Unusual Quantum Interference in the S1 State of DABCO and Observation of Intramolecular Vibrational Redistribution

In this paper we report an experimental study of the time-resolved response of the molecule 1,4-diazabicyclo[2.2.2]octane (DABCO) to 266.3 nm electronic excitation of the S1 state with a femtosecond laser. Rotational decoherence and vibrational oscillation within the S1 state are observed. We perfor...

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Published in:The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2010-03, Vol.114 (9), p.3313-3319
Main Authors: Poisson, Lionel, Maksimenska, Raman, Soep, Benoît, Mestdagh, Jean-Michel, Parker, David H, Nsangou, Mama, Hochlaf, Majdi
Format: Article
Language:English
Subjects:
Chemical Sciences
Lasers
or physical chemistry
Piperazines - chemistry
Quantum Theory
Theoretical and
Time Factors
Vibration
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container_issue 9
container_start_page 3313
container_title The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory
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creator Poisson, Lionel
Maksimenska, Raman
Soep, Benoît
Mestdagh, Jean-Michel
Parker, David H
Nsangou, Mama
Hochlaf, Majdi
description In this paper we report an experimental study of the time-resolved response of the molecule 1,4-diazabicyclo[2.2.2]octane (DABCO) to 266.3 nm electronic excitation of the S1 state with a femtosecond laser. Rotational decoherence and vibrational oscillation within the S1 state are observed. We performed state-of-the-art ab initio calculations on the ground and low electronic states of the neutral molecule and the cation, which assist in the assignment of the observed photoelectron signals. Using our theoretical and spectroscopic data, the experimental findings are interpreted in terms of an unusual quantum interference between two different vibrational modes, with only the ν = 1 level of each mode being populated.
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subjects Chemical Sciences
Lasers
or physical chemistry
Piperazines - chemistry
Quantum Theory
Theoretical and
Time Factors
Vibration
title Unusual Quantum Interference in the S1 State of DABCO and Observation of Intramolecular Vibrational Redistribution
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