Understanding the Surface-Enhanced Raman Spectroscopy 'Background'

S. Mahajan, R.M. Cole, J.D. Speed, S.H. Pelfrey, Ashley Hilary RUSSELL, P.N. Bartlett, S.M. Barnett, J.J. Baumberg

Research output: Contribution to journalArticle

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Abstract

Even 35 years after the discovery of surface-enhanced Raman spectroscopy (SERS) much remains to be learned about the phenomenon.(1-3) Despite broad consensus on the mechanism of SERS, many features remain poorly understood and in particular much less effort has been put into understanding the continuum emission called the 'background' observed in SERS spectra. Here the SERS background is studied systematically on sphere segment void (SSV) plasmonic substrates. We establish the physicochemical dependence of the background on plasmons, the identity of the adsorbate, adsorbate coverage and electrochemical potential. In particular, by exchanging electron-donating and electron-withdrawing adsorbates, we demonstrate predictable modulation of the SERS background. Using these observations, we propose a model for the origin of the SERS background. Finally, we test the proposed model against its predictions for anti-Stokes SERS spectra.
Original languageEnglish
Pages (from-to)7242-7250
Number of pages8
JournalJournal of Physical Chemistry C
Volume114
Issue number16
DOIs
Publication statusPublished - 2009

Fingerprint

Raman spectroscopy
Adsorbates
Plasmons
exchanging
Electrons
plasmons
voids
electrons
Modulation
continuums
modulation
Substrates
predictions

Keywords

  • raman spectroscopy

Cite this

Mahajan, S., Cole, R. M., Speed, J. D., Pelfrey, S. H., RUSSELL, A. H., Bartlett, P. N., ... Baumberg, J. J. (2009). Understanding the Surface-Enhanced Raman Spectroscopy 'Background'. Journal of Physical Chemistry C, 114(16), 7242-7250. https://doi.org/10.1021/jp907197b
Mahajan, S. ; Cole, R.M. ; Speed, J.D. ; Pelfrey, S.H. ; RUSSELL, Ashley Hilary ; Bartlett, P.N. ; Barnett, S.M. ; Baumberg, J.J. / Understanding the Surface-Enhanced Raman Spectroscopy 'Background'. In: Journal of Physical Chemistry C. 2009 ; Vol. 114, No. 16. pp. 7242-7250.
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Mahajan, S, Cole, RM, Speed, JD, Pelfrey, SH, RUSSELL, AH, Bartlett, PN, Barnett, SM & Baumberg, JJ 2009, 'Understanding the Surface-Enhanced Raman Spectroscopy 'Background'', Journal of Physical Chemistry C, vol. 114, no. 16, pp. 7242-7250. https://doi.org/10.1021/jp907197b

Understanding the Surface-Enhanced Raman Spectroscopy 'Background'. / Mahajan, S.; Cole, R.M.; Speed, J.D.; Pelfrey, S.H.; RUSSELL, Ashley Hilary; Bartlett, P.N.; Barnett, S.M.; Baumberg, J.J.

In: Journal of Physical Chemistry C, Vol. 114, No. 16, 2009, p. 7242-7250.

Research output: Contribution to journalArticle

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AU - RUSSELL, Ashley Hilary

AU - Bartlett, P.N.

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AB - Even 35 years after the discovery of surface-enhanced Raman spectroscopy (SERS) much remains to be learned about the phenomenon.(1-3) Despite broad consensus on the mechanism of SERS, many features remain poorly understood and in particular much less effort has been put into understanding the continuum emission called the 'background' observed in SERS spectra. Here the SERS background is studied systematically on sphere segment void (SSV) plasmonic substrates. We establish the physicochemical dependence of the background on plasmons, the identity of the adsorbate, adsorbate coverage and electrochemical potential. In particular, by exchanging electron-donating and electron-withdrawing adsorbates, we demonstrate predictable modulation of the SERS background. Using these observations, we propose a model for the origin of the SERS background. Finally, we test the proposed model against its predictions for anti-Stokes SERS spectra.

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Mahajan S, Cole RM, Speed JD, Pelfrey SH, RUSSELL AH, Bartlett PN et al. Understanding the Surface-Enhanced Raman Spectroscopy 'Background'. Journal of Physical Chemistry C. 2009;114(16):7242-7250. https://doi.org/10.1021/jp907197b