Quantum control of ro-vibrational dynamics and application to light-induced molecular chirality
arXiv (Cornell University)(2023)
摘要
Achiral molecules can be made temporarily chiral by excitation with electric
fields, in the sense that an average over molecular orientations displays a net
chiral signal [Tikhonov et al., Sci. Adv. 8, eade0311 (2022)]. Here, we go
beyond the assumption of molecular orientations to remain fixed during the
excitation process. Treating both rotations and vibrations quantum
mechanically, we identify conditions for the creation of chiral vibrational
wavepackets – with net chiral signals – in ensembles of achiral molecules
which are initially randomly oriented. Based on the analysis of symmetry and
controllability, we derive excitation schemes for the creation of chiral
wavepackets using a combination of (a) microwave and IR pulses and (b) a static
field and a sequence of IR pulses. These protocols leverage quantum rotational
dynamics for pump-probe spectroscopy of chiral vibrational dynamics, extending
the latter to regions of the electromagnetic spectrum other than the UV.
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关键词
quantum,molecular,dynamics,ro-vibrational,light-induced
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