Resolving sub-angstrom ambient motion through reconstruction from vibrational spectra

Jack Griffiths, Tamás Földes, Bart Nijs (), Rohit Chikkaraddy, Demelza Wright, William M. Deacon, Dénes Berta, Charlie Readman, David-Benjamin Grys, Edina Rosta and Jeremy J. Baumberg ()
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Jack Griffiths: University of Cambridge
Tamás Földes: King’s College London
Bart Nijs: University of Cambridge
Rohit Chikkaraddy: University of Cambridge
Demelza Wright: University of Cambridge
William M. Deacon: University of Cambridge
Dénes Berta: King’s College London
Charlie Readman: University of Cambridge
David-Benjamin Grys: University of Cambridge
Edina Rosta: King’s College London
Jeremy J. Baumberg: University of Cambridge

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Metal/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.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26898-1

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DOI: 10.1038/s41467-021-26898-1

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