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SUMMARY:Inhibiting Vibrational Coherence Transfer in a Small Molecular Syst
 em via Isotope Substitution
LOCATION:Chemistry A101
TZID:America/Denver
DTSTART:20240809T160000
UID:2026-04-27-09-54-55@natsci.colostate.edu
DTSTAMP:20260427T095455
Description:Coherence transfer (CT) describes dynamic pathways in which non
 trivial system-bath coupling leads to the interconversion of quantum super
 positions\, representing a quantum mechanical analog of population relaxat
 ion.1 Time dependent spectroscopic techniques such as transient absorption
  and two-dimensional spectroscopies previously identified signatures of CT
  in processes ranging from charge transfer in photosynthetic proteins2 to 
 vibrational relaxation in small molecules. However\, spectral overlap betw
 een CT and population relaxation pathways complicates the interpretation o
 f experimental data. Computational models of CT are not always practical t
 o implement\, particularly for CT occurring between superpositions of vibr
 ational energy levels.3 As such\, identifying experimental methods to supp
 ress vibrational CT could provide a convenient means of recovering populat
 ion dynamics from time-dependent spectra.\n\nSupporting this effort\, we u
 se two-dimensional infrared spectroscopy (2DIR) to investigate the carbony
 l stretching region of ethylene carbonate dissolved in tetrahydrofuran. Al
 though only one fundamental vibrational transition exists in this region\,
  Fermi resonance coupling leads to the observation of multiple bands in th
 e experimental spectra.4 Our 2DIR experiments reveal extensive evidence of
  CT in the carbonyl region. We investigate the role of Fermi resonance cou
 pling in vibrational CT\, utilizing isotope substitution to modify the Fer
 mi coupling strength. We then compare signatures of CT between ethylene ca
 rbonate isotopologues and find a significant reduction of CT upon weakenin
 g the Fermi resonance coupling. These findings demonstrate that the effect
 s of vibrational CT in 2DIR spectra can be suppressed by isotope substitut
 ion\, and applications to other systems will allow for time-dependent vibr
 ational spectroscopies to report on the population dynamics of a wider ran
 ge of chemical systems. 4:00 pm
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