TY  - JOUR
A1  - Titov, Evgenii
A1  - Kopp, Tristan
A1  - Hoche, Joscha
A1  - Humeniuk, Alexander
A1  - Mitrić, Roland
T1  - (De)localization dynamics of molecular excitons
BT  - comparison of mixed quantum-classical and fully quantum treatments
JF  - Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies
N2  - Molecular excitons play a central role in processes of solar energy conversion, both natural and artificial. It is therefore no wonder that numerous experimental and theoretical investigations in the last decade, employing state-of-the-art spectroscopic techniques and computational methods, have been driven by the common aim to unravel exciton dynamics in multichromophoric systems. Theoretically, exciton (de)localization and transfer dynamics are most often modelled using either mixed quantum-classical approaches (e.g., trajectory surface hopping) or fully quantum mechanical treatments (either using model diabatic Hamiltonians or direct dynamics). Yet, the terms such as "exciton localization" or "exciton transfer" may bear different meanings in different works depending on the method in use (quantum-classical vs. fully quantum). Here, we relate different views on exciton (de)localization. For this purpose, we perform molecular surface hopping simulations on several tetracene dimers differing by a magnitude of exciton coupling and carry out quantum dynamical as well as surface hopping calculations on a relevant model system. The molecular surface hopping simulations are done using efficient long-range corrected time-dependent density functional tight binding electronic structure method, allowing us to gain insight into different regimes of exciton dynamics in the studied systems.
Y1  - 2022
U6  - https://doi.org/10.1039/d2cp00586g
SN  - 1463-9076
SN  - 1463-9084
VL  - 24
IS  - 20
SP  - 12136
EP  - 12148
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  -