PROBING QUANTUM COHERENCE IN MOLECULAR SYSTEMS

Olowolafe, Temitayo A.

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Description

Title

PROBING QUANTUM COHERENCE IN MOLECULAR SYSTEMS

Author(s)

Olowolafe, Temitayo A.

Contributor(s)

• Li, Wen
• Schlegel, H. Bernhard
• Lee, Suk Kyoung
• Yarlagadda, Suresh

Issue Date

2023-06-19

Keyword(s)

Mini-symposium: Spectroscopy at Large-scale Facilities

Abstract

Ultrafast spectroscopy can initiate and probe electronic dynamics in molecules within femtoseconds to attoseconds timescale. Here, we report the use of strong field ionization pump-probe technique to detect multimode vibrational motions and electronic coherence in methyl iodide cation (CH3I+). For the first time, the coherence between the spin-orbit components of methyl iodide cation ground states and all symmetric vibrational modes were captured. The periodicities of the detected quantum beats vary between 6.0 fs and 117.0 fs. A few vibrational beatings from the first excited state (A state) were also detected. Furthermore, our approach reveals the time evolution of the quantum coherence in methyl iodide cation. The electronic coherence decays in the first picosecond while vibrational quantum beats persist. Our study further showed that rotational revival does not revive electronic coherence, suggesting both vibrational and rotational dephasings play a role in the decay of electronic quantum beatings. Theoretical analysis using a quantum model reveals intimate interaction between electronic and vibrational coherence in polyatomic systems.

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

Text

Language

eng

Handle URL

https://hdl.handle.net/2142/122640

DOI

https://doi.org/10.15278/isms.2023.7158

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