ArticlePhilosophical transactions. Series A, Mathematical, physical, and engineering sciences2022
Instanton theory for Fermi's golden rule and beyond.
Article in Philosophical transactions. Series A, Mathematical, physical, and engineering sciences, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 12 papers.
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12 citing papers in PubMed.
- Nuclear-Electronic Orbital General Rate Theory: Predicting Hydrogen Kinetic Isotope Effects in the Deep Tunneling Regime.Journal of chemical theory and computation · 2026Article
- Attosecond spectroscopy of molecular charge transfer uncovers a 1.5-fs delay in population transfer.Nature communications · 2025Article
- Nonadiabatic Tunneling in Chemical Reactions.The journal of physical chemistry letters · 2024Review
- Heavy-atom tunnelling in singlet oxygen deactivation predicted by instanton theory with branch-point singularities.Nature communications · 2024Article
- Unraveling the mechanisms of triplet state formation in a heavy-atom free photosensitizer.Chemical science · 2024Article
- Competing quantum effects in heavy-atom tunnelling through conical intersections.Chemical science · 2023Article
- Nonadiabatic Couplings Can Speed Up Quantum Tunneling Transition Path Times.The journal of physical chemistry letters · 2022Article
- Improved microcanonical instanton theory.Faraday discussions · 2022Article
- Heavy-Atom Quantum Tunnelling in Spin Crossovers of Nitrenes.Angewandte Chemie (International ed. in English) · 2022Article
- Transition Path Flight Times and Nonadiabatic Electronic Transitions.The journal of physical chemistry letters · 2022Article
- Fascial Nomenclature: Update 2022.Cureus · 2022Review
- Chemistry without the Born-Oppenheimer approximation.Philosophical transactions. Series A, Mathematical, physical, and engineering sciences · 2022Article
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4 authors.
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Abstract
Instanton theory provides a semiclassical approximation for computing quantum tunnelling effects in complex molecular systems. It is typically applied to proton-transfer reactions for which the Born-Oppenheimer approximation is valid. However, many processes in physics, chemistry and biology, such as electron transfers, are non-adiabatic and are correctly described instead using Fermi's golden rule. In this work, we discuss how instanton theory can be generalized to treat these reactions in the golden-rule limit. We then extend the theory to treat fourth-order processes such as bridge-mediated electron transfer and apply the method to simulate an electron moving through a model system of three coupled quantum dots. By comparison with benchmark quantum calculations, we demonstrate that the instanton results are much more reliable than alternative approximations based on superexchange-mediated effective coupling or a classical sequential mechanism. This article is part of the theme issue 'Chemistry without the Born-Oppenheimer approximation'.
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