Time-resolved photoelectron spectroscopy of coupled electron-nuclear motion

Abstract

We investigate pump-probe electron detachment spectroscopy in a model system which is ideally suited to study coupled electronic and nuclear wave-packet dynamics. Time-resolved photoelectron spectra are calculated within the adiabatic approximation and a discretization of the detachment continuum. These spectra are compared to those which derive from a non-Born-Oppenheimer description and a numerically exact treatment of the detachment process. In this way it is possible to identify the influence of non-adiabatic effects on the spectra in a systematic way and also to test commonly applied approximations.

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

“…We attribute this to the chosen near-equilibrium initial conditions for χ(R). Previous studies have shown, that nuclear dynamics following initial non-equilibrium configurations is reflected in the photoelectron momentum distribution [37,38]. Investigations of such effects on the correlation-driven knock-up and knockdown processes are currently under way in our workgroup.…”

Time-Resolved Photoelectron Spectroscopy of Coupled Nuclear-Electronic Dynamics

“…The relative heights of these peaks provide an estimate of the nonadiabatic transition amplitudes, see Ref. [11].…”

“…Left panels: weak coupling (R c = 1.5 Å), right panels: strong coupling (R c = 2.5 Å), as labeled (adapted from Ref. [11]). …”

“…We numerically solve the coupled nuclear electronic Schrödinger equation (2D), as well as the nuclear Schrödinger equation in a fixed electronic state |n〉 within the Born-Oppenheimer approximation (BO) on a grid using the splitoperator method. The XUV interaction for the BO calculations is treated within first order perturbation theory, for details see [11]. …”

Atomic photoionization dynamics in ultrashort cycloidal laser fields

“…Since photoionization with CRCP or COCP pulses cancels the cylindrical symmetry of the electron wave function, 2D numerical simulations are necessary to describe the asymmetric polarization profiles but also sufficient to capture the essential features of the PMD. Two-dimensional approaches to solve the TDSE (2dTDSE) have successfully been applied, amongst others, to model the scattering of free particles [29], atomic double ionization [30,31], coupled electron-nuclear dynamics in molecules [32][33][34] and the photoelectron circular dichroism [35]. Very recently, Zhen et al [21] applied the 2dTDSE method to study electron vortices in the photoionization of hydrogen atoms by CRCP pulse sequences.…”