Begušić Group - Quantum Dynamics
Prof. Dr. Tomislav Begušić
2015 BSc in Chemistry, University of Zagreb
2017 MSc in Chemistry, EPFL
2021 PhD under Jiří Vaníček, EPFL
2021-2023 Postdoc with Thomas Miller & Geoffrey Blake, Caltech
2023-2025 Postdoc with Garnet Chan, Caltech
Since 2025 Professor, University of Würzburg
Quantum dynamics
Our research focuses on quantum dynamics of molecular systems, with applications to ultrafast processes and time-resolved spectroscopy. To tackle the simulation of high-dimensional quantum dynamics, we build our methods on semiclassical approximations, as well as efficient sparse or low-rank representations. Our group is particularly interested in combining these concepts to yield new systematically improvable approaches employing CPU, GPU, and quantum computing resources. These dynamical tools are then applied to individual molecules or supramolecular assemblies, where we investigate how the features in state-of-the-art time-resolved and high-order optical spectroscopies correlate with nuclear and electronic dynamics.
PRX Quantum 6, 020302 (2025)
Sci. Adv. 10, eadk4321 (2024)
J. Phys. Chem. Lett. 12(11), 2997 (2021)
J. Chem. Phys. 153, 024105 (2020)
Liquids and solvation
We are also exploring the capabilities of new nonlinear vibrational spectroscopies, such as 2D infrared or hybrid infrared-Raman spectroscopies, to understand the structure and dynamics in molecular liquids. Here, we focus on classical and ring-polymer molecular dynamics methods. The developments include extending the existing approaches to multi-time response functions and combining them with accurate potential energy and dipole moment surfaces. We then employ these simulation techniques to propose and analyze new spectroscopic observables that carry information about vibrations in molecular liquids, solvated chromophores, or at solid-liquid interfaces. In this context, we also research new types of vibrational probes that report on the structure and dynamics of the surrounding solvent molecules.
J. Chem. Phys. 156 (13), 131102 (2022)
Nat. Commun. 14, 1950 (2023)
J. Phys. Chem. B 127 (22) 4979 (2023)
