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Single-molecule surface-enhanced Raman spectroscopy with nanowatt excitation.

Brendan L Darby1, Pablo G Etchegoin, Eric C Le Ru

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Single-molecule surface-enhanced Raman spectroscopy (SM-SERS) detection is achievable with ultra-low laser powers and in unaggregated silver colloids. This finding suggests SM-SERS is more common than previously assumed, especially under resonance conditions.

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Area of Science:

  • Analytical Chemistry
  • Spectroscopy
  • Nanotechnology

Background:

  • Surface-Enhanced Raman Spectroscopy (SERS) is a powerful technique for detecting molecules at low concentrations.
  • Achieving single-molecule detection (SM-SERS) is often considered challenging, requiring specific conditions and high-quality substrates.
  • Resonance Raman excitation is known to enhance signal intensity.

Purpose of the Study:

  • To demonstrate the feasibility of SM-SERS under non-ideal conditions: ultra-low excitation power and as-synthesized colloidal solutions.
  • To re-evaluate the common assumption that SM-SERS detection implies superior SERS substrate performance.
  • To highlight the significant role of resonance Raman excitation in facilitating SM-SERS.

Main Methods:

  • Utilized the bi-analyte method with a methylated Rhodamine 6G and its isotopologue.
  • Employed ultra-low excitation powers (nanowatt range) at 514 nm, close to the electronic resonance of the analytes.
  • Used as-synthesized, not deliberately aggregated, silver colloid solutions as the SERS substrate.

Main Results:

  • Successfully achieved single-molecule detection (SM-SERS) even with excitation powers as low as nanowatts.
  • Demonstrated SM-SERS in a simple, unaggregated silver colloid solution, challenging previous notions.
  • Observed that resonance Raman excitation significantly facilitates SM-SERS, making it more accessible.

Conclusions:

  • Single-molecule SERS detection is more readily achievable than commonly believed, particularly when using resonance Raman excitation.
  • The occurrence of SM-SERS in challenging conditions (low power, unaggregated colloids) should not automatically be interpreted as evidence of exceptional SERS substrate quality.
  • This study provides a more nuanced understanding of the factors influencing SM-SERS, emphasizing the importance of excitation conditions.