Title: Broadband surface-enhanced coherent anti-Stokes Raman spectroscopy with high spectral resolution

Abstract

Both the surface-enhanced Raman spectroscopy (SERS) and coherent anti-Stokes Raman spectroscopy (CARS) are widely used methods in the bio-sensing field for improving the intensity of Raman scattering process. By combining the mechanisms of CARS (coherence and nonlinear process) and SERS (plasmon resonance), a multiplicative enhancement can be achieved through surface-enhanced CARS (SECARS). Besides sensitivity, high specificity with wide spectral bandwidth is also preferred for bio-sensing techniques but not well developed in SECARS setups reported in the literature. A broadband SECARS setup with high sensitivity and high spectral resolution is presented. Rhodamine 6G dye molecules and several biomolecules are used as the model system to benchmark the functionality of the SECARS system in terms of its sensitivity, the lowest detectable concentration, and the spectral resolution. Our setup rendered single-molecule sensitivity with spectral resolution of <35 cm^-1. More than 10² times stronger signal-to-noise ratio compared with that of SERS is observed with the detection limit being 10^-9 m. Different from the SECARS systems in the literature, our setup employs a unique graphene-Au pyramids hybrid platform. The graphene in this structure provides additional SERS enhancement and a bio-compatible surface. Finally, this powerful technique could be instrumental in furthering the understanding of various chemicalmore » and biological processes.« less

Authors:

Yan, Zhongbo  ^[1];

• Search DOE PAGES for author "Yan, Zhongbo"
• Search DOE PAGES for ORCID "0000-0002-2270-3132"

Liu, Zirui ^[2]; Xia, Ming  ^[2];

• Search DOE PAGES for author "Xia, Ming"
• Search DOE PAGES for ORCID "0000-0001-6028-4437"

Efimov, Anatoly ^[3]; Xie, Ya-Hong ^[2]

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+ Show Author Affiliations

1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
2. Univ. of California, Los Angeles, CA (United States). Dept. of Materials Science and Engineering
3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:

Wed May 31 00:00:00 EDT 2017

Research Org.:

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, Los Angeles, CA (United States)

Sponsoring Org.:

USDOE

OSTI Identifier:

1483528

Report Number(s):

LA-UR-18-23396
Journal ID: ISSN 0377-0486

Grant/Contract Number:  

AC52-06NA25396

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Raman Spectroscopy

Additional Journal Information:

Journal Volume: 48; Journal Issue: 7; Journal ID: ISSN 0377-0486

Publisher:

Wiley

Country of Publication:

United States

Language:

English

Subject:

42 ENGINEERING; surface-enhanced coherent anti-Stokes Raman spectroscopy; graphene; Au-pyramids plasmonic substrate; broadband spectrum; spectral resolution