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Title: The information content in single-molecule Raman nanoscopy

Abstract

Nowadays, it is possible to establish the chemical identity of a substance at the ultimate detection limit of a single molecule, i.e. the sensitivity required to probe 1.66 yoctomoles (1/NA), using surface-enhanced Raman scattering (SERS). It is also possible to image within an individual molecule, all while retaining chemical selectivity, using tip-enhanced Raman scattering (TERS). The potential applications of ultrasensitive SERS and TERS in chemical and biological detection and imaging are evident, and have attracted significant attention over the past decade. Rather than focusing on conventional single/few-molecule SERS and TERS experiments, where the objective is ultrasensitive spectroscopy and nanoscale chemical imaging, we consider the reverse problem herein. Namely, we review recent efforts ultimately aimed at probing different aspects of a molecule’s local environment through a detailed analysis of its SERS and TERS signatures. Particular attention is devoted to local electric field imaging using TERS; we describe how the vector components and absolute magnitude of a local electric field may be inferred from molecular Raman spectra and images. We also propose experiments that can potentially be used to cross-check the insights gained from the described SERS and TERS measurements. The ultimate goal of this review is to demonstrate that there ismore » much more to single molecule Raman scattering than mere ultrasensitive chemical nanoscopy.« less

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1337226
Report Number(s):
PNNL-SA-114470
Journal ID: ISSN 2374-6149; 49123; KC0301050
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Advances in Physics: X
Additional Journal Information:
Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2374-6149
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

El-Khoury, Patrick Z., Abellan, Patricia, Chantry, Ruth L., Gong, Yu, Joly, Alan G., Novikova, Irina V., Evans, James E., Aprà, Edoardo, Hu, Dehong, Ramasse, Quentin M., and Hess, Wayne P. The information content in single-molecule Raman nanoscopy. United States: N. p., 2016. Web. doi:10.1080/23746149.2016.1140010.
El-Khoury, Patrick Z., Abellan, Patricia, Chantry, Ruth L., Gong, Yu, Joly, Alan G., Novikova, Irina V., Evans, James E., Aprà, Edoardo, Hu, Dehong, Ramasse, Quentin M., & Hess, Wayne P. The information content in single-molecule Raman nanoscopy. United States. https://doi.org/10.1080/23746149.2016.1140010
El-Khoury, Patrick Z., Abellan, Patricia, Chantry, Ruth L., Gong, Yu, Joly, Alan G., Novikova, Irina V., Evans, James E., Aprà, Edoardo, Hu, Dehong, Ramasse, Quentin M., and Hess, Wayne P. 2016. "The information content in single-molecule Raman nanoscopy". United States. https://doi.org/10.1080/23746149.2016.1140010.
@article{osti_1337226,
title = {The information content in single-molecule Raman nanoscopy},
author = {El-Khoury, Patrick Z. and Abellan, Patricia and Chantry, Ruth L. and Gong, Yu and Joly, Alan G. and Novikova, Irina V. and Evans, James E. and Aprà, Edoardo and Hu, Dehong and Ramasse, Quentin M. and Hess, Wayne P.},
abstractNote = {Nowadays, it is possible to establish the chemical identity of a substance at the ultimate detection limit of a single molecule, i.e. the sensitivity required to probe 1.66 yoctomoles (1/NA), using surface-enhanced Raman scattering (SERS). It is also possible to image within an individual molecule, all while retaining chemical selectivity, using tip-enhanced Raman scattering (TERS). The potential applications of ultrasensitive SERS and TERS in chemical and biological detection and imaging are evident, and have attracted significant attention over the past decade. Rather than focusing on conventional single/few-molecule SERS and TERS experiments, where the objective is ultrasensitive spectroscopy and nanoscale chemical imaging, we consider the reverse problem herein. Namely, we review recent efforts ultimately aimed at probing different aspects of a molecule’s local environment through a detailed analysis of its SERS and TERS signatures. Particular attention is devoted to local electric field imaging using TERS; we describe how the vector components and absolute magnitude of a local electric field may be inferred from molecular Raman spectra and images. We also propose experiments that can potentially be used to cross-check the insights gained from the described SERS and TERS measurements. The ultimate goal of this review is to demonstrate that there is much more to single molecule Raman scattering than mere ultrasensitive chemical nanoscopy.},
doi = {10.1080/23746149.2016.1140010},
url = {https://www.osti.gov/biblio/1337226}, journal = {Advances in Physics: X},
issn = {2374-6149},
number = 1,
volume = 1,
place = {United States},
year = {Sat Jan 02 00:00:00 EST 2016},
month = {Sat Jan 02 00:00:00 EST 2016}
}