Modified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons.

Abstract:

:Coupling vibrational transitions to resonant optical modes creates vibrational polaritons shifted from the uncoupled molecular resonances and provides a convenient way to modify the energetics of molecular vibrations. This approach is a viable method to explore controlling chemical reactivity. In this work, we report pump-probe infrared spectroscopy of the cavity-coupled C-O stretching band of W(CO)6 and the direct measurement of the lifetime of a vibration-cavity polariton. The upper polariton relaxes 10 times more quickly than the uncoupled vibrational mode. Tuning the polariton energy changes the polariton transient spectra and relaxation times. We also observe quantum beats, so-called vacuum Rabi oscillations, between the upper and lower vibration-cavity polaritons. In addition to establishing that coupling to an optical cavity modifies the energy-transfer dynamics of the coupled molecules, this work points out the possibility of systematic and predictive modification of the excited-state kinetics of vibration-cavity polariton systems.

journal_name

Nat Commun

journal_title

Nature communications

authors

Dunkelberger AD,Spann BT,Fears KP,Simpkins BS,Owrutsky JC

doi

10.1038/ncomms13504

subject

Has Abstract

pub_date

2016-11-22 00:00:00

pages

13504

issn

2041-1723

pii

ncomms13504

journal_volume

7

pub_type

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