Abstract
Electronic coherences in molecules are ultrafast charge oscillations on the molecular frame (MF) and their direct observation and separation from electronic population dynamics is challenging. Here we present a valence shell lab frame (LF) scattering method suited to probing electronic coherences in isolated systems. MF electronic coherences lead to LF electronic anisotropies observable by ultrafast angle-resolved scattering. Moment analysis of the LF anisotropy completely separates electronic coherences from population dynamics, demonstrated in excited state NH3 using ultrafast time-energy-angle-resolved photoelectron spectroscopy. This general approach applies equally to attosecond/femtosecond electronic coherences in isolated systems.
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