Theorie der thermisch aktivierten polaritonischen chemischen Prozesse
Theoretische Chemie: Moleküle, Materialien, Oberflächen
Zusammenfassung der Projektergebnisse
Over the past decade, researchers have been exploring the modification of chemical reactions through strong coupling to electromagnetic modes, particularly in resonant cavities. The primary aim of this project was to theoretically understand the microscopic mechanisms governing the alteration of thermal chemistry and the mechanisms of energy redistribution in these resonant cavities, particularly those resonant with infrared (IR) vibrational modes. The outcomes of the project touched on various theoretical aspects, such as Fermi resonances enabled by cavities, transient absorption spectroscopy, and cavity-induced isomerization rate modifications. Important advancements in the field stemming from this project involved the precise characterization and understanding of the modification of recrossing coefficients and dynamical and collective effects in cavity-modified reactivity on the basis of realistic, ab initio modelling of an isomerization reaction. Several papers in reputed physical chemistry journals were published on the results of our investigations. While experimental challenges persist due to the complexity of the condensed phase in connection with the cavity environment, there is potential for significant advancements in newly reported gas-phase experiments, and this could represent the conceptual basis for a follow-up project in the near future. The results of the this project are of fundamental nature and contributed to deepening our understanding molecular interactions in complex electromagnetic environments.
Projektbezogene Publikationen (Auswahl)
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Many-photon excitation of organic molecules in a cavity—Superradiance as a measure of coherence. The Journal of Chemical Physics, 153(24).
Ulusoy, Inga S.; Gomez, Johana A. & Vendrell, Oriol
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Suppression and Enhancement of Thermal Chemical Rates in a Cavity. The Journal of Physical Chemistry Letters, 13(20), 4441-4446.
Sun, Jing & Vendrell, Oriol
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Classical description of cavity-controlled reactivity and fermionic quantum dynamics. Doctoral thesis, Heidelberg University 2023
Jing Sun
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Modification of Thermal Chemical Rates in a Cavity via Resonant Effects in the Collective Regime. The Journal of Physical Chemistry Letters, 14(38), 8397-8404.
Sun, Jing & Vendrell, Oriol
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Vibrational Energy Redistribution and Polaritonic Fermi Resonances in the Strong Coupling Regime. The Journal of Physical Chemistry A, 127(7), 1598-1608.
Gómez, Johana A. & Vendrell, Oriol
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Quantum dynamics of polaritons in vibrational strong coupling: new polaritondriven intramolecular energy redistribution pathways, Doctoral thesis, Heidelberg University 2024
Johana Alexandra Gomez
