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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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Cites
Two‐Dimensional Correlation Spectroscopy – Applications in Vibrational and Optical Spectroscopy
Noda, I., & Ozaki, Y. (2004) · doi:10.1002/0470012404 · Cited by 1,385
Cited by
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Yang, X., Yang, M., Pang, B., Vara, M., & Xia, Y. (2015) · Chemical Reviews · doi:10.1021/acs.chemrev.5b00193 · Cited by 1,162
SERS Nanoparticles in Medicine: From Label-Free Detection to Spectroscopic Tagging
Lane, L. A., Qian, X., & Nie, S. (2015) · Chemical Reviews · doi:10.1021/acs.chemrev.5b00265 · Cited by 873
Creating, characterizing, and controlling chemistry with SERS hot spots
Kleinman, S. L., Frontiera, R. R., Henry, A.-I., Dieringer, J. A., & Van Duyne, R. P. (2013) · Phys. Chem. Chem. Phys. · doi:10.1039/c2cp42598j · Cited by 733
Self-citationDasary, 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
Large-Scale Hot Spot Engineering for Quantitative SERS at the Single-Molecule Scale
Chen, H.-Y., Lin, M.-H., Wang, C.-Y., Chang, Y.-M., & Gwo, S. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b09111 · Cited by 426
Stimulated Raman Scattering: From Bulk to Nano
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Tip‐Enhanced Near‐Field Optical Microscopy
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Surface-enhanced Raman spectroscopy at single-molecule scale and its implications in biology
Wang, Y., & Irudayaraj, J. (2013) · Philosophical Transactions of the Royal Society B: Biological Sciences · doi:10.1098/rstb.2012.0026 · Cited by 125
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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