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Imaging ultrafast hydrogen migration with few- or sub-femtosecond time resolution is a challenge for ultrafast spectroscopy due to the lightness and small scattering cross-section of the moving hydrogen atom. Here we propose time- and momentum-resolved photoelectron diffraction (TMR-PED) as a way to overcome limitations of existing methodologies and illustrate its performance in the ethanol molecule. By combining different theoretical methods, namely molecular dynamics and electron scattering methods, we show that TMR-PED, along with a judicious choice of the reference frame for multi-coincidence detection, allows for direct imaging of single and double hydrogen migration in doubly-charged ethanol with both few-fs and Å resolutions, all the way from its birth to the very end. It also provides hints of proton extraction following H 2 roaming. The signature of hydrogen dynamics shows up in polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) as moving features that allow for a straightforward visualization in space.

Imaging intramolecular hydrogen migration with time- and momentum-resolved photoelectron diffraction