Variable-Temperature Tip-Enhanced Raman Spectroscopy of Single-Molecule Fluctuations and Dynamics

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  • Park, Kyoung-Duck
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
  • Muller, Eric A.
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
  • Kravtsov, Vasily
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
  • Sass, Paul M.
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
  • Dreyer, Jens
    • Other Affiliation: German Research School for Simulation Sciences; RWTH Aachen University; Forschungszentrum Jülich
  • Atkin, Joanna M.
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
  • Raschke, Markus B.
    • Other Affiliation: Department of Physics; Department of Chemistry; JILA; University of Colorado
Abstract
  • Structure, dynamics, and coupling involving single-molecules determine function in catalytic, electronic or biological systems. While vibrational spectroscopy provides insight into molecular structure, rapid fluctuations blur the molecular trajectory even in single-molecule spectroscopy, analogous to spatial averaging in measuring large ensembles. To gain insight into intramolecular coupling, substrate coupling, and dynamic processes, we use tip-enhanced Raman spectroscopy (TERS) at variable and cryogenic temperatures, to slow and control the motion of a single molecule. We resolve intrinsic line widths of individual normal modes, allowing detailed and quantitative investigation of the vibrational modes. From temperature dependent line narrowing and splitting, we quantify ultrafast vibrational dephasing, intramolecular coupling, and conformational heterogeneity. Through statistical correlation analysis of fluctuations of individual modes, we observe rotational motion and spectral fluctuations of the molec...
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  • Article
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  • In Copyright
Journal title
  • Nano Letters
Journal volume
  • 16
Journal issue
  • 1
Page start
  • 479
Page end
  • 487
Language
  • English
ISSN
  • 1530-6992
  • 1530-6984

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