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Negligible Effect of Vibrational Polaritons on Chemical Reaction Rates via the Density of States Pathway
- Source :
- The journal of physical chemistry letters. 11(9)
- Publication Year :
- 2020
-
Abstract
- We show that the polariton density of states in planar optical cavities strongly coupled to vibrational excitations remains much lower than the density of vibrational states even at the frequency of the lower and upper polaritons under most practical circumstances. The polariton density of states is higher within a narrow window only when the inhomogeneous line width is at least an order of magnitude smaller than the Rabi splitting. Therefore, modification of reaction rates via the density-of-states pathway appears small or negligible for the scenarios reported in the literature. While the polariton density of states is bounded from above by the free-space optical density of states in dielectric cavities, it can be much higher for localized phonon polariton modes of nanoscale particles. We conclude that other potential explanations of the reported reactivity changes under vibrational strong coupling should be examined.
- Subjects :
- Physics
Strongly coupled
Physics::Optics
02 engineering and technology
010402 general chemistry
021001 nanoscience & nanotechnology
01 natural sciences
Molecular physics
Chemical reaction
0104 chemical sciences
Planar
Physics::Atomic and Molecular Clusters
Density of states
Polariton
General Materials Science
Physics::Chemical Physics
Physical and Theoretical Chemistry
0210 nano-technology
Subjects
Details
- ISSN :
- 19487185
- Volume :
- 11
- Issue :
- 9
- Database :
- OpenAIRE
- Journal :
- The journal of physical chemistry letters
- Accession number :
- edsair.doi.dedup.....55aef5846cedc94ede8b6e240983d3b7