Measuring excitation-energy transfer with a real-time time-dependent density functional theory approach

Abstract

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schrödinger equation and uses a Hamiltonian from time-dependent density functional theory (TDDFT). It treats electronic-structure properties and intermolecular coupling on the level of TDDFT, while it opens a route to the description of dissipation and relaxation via a bath operator that couples to the dipole moment of the density. Within our study, we find that in supermolecular setups small deviations of the electronic structure from the perfectly resonant case have only minor influence on the pathways of excitation-energy transfer, thus lead to similar transfer times. Yet, sizable defects cause notable slowdown of the energy spread.

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Cited by in corpus (3)

• The Driven Liouville von Neumann Equation in Lindblad Form
• Probing quantum coherence in ultrafast molecular processes: an ab initio approach to open quantum systems
• A State Representation Approach for Atomistic Time-Dependent Transport Calculations in Molecular Junctions