Real-Time Probing of Structural Dynamics by Interaction between Chromophores

Rasmus Y. Brogaard; Klaus Braagaard Møller; Theis Ivan Sølling

doi:10.1021/jp2072588

Real-Time Probing of Structural Dynamics by Interaction between Chromophores

Rasmus Y. Brogaard, Klaus Braagaard Møller, Theis Ivan Sølling

Department of Chemistry

Research output: Contribution to journal › Journal article › Research › peer-review

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Abstract

We present an investigation of structural dynamics in excited-state cations probed in real-time by femtosecond timeresolved ion photofragmentation spectroscopy. From photoelectron spectroscopy data on 1,3-dibromopropane we conclude that the pump pulse ionizes the molecule, populating an excited electronic state of the radical cation. In this state a coherent torsional vibration of the bromomethylene groups with a period of 700 fs is started and probed by photoinduced fragmentation of the molecular cation. The vibrational coherence dephases with the decay of the excited state to the ground state of the cation in 1.6 ps. The real-time probing of the excited-state dynamics is made possible by exploiting the interaction between the two bromine chromophores and its dependence on molecular conformation. This experiment therefore illustrates the applicability of the concept of probing ultrafast molecular dynamics using the intramolecular interaction between two chromophores.

Original language	English
Journal	Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory
Volume	115
Pages (from-to)	12120-12125
ISSN	1089-5639
DOIs	https://doi.org/10.1021/jp2072588
Publication status	Published - 2011

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title = "Real-Time Probing of Structural Dynamics by Interaction between Chromophores",

abstract = "We present an investigation of structural dynamics in excited-state cations probed in real-time by femtosecond timeresolved ion photofragmentation spectroscopy. From photoelectron spectroscopy data on 1,3-dibromopropane we conclude that the pump pulse ionizes the molecule, populating an excited electronic state of the radical cation. In this state a coherent torsional vibration of the bromomethylene groups with a period of 700 fs is started and probed by photoinduced fragmentation of the molecular cation. The vibrational coherence dephases with the decay of the excited state to the ground state of the cation in 1.6 ps. The real-time probing of the excited-state dynamics is made possible by exploiting the interaction between the two bromine chromophores and its dependence on molecular conformation. This experiment therefore illustrates the applicability of the concept of probing ultrafast molecular dynamics using the intramolecular interaction between two chromophores.",

author = "Brogaard, {Rasmus Y.} and M{\o}ller, {Klaus Braagaard} and S{\o}lling, {Theis Ivan}",

year = "2011",

doi = "10.1021/jp2072588",

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volume = "115",

pages = "12120--12125",

journal = "Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory",

issn = "1089-5639",

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Real-Time Probing of Structural Dynamics by Interaction between Chromophores. / Brogaard, Rasmus Y.; Møller, Klaus Braagaard; Sølling, Theis Ivan.

In: Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, Vol. 115, 2011, p. 12120-12125.

Research output: Contribution to journal › Journal article › Research › peer-review

TY - JOUR

T1 - Real-Time Probing of Structural Dynamics by Interaction between Chromophores

AU - Brogaard, Rasmus Y.

AU - Møller, Klaus Braagaard

AU - Sølling, Theis Ivan

PY - 2011

Y1 - 2011

N2 - We present an investigation of structural dynamics in excited-state cations probed in real-time by femtosecond timeresolved ion photofragmentation spectroscopy. From photoelectron spectroscopy data on 1,3-dibromopropane we conclude that the pump pulse ionizes the molecule, populating an excited electronic state of the radical cation. In this state a coherent torsional vibration of the bromomethylene groups with a period of 700 fs is started and probed by photoinduced fragmentation of the molecular cation. The vibrational coherence dephases with the decay of the excited state to the ground state of the cation in 1.6 ps. The real-time probing of the excited-state dynamics is made possible by exploiting the interaction between the two bromine chromophores and its dependence on molecular conformation. This experiment therefore illustrates the applicability of the concept of probing ultrafast molecular dynamics using the intramolecular interaction between two chromophores.

AB - We present an investigation of structural dynamics in excited-state cations probed in real-time by femtosecond timeresolved ion photofragmentation spectroscopy. From photoelectron spectroscopy data on 1,3-dibromopropane we conclude that the pump pulse ionizes the molecule, populating an excited electronic state of the radical cation. In this state a coherent torsional vibration of the bromomethylene groups with a period of 700 fs is started and probed by photoinduced fragmentation of the molecular cation. The vibrational coherence dephases with the decay of the excited state to the ground state of the cation in 1.6 ps. The real-time probing of the excited-state dynamics is made possible by exploiting the interaction between the two bromine chromophores and its dependence on molecular conformation. This experiment therefore illustrates the applicability of the concept of probing ultrafast molecular dynamics using the intramolecular interaction between two chromophores.

U2 - 10.1021/jp2072588

DO - 10.1021/jp2072588

M3 - Journal article

C2 - 21958192

VL - 115

SP - 12120

EP - 12125

JO - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

JF - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

SN - 1089-5639

ER -