Observation of structural relaxation during exciton self-trapping via excited-state resonant impulsive stimulated Raman spectroscopy

The Journal of Chemical Physics
J G ManceS L Dexheimer

Abstract

We detect the change in vibrational frequency associated with the transition from a delocalized to a localized electronic state using femtosecond vibrational wavepacket techniques. The experiments are carried out in the mixed-valence linear chain material [Pt(en)2][Pt(en)2Cl2]⋅(ClO4)4 (en = ethylenediamine, C2H8N2), a quasi-one-dimensional system with strong electron-phonon coupling. Vibrational spectroscopy of the equilibrated self-trapped exciton is carried out using a multiple pulse excitation technique: an initial pump pulse creates a population of delocalized excitons that self-trap and equilibrate, and a time-delayed second pump pulse tuned to the red-shifted absorption band of the self-trapped exciton impulsively excites vibrational wavepacket oscillations at the characteristic vibrational frequencies of the equilibrated self-trapped exciton state by the resonant impulsive stimulated Raman mechanism, acting on the excited state. The measurements yield oscillations at a frequency of 160 cm(-1) corresponding to a Raman-active mode of the equilibrated self-trapped exciton with Pt-Cl stretching character. The 160 cm(-1) frequency is shifted from the previously observed wavepacket frequency of 185 cm(-1) associated with the i...Continue Reading

References

Sep 1, 1993·Physical Review. B, Condensed Matter·I BatisticA Saxena
Sep 16, 2000·Physical Review Letters·S L DexheimerB I Swanson
Dec 22, 2006·The Review of Scientific Instruments·David W McCamantRichard A Mathies
Feb 2, 2013·Physical Review Letters·Denis GoležStuart A Trugman
Mar 13, 2013·Journal of Physics. Condensed Matter : an Institute of Physics Journal·F X MorrisseyS L Dexheimer
Jul 31, 2013·Physical Chemistry Chemical Physics : PCCP·Jan Philip KraackSanford Ruhman

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