MBI Colloquium
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Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy
Max-Born-Straße 2a,
12489 Berlin
Max Born Hall
Ultrafast Molecular Dynamics Driven by Electrons and Nuclei
Prof. Oriol Vendrell | Heidelberg University
When electronic states are energetically well separated from each other, electrons in molecules follow the motion of nuclei instantaneously and, in turn, the nuclei move on a single potential determined by one of the adiabatic electronic states. However, most photo-physics and photo-chemistry take place under conditions where this separation of time-scales breaks down, with dramatic consequences for the short-time dynamics after photo-absorption, the stability of photo-excited molecules, and the underlying mechanisms of charge and energy
transfer triggered by light.
In this talk, we shortly review the theoretical description of quantum non-adiabatic molecular dynamics and the computational tools needed to tackle it accurately and efficiently. Next, we explore the relation between non-adiabatic phenomena and electronic coherence, and show theoretically how pump-probe schemes using ultrafast x-rays can be used to both trigger and probe such dynamics. Finally, we describe how electronic angular momentum and non-adiabaticity are connected in ring-shaped molecules in, maybe, surprising ways.
References:
[1] Freibert, A.; Mendive-Tapia, D.; Huse, N.; Vendrell, O.
Femtosecond X-Ray Absorption Spectroscopy of Pyrazine at the Nitrogen K-Edge: On the Validity of the Lorentzian Limit.
J. Phys. B: At. Mol. Opt. Phys. 54, 244003 (2021) [doi: 10.1088/1361-6455/ac3846]
[2] Freibert, A.; Mendive-Tapia, D.; Huse, N.; Vendrell, O.
Time-Dependent Resonant Inelastic X-ray Scattering of Pyrazine at the Nitrogen K-Edge: A Quantum Dynamics Approach.
J. Chem. Theory Comput. 20, 2167 (2024) [doi: 10.1021/acs.jctc.3c01259]
[3] Rodriguez-Cuenca, E; Pic n, A; Oberly, S; Kuleff, A.I.; Vendrell, O.
Core-hole Coherent Spectroscopy in Molecules
Phys. Rev. Lett. 132, 263202 (2024) [doi: 10.1103/PhysRevLett.132.263202]
[4] Nandipati, K.R.; Sasmal, S; Vendrell, O.
Inverse Optically-Induced Ring Currents in Ring-Shaped Molecules
J. Phys. Chem. Lett. 5034, 15 (2024) [doi: 10.1021/acs.jpclett.4c00570]