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Observation and Analysis of Blinking Surface-enhanced Raman Scattering

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Published on: January 11, 2018

High-Speed Spectral Characterization of Single-Molecule SERS Fluctuations.

Makayla M Schmidt¹, Emily A Farley¹, Marit A Engevik¹

¹Department of Physics and Engineering, Bethel University, 3900 Bethel Drive, St. Paul, Minnesota 55112, United States.

|March 23, 2023

Summary

Plasmonic hotspots in surface-enhanced Raman scattering (SERS) exhibit dynamic fluctuations. High-speed SERS analysis reveals these transient hotspots influence spectral signals across various timescales, impacting single-molecule detection.

Keywords:

High-Speed Fluctuations High-Speed Spectroscopy Plasmonic Hotspots Single Molecule SERS Surface Enhanced Raman Spectroscopy (SERS)

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Area of Science:

Nanophotonics
Surface-Enhanced Raman Scattering (SERS)
Single-Molecule Spectroscopy

Background:

Plasmonic hotspots significantly enhance Raman scattering efficiency in SERS.
Single-molecule SERS signals exhibit fluctuations, questioning the static nature of hotspots.
Fluctuations occur across a wide range of timescales, from seconds to microseconds.

Purpose of the Study:

Investigate the dynamic nature of plasmonic hotspots.
Understand the origins of SERS intensity fluctuations (SIFs) at high speeds.
Characterize SERS signals with microsecond time resolution.

Main Methods:

Developed a high-speed acquisition system capturing 100,000 SERS spectra per second.
Analyzed SERS spectra with microsecond time resolution.
Studied SERS intensity fluctuations (SIFs) across spectral ranges.

Main Results:

SIF events enhance different spectral regions over 10s to 100s of microseconds.
SIF events do not favor specific spectral regions, occurring equally on Stokes and anti-Stokes sides.
Observed anomalously large anti-Stokes peaks due to transient hotspots.

Conclusions:

SIFs are driven by both temporal and spectral transient hotspots.
High-speed SERS is crucial for understanding nanoscale light-matter dynamics.
Dynamic hotspot behavior is key to SERS signal fluctuations.