Berlin 2024 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 88: Focus Session: Ultrafast Processes in Organic Semiconductors and Perovskites II (joint session O/CPP)
O 88.4: Vortrag
Donnerstag, 21. März 2024, 16:00–16:15, MA 004
Two-Dimensional Electronic Spectroscopy from First Principles — •Jannis Krumland1,2, Michele Guerrini1, Antonietta De Sio1, Christoph Lienau1, and Caterina Cocchi1,2 — 1Carl von Ossietzky Universität Oldenburg, Physics Department and Center for Nanoscale Dynamics (CeNaD), D-26129 Oldenburg, Germany — 2Humboldt-Universität zu Berlin, Physics Department and IRIS Adlershof, D-12489 Berlin, Germany
In recent decades, two-dimensional electronic spectroscopy has been established as an experimental tool that can provide unprecedented insight into ultrafast light-matter interaction. Employing three to four concerted laser pulses, this technique is able to map out the third-order polarizability of molecules and extended systems, which contains rich information about nonlinear optical properties as well as vibronic excited-state dynamics following photoexcitation. Here, we present a first-principles approach to the simulation of two-dimensional spectra based on real-time time-dependent density functional theory and Ehrenfest molecular dynamics, applying it to prototypical molecules such as benzene and pyrene [1]. In contrast to other theoretical schemes, our approach does not require any external parameters and thus offers more predictive power. Several numerical techniques are employed to mitigate the computational complexity, making it manageable even for larger systems that are out of reach with other atomistic methods.
[1] J. Krumland et al., arXiv:2308.09062 (2023)