Signature of Attochemical Quantum Interference upon Ionization and Excitation of an Electronic Wave Packet in Fluorobenzene

Phys Rev Lett. 2024 Nov 15;133(20):203201. doi: 10.1103/PhysRevLett.133.203201.

Abstract

Ultrashort pulses can excite or ionize molecules and populate coherent electronic wave packets, inducing complex dynamics. In this Letter, we simulate the coupled electron-nuclear dynamics upon ionization to different electronic wave packets of (deuterated) benzene and fluoro-benzene molecules, quantum mechanically and in full dimensionality. In fluoro-benzene, the calculations unravel both interstate and intrastate quantum interferences that leave clear signatures of attochemistry and charge-directed dynamics in the shape of the autocorrelation function. The latter are in agreement with experimental high-harmonic spectroscopy measurements of benzenes and fluoro-benzene.