Polarized pump-probe measurements of electronic motion via a conical intersection

The Journal of Chemical Physics
Darcie A FarrowDavid M Jonas

Abstract

Polarized femtosecond pump-probe spectroscopy is used to observe electronic wavepacket motion for vibrational wavepackets centered on a conical intersection. After excitation of a doubly degenerate electronic state in a square symmetric silicon naphthalocyanine molecule, electronic motions cause a approximately 100 fs drop in the polarization anisotropy that can be quantitatively predicted from vibrational quantum beat modulations of the pump-probe signal. Vibrational symmetries are determined from the polarization anisotropy of the vibrational quantum beats. The polarization anisotropy of the totally symmetric vibrational quantum beats shows that the electronic wavepackets equilibrate via the conical intersection within approximately 200 fs. The relationship used to predict the initial electronic polarization anisotropy decay from the asymmetric vibrational quantum beat amplitudes indicates that the initial width of the vibrational wavepacket determines the initial speed of electronic wavepacket motion. For chemically reactive conical intersections, which can have 1000 times greater stabilization energies than the one observed here, the same theory predicts electronic equilibration within 2 fs. Such electronic movements would ...Continue Reading

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Citations

Mar 23, 2011·The Journal of Physical Chemistry. a·Eric R Smith, David M Jonas
Aug 24, 2011·The Journal of Physical Chemistry. a·Anat KahanYehuda Haas
May 1, 2013·The Journal of Physical Chemistry. a·Inchan HwangGregory D Scholes
Dec 4, 2013·The Journal of Physical Chemistry. a·Brian P Molesky, Andrew M Moran
Dec 17, 2009·The Journal of Chemical Physics·Jason D Biggs, Jeffrey A Cina
Apr 5, 2014·The Journal of Chemical Physics·Katherine A Kitney-HayesDavid M Jonas
Dec 18, 2013·The Journal of Chemical Physics·Yu LiangAndreas-Neil Unterreiner
Dec 10, 2015·The Journal of Physical Chemistry Letters·Johanna BrazardDaniel B Turner
Mar 5, 2016·The Journal of Physical Chemistry. a·Alexey BukreevVictor A Nadtochenko
May 27, 2017·Nature Communications·Erling ThyrhaugDonatas Zigmantas
Sep 1, 2019·The Journal of Chemical Physics·Thomas Schaupp, Volker Engel
Mar 3, 2018·The Journal of Chemical Physics·Vivek Tiwari, David M Jonas
Feb 19, 2013·Chemical Society Reviews·Elisabetta Collini
Feb 24, 2017·The Journal of Chemical Physics·Kilian HaderVolker Engel
Aug 9, 2020·Physical Chemistry Chemical Physics : PCCP·Ioanna A GorbunovaOleg S Vasyutinskii
Jun 26, 2013·Angewandte Chemie·Fabrizio MessinaMajed Chergui
Feb 28, 2009·The Journal of Physical Chemistry. a·Elisabetta Collini, Gregory D Scholes
Apr 24, 2021·The Journal of Chemical Physics·Julian LüttigPavel Malý
Jun 7, 2012·The Journal of Physical Chemistry Letters·Tomáš MančalJürgen Hauer
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Sep 20, 2012·The Journal of Physical Chemistry Letters·Brantley A West, Andrew M Moran
Dec 19, 2018·The Journal of Physical Chemistry Letters·M E CorralesL Bañares

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