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Phys Rev Lett. 2009 Aug 7;103(6):063003. Epub 2009 Aug 5.

Ultrafast nonradiative decay rates on metallic surfaces by comparing surface-enhanced Raman and fluorescence signals of single molecules.

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  • 1The MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, New Zealand.


By the simultaneous observation of surface-enhanced Raman scattering and surface-enhanced fluorescence signals from a single molecule, we can measure and quantify the modification of the total decay rate of emitters in very close proximity to metals, even down to adsorbed molecules. This modified decay rate is shown to be largely dominated by its nonradiative component, which would be extremely difficult to estimate with conventional approaches. The method provides an indirect measurement of ultrafast (approximately 25 fs) mechanisms, which would be impossible to gain with time-resolved spectroscopy of a single molecule.

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