ArticleProceedings of the National Academy of Sciences of the United States of America2019
Modification of excitation and charge transfer in cavity quantum-electrodynamical chemistry.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2019. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 45 papers.
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45 citing papers in PubMed.
- Polaritonic Spectra of Optical Mie Voids.Nanophotonics (Berlin, Germany) · 2026Article
- Quantum-Electrodynamical Time-Dependent Density Functional Theory Description of Molecules in Optical Cavities.Journal of chemical theory and computation · 2026Article
- Efficient and tunable photochemical charge transfer via long-lived Bloch surface wave polaritons.Nature nanotechnology · 2025Article
- Cavity-mediated electron-electron interactions: Renormalizing Dirac states in graphene.Science advances · 2025Article
- Excited State Dynamics of COJournal of the American Chemical Society · 2025Article
- Van der Waals Photodetector with an Integrated WSACS photonics · 2025Article
- Polariton mediated electron transfer under the collective molecule-cavity coupling regime.Chemical science · 2025Article
- Nonadiabatic Field: A Conceptually Novel Approach for Nonadiabatic Quantum Molecular Dynamics.Journal of chemical theory and computation · 2025Review
- Global Spectral Analysis of Polaritonic Coupling of Multiple Organic Dyes to a Tunable Fabry-Pérot Resonator Operating with Mirror Separations up to 10 μm.Chemistry (Weinheim an der Bergstrasse, Germany) · 2025Article
- Cavity-enhanced energy transport in molecular systems.Nature materials · 2025Review
- Controlling Plasmonic Catalysis via Strong Coupling with Electromagnetic Resonators.Nano letters · 2024Article
- Enhancement of the internal quantum efficiency in strongly coupled P3HT-CNanophotonics (Berlin, Germany) · 2024Article
- Machine Learning for Polaritonic Chemistry: Accessing Chemical Kinetics.Journal of the American Chemical Society · 2024Article
- Plasmon mediated coherent population oscillations in molecular aggregates.Nature communications · 2023Article
- Cavity-Modified Chemiluminescent Reaction of Dioxetane.The journal of physical chemistry. A · 2023Article
- Understanding Polaritonic Chemistry from Ab Initio Quantum Electrodynamics.Chemical reviews · 2023Review
- The Rise and Current Status of Polaritonic Photochemistry and Photophysics.Chemical reviews · 2023Review
- Theory for Cavity-Modified Ground-State Reactivities via Electron-Photon Interactions.The journal of physical chemistry. A · 2023Article
- Theoretical Analysis of Exciton Wave Packet Dynamics in Polaritonic Wires.The journal of physical chemistry letters · 2023Article
- Chiral Polaritonics: Analytical Solutions, Intuition, and Use.The journal of physical chemistry letters · 2023Article
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Abstract
Energy transfer in terms of excitation or charge is one of the most basic processes in nature, and understanding and controlling them is one of the major challenges of modern quantum chemistry. In this work, we highlight that these processes as well as other chemical properties can be drastically altered by modifying the vacuum fluctuations of the electromagnetic field in a cavity. By using a real-space formulation from first principles that keeps all of the electronic degrees of freedom in the model explicit and simulates changes in the environment by an effective photon mode, we can easily connect to well-known quantum-chemical results such as Dexter charge-transfer and Förster excitation-transfer reactions, taking into account the often-disregarded Coulomb and self-polarization interaction. We find that the photonic degrees of freedom introduce extra electron-electron correlations over large distances and that the coupling to the cavity can drastically alter the characteristic charge-transfer behavior and even selectively improve the efficiency. For excitation transfer, we find that the cavity renders the transfer more efficient, essentially distance-independent, and further different configurations of highest efficiency depending on the coherence times. For strong decoherence (short coherence times), the cavity frequency should be in between the isolated excitations of the donor and acceptor, while for weak decoherence (long coherence times), the cavity should enhance a mode that is close to resonance with either donor or acceptor. Our results highlight that changing the photonic environment can redefine chemical processes, rendering polaritonic chemistry a promising approach toward the control of chemical reactions.
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