Abstract:
:Interaction between light and matter results in new quantum states whose energetics can modify chemical kinetics. In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number [Formula: see text] of molecular transitions couple to each resonant cavity mode, yielding two hybrid light-matter (polariton) modes and a reservoir of [Formula: see text] dark states whose chemical dynamics are essentially those of the bare molecules. This fact is seemingly in opposition to the recently reported modification of thermally activated ground electronic state reactions under VSC. Here we provide a VSC Marcus-Levich-Jortner electron transfer model that potentially addresses this paradox: although entropy favors the transit through dark-state channels, the chemical kinetics can be dictated by a few polaritonic channels with smaller activation energies. The effects of catalytic VSC are maximal at light-matter resonance, in agreement with experimental observations.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Campos-Gonzalez-Angulo JA,Ribeiro RF,Yuen-Zhou Jdoi
10.1038/s41467-019-12636-1subject
Has Abstractpub_date
2019-10-15 00:00:00pages
4685issue
1issn
2041-1723pii
10.1038/s41467-019-12636-1journal_volume
10pub_type
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