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A Frequency Domain Existence Proof of Single-Molecule Surface-Enhanced Raman Spectroscopy
Abstract
The existence of single-molecule surface-enhanced Raman spectroscopy (SMSERS) is proven by employing a frequency-domain approach. This is demonstrated using two isotopologues of Rhodamine 6G that offer unique vibrational signatures. When an average of one molecule was adsorbed per silver nanoparticle, only one isotopologue was typically observed under dry N2 environment. Additionally, the distribution of vibrational frequencies hidden under the ensemble average is revealed by examining the single-molecule spectra. Correlation with transmission electron microscopy reveals that SMSERS active aggregates are composed of multiple randomly sized and shaped nanoparticles. At higher coverage and in a humid environment, adsorbate interchange was detected. Using 2D cross correlation, vibrational modes from different isotopologues were anti-correlated, indicating that the dynamic behavior was from multiple molecules competing for a single hot spot. This allows hot-spot diffusion to be directly observed without analyzing the peak intensity fluctuations.
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Citations
Cites
Two‐Dimensional Correlation Spectroscopy – Applications in Vibrational and Optical Spectroscopy
Noda, I., & Ozaki, Y. (2004) · doi:10.1002/0470012404 · Cited by 1,385
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Dasary, S. S. R., Singh, A. K., Senapati, D., Yu, H., & Ray, P. C. (2009) · Journal of the American Chemical Society · doi:10.1021/ja905134d · Cited by 722
Theoretical Studies of Plasmonics using Electronic Structure Methods
Morton, S. M., Silverstein, D. W., & Jensen, L. (2011) · Chemical Reviews · doi:10.1021/cr100265f · Cited by 474
Qiao, X., Su, B., Liu, C., Song, Q., Luo, D., Mo, G., & Wang, T. (2018) · Advanced Materials · doi:10.1002/adma.201702275 · Cited by 469
Single molecule analysis by surfaced-enhanced Raman scattering
Pieczonka, N. P. W., & Aroca, R. F. (2008) · Chemical Society Reviews · doi:10.1039/b709739p · Cited by 451
Metadata
- Authors
- Dieringer, J. A., Lettan, R. B., Scheidt, K. A., & Van Duyne, R. P.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2007-12-01
- Volume
- 129
- Issue
- 51
- Pages
- 16249-16256
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2026075600
- Cited by
- 540
- References
- 1
- FWCI
- 17.95
- Type
- journal article
- Language
- en
- Open access
- closed
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