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Volume 132, 2006
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Vibrational pumping and heating under SERS conditions: fact or myth?

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Abstract

We address in this paper the long debated issue of the possibility of vibrational pumping under Surface Enhanced Raman Scattering (SERS) conditions, both theoretically and experimentally. We revisit with simple theoretical models the mechanisms of vibrational pumping and its relation to heating. This presentation provides a clear classification of the various regimes of heating/pumping, from simple global laser heating to selective pumping of a single vibrational mode. We also propose the possibility of extreme pumping driven by stimulated phonon emission, and we introduce and apply a new experimental technique to study these effects in SERS. Our method relies on correlations between Raman peak parameters, and cross-correlation for two Raman peaks. We find strong evidence for local and dynamical heating, but no convincing evidence for selective pumping under our specific experimental SERS conditions.

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Publication details

The article was received on 18 Apr 2005, accepted on 25 May 2005 and first published on 17 Oct 2005


Article type: Paper
DOI: 10.1039/B505343A
Citation: Faraday Discuss., 2006,132, 63-75
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    Vibrational pumping and heating under SERS conditions: fact or myth?

    E. C. Le Ru and P. G. Etchegoin, Faraday Discuss., 2006, 132, 63
    DOI: 10.1039/B505343A

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