | Physical Chemistry Chemical Physics |
Volume | 26 |
Issue number | 38 |
DOIs | |
State | Published - 2024/08/23 |
ASJC Scopus subject areas
- General Physics and Astronomy
- Physical and Theoretical Chemistry