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Molecular orbital theory in cavity QED environments

Author

Listed:
  • Rosario R. Riso

    (Norwegian University of Science and Technology)

  • Tor S. Haugland

    (Norwegian University of Science and Technology)

  • Enrico Ronca

    (Istituto per i Processi Chimico Fisici del CNR (IPCF-CNR))

  • Henrik Koch

    (Norwegian University of Science and Technology
    Scuola Normale Superiore)

Abstract

Coupling between molecules and vacuum photon fields inside an optical cavity has proven to be an effective way to engineer molecular properties, in particular reactivity. To ease the rationalization of cavity induced effects we introduce an ab initio method leading to the first fully consistent molecular orbital theory for quantum electrodynamics environments. Our framework is non-perturbative and explains modifications of the electronic structure due to the interaction with the photon field. In this work, we show that the newly developed orbital theory can be used to predict cavity induced modifications of molecular reactivity and pinpoint classes of systems with significant cavity effects. We also investigate electronic cavity-induced modifications of reaction mechanisms in vibrational strong coupling regimes.

Suggested Citation

  • Rosario R. Riso & Tor S. Haugland & Enrico Ronca & Henrik Koch, 2022. "Molecular orbital theory in cavity QED environments," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29003-2
    DOI: 10.1038/s41467-022-29003-2
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    References listed on IDEAS

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    2. A. Shalabney & J. George & J. Hutchison & G. Pupillo & C. Genet & T. W. Ebbesen, 2015. "Coherent coupling of molecular resonators with a microcavity mode," Nature Communications, Nature, vol. 6(1), pages 1-6, May.
    3. Rohit Chikkaraddy & Bart de Nijs & Felix Benz & Steven J. Barrow & Oren A. Scherman & Edina Rosta & Angela Demetriadou & Peter Fox & Ortwin Hess & Jeremy J. Baumberg, 2016. "Single-molecule strong coupling at room temperature in plasmonic nanocavities," Nature, Nature, vol. 535(7610), pages 127-130, July.
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