Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 38, Pages 11462-11466Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201605504
Keywords
IR spectroscopy; kinetics; strong coupling; thermodynamics; vibrations
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Funding
- International Center for Frontier Research in Chemistry (icFRC, Strasbourg)
- ANR Equipex Union [ANR-10-EQPX-52-01]
- Labex NIE projects [ANR-11-LABX-0058 NIE]
- CSC [ANR-10-LABX-0026 CSC]
- USIAS within the Investissement d'Avenir program [ANR-10-IDEX-0002-02]
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The ground-state deprotection of a simple alkynylsilane is studied under vibrational strong coupling to the zero-point fluctuations, or vacuum electromagnetic field, of a resonant IR microfluidic cavity. The reaction rate decreased by a factor of up to 5.5 when the Si-C vibrational stretching modes of the reactant were strongly coupled. The relative change in the reaction rate under strong coupling depends on the Rabi splitting energy. Product analysis by GC-MS confirmed the kinetic results. Temperature dependence shows that the activation enthalpy and entropy change significantly, suggesting that the transition state is modified from an associative to a dissociative type. These findings show that vibrational strong coupling provides a powerful approach for modifying and controlling chemical landscapes and for understanding reaction mechanisms.
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