On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap

Bao-Qin Chen; Chao Zhang; Jiafang Li; Zhi-Yuan Li; Younan Xia

doi:10.1039/C6NR04574J

On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap

Bao-Qin Chen,^ab Chao Zhang,^b Jiafang Li,^b Zhi-Yuan Li*^ab and Younan Xia^c

Author affiliations

* Corresponding authors

^a College of Physics and Optoelectronics, South China University of Technology, Guangzhou 510640, China

^b Laboratory of Optical Physics, Institute of Physics, Chinese Academy of Sciences, P. O. Box 603, Beijing 100190, China
E-mail: lizy@aphy.iphy.ac.cn

^c The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, and School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA 30332, USA

Abstract

Electromagnetic and chemical enhancement mechanisms are commonly used to account for single-molecule surface-enhanced Raman scattering (SM-SERS). Due to many practical limitations, however, the overall enhancement factor summed up from these two mechanisms is typically 5–6 orders of magnitude below the level of 10¹⁴–10¹⁵ required for SM-SERS. Here, we demonstrate that the multiple elastic Rayleigh scattering of a molecule could play a critical role in further enhancing the Raman signal, when the molecule is trapped in a 2 nm gap between two Ag nanoparticles, pushing the overall enhancement factor close to the level needed for SM-SERS. As a universal physical process for all molecules interacting with light, we believe that Rayleigh scattering plays a pivotal and as yet unrecognized role in SERS, in particular, for enabling single-molecule sensitivity.

Article information

https://doi.org/10.1039/C6NR04574J

Article type

Paper

Submitted

06 Jun 2016

Accepted

30 Jul 2016

First published

02 Aug 2016

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Nanoscale, 2016,8, 15730-15736

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On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap

B. Chen, C. Zhang, J. Li, Z. Li and Y. Xia, Nanoscale, 2016, 8, 15730 DOI: 10.1039/C6NR04574J

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On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap

Abstract

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On the critical role of Rayleigh scattering in single-molecule surface-enhanced Raman scattering via a plasmonic nanogap

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