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Super-resolution Optical Imaging of Single-Molecule SERS Hot Spots
Abstract
We present the first super-resolution optical images of single-molecule surface-enhanced Raman scattering (SM-SERS) hot spots, using super-resolution imaging as a powerful new tool for understanding the interaction between single molecules and nanoparticle hot spots. Using point spread function fitting, we map the centroid position of SM-SERS with +/-10 nm resolution, revealing a spatial relationship between the SM-SERS centroid position and the highest SERS intensity. We are also able to measure the unique position of the SM-SERS centroid relative to the centroid associated with nanoparticle photoluminescence, which allows us to speculate on the presence of multiple hot spots within a single diffraction-limited spot. These measurements allow us to follow dynamic movement of the SM-SERS centroid position over time as it samples different locations in space and explores regions larger than the expected size of a SM-SERS hot spot. We have proposed that the movement of the SERS centroid is due to diffusion of a single molecule on the surface of the nanoparticle, which leads to changes in coupling between the scattering dipole and the optical near field of the nanoparticle.
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Cites
Precise Nanometer Localization Analysis for Individual Fluorescent Probes
Thompson, R. E., Larson, D. R., & Webb, W. W. (2002) · Biophysical Journal · doi:10.1016/s0006-3495(02)75618-x · Cited by 2,320
Cited by
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Pérez-Jiménez, A. I., Lyu, D., Lu, Z., Liu, G., & Ren, B. (2020) · Chemical Science · doi:10.1039/d0sc00809e · Cited by 912
Surface-enhanced Raman spectroscopy
Han, X. X., Rodriguez, R. S., Haynes, C. L., Ozaki, Y., & Zhao, B. (2022) · Nature Reviews Methods Primers · doi:10.1038/s43586-021-00083-6 · Cited by 907
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
Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy
Zrimsek, A. B., Chiang, N., Mattei, M., Zaleski, S., McAnally, M. O., Chapman, C. T., Henry, A.-I., Schatz, G. C., & Van Duyne, R. P. (2017) · Chemical Reviews · doi:10.1021/acs.chemrev.6b00552 · Cited by 720
Fundamental understanding and applications of plasmon-enhanced Raman spectroscopy
Wang, X., Huang, S.-C., Hu, S., Yan, S., & Ren, B. (2020) · Nature Reviews Physics · doi:10.1038/s42254-020-0171-y · Cited by 689
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
Kleinman, S. L., Sharma, B., Blaber, M. G., Henry, A.-I., Valley, N., Freeman, R. G., Natan, M. J., Schatz, G. C., & Van Duyne, R. P. (2013) · Journal of the American Chemical Society · doi:10.1021/ja309300d · Cited by 353
Persistent misconceptions regarding SERS
Moskovits, M. (2013) · Physical Chemistry Chemical Physics · doi:10.1039/c2cp44030j · Cited by 295
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
- Stranahan, S. M., & Willets, K. A.
- Venue
- Nano Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2010-08-18
- Volume
- 10
- Issue
- 9
- Pages
- 3777-3784
- ISSN
- 1530-6984 (ISSN-L)
- 1530-6992
- OpenAlex
- W1989560527
- Cited by
- 317
- References
- 1
- FWCI
- 11.68
- Type
- journal article
- Language
- en
- Open access
- closed
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