Dissertation

Coupled Electronic and Nuclear Dynamics at Interfaces of Artificial Photosynthesis Devices

Reducing greenhouse gas emissions is one of the most pressing challenges that humanity faces in the coming decades.

Author: T. de Haas
Date: 04 September 2025
Links: Thesis in Leiden Repository

As a platform for generating solar fuels, dye-sensitized photoelectrochemical cells (DS-PECs) offer a promising solution. DS-PECs effectively address the intermittency issues inherent to solar and wind energy by storing solar energy in chemical bonds to generate sustainable fuels. However, the design of efficient DS-PECs remains challenging due to sluggish catalytic turnovers and low charge separation efficiencies. Addressing these limitations requires a deeper understanding of the physical mechanisms that govern these processes. With this goal in mind, this dissertation aims to elucidate at an atomistic level the mechanisms that drive photo-induced charge separation and catalysis in various components of DS-PEC devices. A strong emphasis is placed on the coupled motion of nuclear and electronic degrees of freedom, which I demonstrate to be crucial for many of the investigated systems.