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Article Abstract
We propose polarization-selective Raman measurement as a decent method for single-molecule surface-enhanced Raman scattering (SMSERS) verification. This approach features rapid acquisition of SMSERS events and appeals liberal requirements for analyte concentration. It is demonstrated as an efficient tool in sorting out dozens of SMSERS events from a large-scale plasmonic dimer array. In addition, it allows identification of a mixed SMSERS event containing two different individual molecules. In this article, the RPM method is employed to explore the underlying mechanisms of signal blinking, spectral wandering, and other unique characteristics in SMSERS. We observed synchronized blinking of different modes from one Rhodamine 6G (R6G) molecule, but a disagreement is found in a mixed SMSERS event containing one R6G molecule and one crystal violet molecule. Our approach offers a reliable means to interpret SMSERS events in statistical terms and facilitate the fundamental understanding of SMSERS.
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Single-Molecule Surface-Enhanced Raman Spectroscopy.
Sensors (Basel)
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State Key Laboratory of Modern Optical Instrumentation, College of Optical Science & Engineering, Zhejiang University, Hangzhou 310027, China.
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Anal Chem
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Institute for Integrative Nanosciences, Leibniz IFW, Helmholtzstraße 20, Dresden 01069, Germany.
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Department of Chemistry , Seoul National University, Seoul 08826 , Korea.
The initial observations of surface-enhanced Raman scattering (SERS) from individual molecules (single-molecule SERS, SMSERS) have triggered ever more detailed mechanistic studies on the SERS process. The studies not only reveal the existence of extremely enhanced and confined fields at the gaps of Ag or Au nanoparticles but also reveal that the spatial, spectral, and temporal behaviors of the SMSERS signal critically depend on many factors, including plasmon resonances of nanostructures, diffusion (lateral and orientational) of molecules, molecular electronic resonances, and metal-molecule charge transfers. SMSERS spectra, with their , should in principle provide molecule-specific information on individual molecules in a way that any other existing single-molecule detection method (such as the ones based on fluorescence, mechanical forces, or electrical currents) cannot.
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Anal Chem
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Department of Chemistry, University of Victoria, Victoria, British Columbia V8P 5C2, Canada.
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