Coupled nuclear and electron dynamics in the vicinity of a conical intersection

Abstract

Ultrafast optical techniques allow to study ultrafast molecular dynamics involving both nuclear and electronic motion.To support interpretation, theoretical approaches are needed that can describe both the nuclear and electron dynamics.Hence, we revisit and expand our ansatz for the coupled description of the nuclear and electron dynamics in molecular systems (NEMol). In this purely quantum mechanical ansatz the quantum-dynamical description of the nuclear motion is combined with the calculation of the electron dynamics in the eigenfunction basis. The NEMol ansatz is applied to simulate the coupled dynamics of the molecule NO2 in the vicinity of a conical intersection (CoIn) with a special focus on the coherent electron dynamics induced by the non-adiabatic coupling. Furthermore, we aim to control the dynamics of the system when passing the CoIn. The control scheme relies on the carrier envelope phase (CEP) of a few-cycle IR pulse. The laser pulse influences both the movement of the nuclei and the electrons during the population transfer through the CoIn.

References in corpus (6)

• Attosecond control of electron dynamics in carbon monoxide
• Electronic decoherence following photoionization: full quantum-dynamical treatment of the influence of nuclear motion
• Unitary theory of laser Carrier-Envelope Phase effects
• Control of charge migration in molecules by ultrashort laser pulses
• Time-dependent coupled cluster theory for ultrafast transient absorption spectroscopy
• The role of geometric phase in the formation of electronic coherences at conical intersections