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dc.contributor.authorGriffiths, Jack
dc.contributor.authorFöldes, Tamás
dc.contributor.authorde Nijs, Bart
dc.contributor.authorChikkaraddy, Rohit
dc.contributor.authorWright, Demelza
dc.contributor.authorDeacon, William M
dc.contributor.authorBerta, Dénes
dc.contributor.authorReadman, Charlie
dc.contributor.authorGrys, David
dc.contributor.authorRosta, Edina
dc.contributor.authorBaumberg, Jeremy
dc.date.accessioned2021-10-28T23:30:43Z
dc.date.available2021-10-28T23:30:43Z
dc.date.issued2021-11-19
dc.identifier.issn2041-1723
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/330017
dc.description.abstractMetal/organic-molecule interactions underpin many key chemistries but occur on sub-nm scales where nanoscale visualisation techniques tend to average over heterogeneous distributions. Single molecule imaging techniques at the atomic scale have found it challenging to track chemical behaviour under ambient conditions. Surface-enhanced Raman spectroscopy can optically monitor the vibrations of single molecules but understanding is limited by the complexity of spectra and mismatch between theory and experiment. We demonstrate that spectra from an optically generated metallic adatom near a molecule of interest can be inverted into dynamic sub-Å metal-molecule interactions using a comprehensive model, revealing anomalous diffusion of a single atom. Transient metal-organic coordination bonds chemically perturb molecular functional groups > 10 bonds away. With continuous improvements in computational methods for modelling large and complex molecular systems, this technique will become increasingly applicable to accurately tracking more complex chemistries.
dc.description.sponsorshipWe acknowledge financial support from EPSRC grant EP/G060649/1, EP/L027151/1, EP/G037221/1, EP/R013012/1, EPSRC NanoDTC, and EU grant THOR 829067 and ERC starting grant BioNet 757850. B.d.N. acknowledges support from the Leverhulme Trust and Isaac Newton Trust. We acknowledge use of the Rosalind computing facility at King’s College London. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC 397 (EP/P020194/1).
dc.languageeng
dc.publisherSpringer Science and Business Media LLC
dc.rightsAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.titleResolving sub-angstrom ambient motion through reconstruction from vibrational spectra.
dc.typeArticle
prism.issueIdentifier1
prism.publicationDate2021
prism.publicationNameNat Commun
prism.startingPage6759
prism.volume12
dc.identifier.doi10.17863/CAM.77461
dcterms.dateAccepted2021-10-27
rioxxterms.versionofrecord10.1038/s41467-021-26898-1
rioxxterms.versionVoR
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.licenseref.startdate2021-11-19
dc.contributor.orcidde Nijs, Bart [0000-0002-8234-723X]
dc.contributor.orcidChikkaraddy, Rohit [0000-0002-3840-4188]
dc.contributor.orcidGrys, David [0000-0002-4038-6388]
dc.contributor.orcidBaumberg, Jeremy [0000-0002-9606-9488]
dc.identifier.eissn2041-1723
rioxxterms.typeJournal Article/Review
pubs.funder-project-idIsaac Newton Trust (18.08(K))
pubs.funder-project-idLeverhulme Trust (ECF-2018-021)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/G060649/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L027151/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/G037221/1)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (829067)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/R020965/1)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) Research Infrastructures (RI) (861950)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) ERC (883703)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L015978/1)
cam.issuedOnline2021-11-19
datacite.issupplementedby.urlhttps://doi.org/10.17863/CAM.76655
cam.orpheus.successTue Feb 01 19:02:06 GMT 2022 - Embargo updated*
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Attribution 4.0 International
Except where otherwise noted, this item's licence is described as Attribution 4.0 International