Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

Abstract

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

References in corpus (8)

• Photoelectron angular distributions from strong-field ionization of oriented molecules
• Imaging an aligned polyatomic molecule with laser-induced electron diffraction
• Imaging electronic quantum motion with light
• Imaging Molecular Structure through Femtosecond Photoelectron Diffraction on Aligned and Oriented Gas-Phase Molecules
• Theory of time-resolved non-resonant x-ray scattering for imaging ultrafast coherent electron motion
• Imaging interatomic electron current in crystals with ultrafast resonant x-ray scattering
• Imaging instantaneous electron flow with ultrafast resonant x-ray scattering
• Monitoring the Birth of an Electronic Wavepacket in a Neutral Molecule with Attosecond Time-Resolved Photoelectron Spectroscopy

Cited by in corpus (8)

• Photoinduced dynamics of organic molecules using nonequilibrium Green's functions with second-Born, $GW$, $T$-matrix and three-particle ladder correlations
• Ultrafast molecular orbital tomography of a pentacene thin film using time-resolved momentum microscopy at a free-electron laser
• Detecting coherent core-hole wave-packet dynamics in N2 by time- and angle-resolved inner-shell photoelectron spectroscopy
• Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective
• Photophysics of indole upon x-ray absorption
• Attosecond imaging of photo-induced dynamics in molecules using time-resolved photoelectron momentum microscopy
• Photoemission orbital tomography for excitons in organic molecules
• Controlling rotation in the molecular-frame with an optical centrifuge