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Theoretical Modeling of Plasmon-Enhanced Raman Images of a Single Molecule with Subnanometer Resolution
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology. University of Science and Technology of China, China.ORCID iD: 0000-0002-3282-0711
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-3915-300X
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.ORCID iD: 0000-0001-6994-9802
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2015 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 137, no 30, 9515-9518 p.Article in journal (Refereed) Published
Abstract [en]

Under local plasmonic excitation, Raman images of single molecules can now surprisingly reach subnanometer resolution. However, its physical origin has not been fully understood. Here we report a quantum-mechanical description of the interaction between a molecule and a highly confined plasmonic field. We show that When the spatial distribution of the plasmonic field is comparable to the size of the molecule, the optical transition matrix of the molecule becomes dependent on the position and distribution of the plasmonic field, resulting in a spatially resolved high-resolution Raman image of the molecule. The resonant Raman image reflects the electronic transition density of the molecule. In combination with first-principles calculations, the simulated Raman linage of a porphyrin derivative adsorbed on a silver surface nicely reproduces its experimental counterpart. The present theory provides the basic framework for describing linear and nonlinear responses of molecules under highly confined plasmonic fields.

Place, publisher, year, edition, pages
2015. Vol. 137, no 30, 9515-9518 p.
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-173271DOI: 10.1021/jacs.5b03741ISI: 000359279500004PubMedID: 26186284Scopus ID: 2-s2.0-84938875995OAI: oai:DiVA.org:kth-173271DiVA: diva2:852606
Note

QC 20150909

Available from: 2015-09-09 Created: 2015-09-09 Last updated: 2017-12-04Bibliographically approved

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Duan, SaiTian, GuangjunJi, YongfeiLuo, Yi

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