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dc.contributor.author
Ansari, Imaad M.
dc.contributor.author
Heller, Eric R.
dc.contributor.author
Trenins, George
dc.contributor.author
Richardson, Jeremy
dc.date.accessioned
2022-04-07T08:50:21Z
dc.date.available
2021-09-11T13:06:21Z
dc.date.available
2021-09-13T04:58:20Z
dc.date.available
2021-10-15T05:51:29Z
dc.date.available
2021-11-10T07:57:47Z
dc.date.available
2022-01-13T09:25:38Z
dc.date.available
2022-02-15T08:43:25Z
dc.date.available
2022-03-18T06:23:59Z
dc.date.available
2022-04-06T14:12:08Z
dc.date.available
2022-04-07T08:50:21Z
dc.date.issued
2022-05-16
dc.identifier.issn
1364-503X
dc.identifier.issn
1471-2962
dc.identifier.other
10.1098/rsta.2020.0378
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/505272
dc.identifier.doi
10.3929/ethz-b-000505272
dc.description.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 nonadiabatic 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.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
Royal Society
en_US
dc.rights.uri
http://creativecommons.org/licenses/by/4.0/
dc.subject
Theoretical chemistry
en_US
dc.title
Instanton theory for Fermi's golden rule and beyond
en_US
dc.type
Journal Article
dc.rights.license
Creative Commons Attribution 4.0 International
dc.date.published
2022-03-28
ethz.journal.title
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences
ethz.journal.volume
380
en_US
ethz.journal.issue
2223
en_US
ethz.journal.abbreviated
Phil. Trans. R. Soc. A.
ethz.pages.start
20200378
en_US
ethz.size
28 p.; 30 p. accepted version
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.grant
Quantum Tunnelling in Molecular Systems from First Principles
en_US
ethz.identifier.wos
ethz.identifier.scopus
ethz.publication.place
London
ethz.publication.status
published
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02543 - Inst. f. Molekulare Physikalische Wiss. / Institute of Molecular Physical Science::09602 - Richardson, Jeremy / Richardson, Jeremy
ethz.tag
fourth-order rate
en_US
ethz.tag
nonadiabatic
en_US
ethz.tag
tunnelling
en_US
ethz.tag
bridge-mediated electron transfer
en_US
ethz.tag
superexchange
en_US
ethz.tag
instanton
en_US
ethz.grant.agreementno
175696
ethz.grant.agreementno
175696
ethz.grant.agreementno
175696
ethz.grant.agreementno
175696
ethz.grant.fundername
SNF
ethz.grant.fundername
SNF
ethz.grant.fundername
SNF
ethz.grant.fundername
SNF
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.program
Projekte MINT
ethz.grant.program
Projekte MINT
ethz.grant.program
Projekte MINT
ethz.grant.program
Projekte MINT
ethz.relation.isReferencedBy
10.3929/ethz-b-000612202
ethz.date.deposited
2021-09-11T13:06:26Z
ethz.source
FORM
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2022-04-07T08:50:29Z
ethz.rosetta.lastUpdated
2024-02-02T16:40:19Z
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