Precision Franck-Condon spectroscopy from highly-excited vibrational states

Fuente: arXiv
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Main Authors: Pannir-Sivajothi, Sindhana, Yuen-Zhou, Joel
Format: Preprint
Published: 2024
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author Pannir-Sivajothi, Sindhana
Yuen-Zhou, Joel
author_facet Pannir-Sivajothi, Sindhana
Yuen-Zhou, Joel
contents As per the Franck-Condon principle, absorption spectroscopy reveals changes in nuclear geometry in molecules or solids upon electronic excitation. It is often assumed these changes cannot be resolved beyond the ground vibrational wavefunction width ($\sqrt{\hbar/mω}$). Here, we show this resolution dramatically improves with highly-excited vibrational initial states (with occupation number $\langle n\rangle$). These states magnify changes in geometry by $2\langle n\rangle +1$, a possibly counterintuitive result given the spatial uncertainty of Fock states grows with $n$. We also discuss generalizations of this result to multimode systems. Our result is relevant to optical spectroscopy, polariton condensates, and quantum simulators ($\textit{e.g.}$, boson samplers).
format Preprint
id arxiv_https___arxiv_org_abs_2401_10384
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Precision Franck-Condon spectroscopy from highly-excited vibrational states
Pannir-Sivajothi, Sindhana
Yuen-Zhou, Joel
Chemical Physics
Quantum Physics
As per the Franck-Condon principle, absorption spectroscopy reveals changes in nuclear geometry in molecules or solids upon electronic excitation. It is often assumed these changes cannot be resolved beyond the ground vibrational wavefunction width ($\sqrt{\hbar/mω}$). Here, we show this resolution dramatically improves with highly-excited vibrational initial states (with occupation number $\langle n\rangle$). These states magnify changes in geometry by $2\langle n\rangle +1$, a possibly counterintuitive result given the spatial uncertainty of Fock states grows with $n$. We also discuss generalizations of this result to multimode systems. Our result is relevant to optical spectroscopy, polariton condensates, and quantum simulators ($\textit{e.g.}$, boson samplers).
title Precision Franck-Condon spectroscopy from highly-excited vibrational states
topic Chemical Physics
Quantum Physics
url https://arxiv.org/abs/2401.10384