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Title: Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy

Abstract

Single-molecule (SM) surface-enhanced Raman spectroscopy (SERS) and tip-enhanced Raman spectroscopy (TERS) have emerged as analytical techniques for characterizing molecular systems in nanoscale environments. SERS and TERS use plasmonically enhanced Raman scattering to characterize the chemical information on single molecules. Additionally, TERS can image single molecules with subnanometer spatial resolution. Here, we cover the development and history of SERS and TERS, including the concept of SERS hot spots and the plasmonic nanostructures necessary for SM detection, the past and current methodologies for verifying SMSERS, and investigations into understanding the signal heterogeneities observed with SMSERS. Moving on to TERS, we cover tip fabrication and the physical origins of the subnanometer spatial resolution. Then, we highlight recent advances of SMSERS and TERS in fields such as electrochemistry, catalysis, and SM electronics, which all benefit from the vibrational characterization of single molecules. SMSERS and TERS provide new insights on molecular behavior that would otherwise be obscured in an ensemble-averaged measurement.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
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  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1534472
Grant/Contract Number:  
SC0001785; CHE-1414466; FG02-09ER16109; DGE-0824162
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Volume: 117; Journal Issue: 11; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Raman spectroscopy; Metal nanoparticles; Nanoparticles; Molecules; Plasmonics

Citation Formats

Zrimsek, Alyssa B., Chiang, Naihao, Mattei, Michael, Zaleski, Stephanie, McAnally, Michael O., Chapman, Craig T., Henry, Anne-Isabelle, Schatz, George C., and Van Duyne, Richard P. Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy. United States: N. p., 2016. Web. doi:10.1021/acs.chemrev.6b00552.
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Zrimsek, Alyssa B., Chiang, Naihao, Mattei, Michael, Zaleski, Stephanie, McAnally, Michael O., Chapman, Craig T., Henry, Anne-Isabelle, Schatz, George C., & Van Duyne, Richard P. Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy. United States. https://doi.org/10.1021/acs.chemrev.6b00552
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Zrimsek, Alyssa B., Chiang, Naihao, Mattei, Michael, Zaleski, Stephanie, McAnally, Michael O., Chapman, Craig T., Henry, Anne-Isabelle, Schatz, George C., and Van Duyne, Richard P. Thu . "Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy". United States. https://doi.org/10.1021/acs.chemrev.6b00552. https://www.osti.gov/servlets/purl/1534472.
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@article{osti_1534472,
title = {Single-Molecule Chemistry with Surface- and Tip-Enhanced Raman Spectroscopy},
author = {Zrimsek, Alyssa B. and Chiang, Naihao and Mattei, Michael and Zaleski, Stephanie and McAnally, Michael O. and Chapman, Craig T. and Henry, Anne-Isabelle and Schatz, George C. and Van Duyne, Richard P.},
abstractNote = {Single-molecule (SM) surface-enhanced Raman spectroscopy (SERS) and tip-enhanced Raman spectroscopy (TERS) have emerged as analytical techniques for characterizing molecular systems in nanoscale environments. SERS and TERS use plasmonically enhanced Raman scattering to characterize the chemical information on single molecules. Additionally, TERS can image single molecules with subnanometer spatial resolution. Here, we cover the development and history of SERS and TERS, including the concept of SERS hot spots and the plasmonic nanostructures necessary for SM detection, the past and current methodologies for verifying SMSERS, and investigations into understanding the signal heterogeneities observed with SMSERS. Moving on to TERS, we cover tip fabrication and the physical origins of the subnanometer spatial resolution. Then, we highlight recent advances of SMSERS and TERS in fields such as electrochemistry, catalysis, and SM electronics, which all benefit from the vibrational characterization of single molecules. SMSERS and TERS provide new insights on molecular behavior that would otherwise be obscured in an ensemble-averaged measurement.},
doi = {10.1021/acs.chemrev.6b00552},
journal = {Chemical Reviews},
number = 11,
volume = 117,
place = {United States},
year = {2016},
month = {12}
}
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https://doi.org/10.1021/acs.chemrev.6b00552
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Figures / Tables:

Figure 1 Figure 1: (A) Energy diagram showing the spectroscopic transitions involved in Rayleigh, Raman, and resonance Raman scattering. Two pathways can be found in Raman: either the scattered photon has a lower energy than the adsorbed photon (Stokes scattering) or, inversely, the scattered photon has a higher energy than the scatteredmore » photon (anti-Stokes scattering). (B) Schematic drawing (not to scale) of a plasmonic nanosphere when the electric field component of incident light induces an oscillation of the electron cloud at a frequency defined by the nanosphere size and shape, known as the localized surface plasmon resonance.« less
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Single-Molecule Surface-Enhanced (Resonance) Raman Scattering (SE(R)RS) as a Probe for Metal Colloid Aggregation State
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Single-Molecule Surface-Enhanced Raman Spectroscopy of Crystal Violet Isotopologues: Theory and Experiment
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Temperature Dependence of the Homogeneous Broadening of Resonant Raman Peaks Measured by Single-Molecule Surface-Enhanced Raman Spectroscopy
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Resonance Raman Cross-Sections and Vibronic Analysis of Rhodamine 6G from Broadband Stimulated Raman Spectroscopy
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Studying the local character of Raman features of single-walled carbon nanotubes along a bundle using TERS
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Structure and Composition of Insulin Fibril Surfaces Probed by TERS
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Chemical mapping of a single molecule by plasmon-enhanced Raman scattering
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Ultrafast Nonradiative Decay Rates on Metallic Surfaces by Comparing Surface-Enhanced Raman and Fluorescence Signals of Single Molecules
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    Plasmon-enhanced light–matter interactions and applications
    journal, April 2019

    Probing Adsorption Configurations of Small Molecules on Surfaces by Single-Molecule Tip-Enhanced Raman Spectroscopy
    journal, November 2018

    Sensitive detection of polycyclic aromatic hydrocarbons with gold colloid coupled chloride ion SERS sensor
    journal, January 2019

    • Gong, Xuegang; Liao, Xiaoyong; Li, You
    • The Analyst, Vol. 144, Issue 22
    • DOI: 10.1039/c9an01540j

    Chemical bonding mechanism in SERS effect of pyridine by CuO nanoparticles
    journal, July 2019

    • Martinez Nuñez, C. E.; Delgado‐Beleño, Y.; Rocha‐Rocha, O.
    • Journal of Raman Spectroscopy, Vol. 50, Issue 10
    • DOI: 10.1002/jrs.5643

    Probing ring contraction and decarboxylation of Rhodizonate and the influence of Cu (II) using surface‐enhanced Raman Scattering
    journal, November 2019

    • Milán‐Garcés, Erix A.; Georgopoulos, Stéfanos Leite; Barros Santos, Patrícia
    • Journal of Raman Spectroscopy, Vol. 51, Issue 2
    • DOI: 10.1002/jrs.5767

    Simple, Flexible, and Ultrastable Surface Enhanced Raman Scattering Substrate Based on Plasmonic Nanopaper Decorated with Graphene Oxide
    journal, July 2018

    • Rodríguez-Sevilla, Erika; Vázquez, Gloria Verónica; Morales-Narváez, Eden
    • Advanced Optical Materials, Vol. 6, Issue 19
    • DOI: 10.1002/adom.201800548

    Ultrasonic‐Assisted Synthesis of Highly Defined Silver Nanodimers by Self‐Assembly for Improved Surface‐Enhanced Raman Spectroscopy
    journal, January 2020

    • Zhang, Junfang; Gim, Soeun; Paris, Grigori
    • Chemistry – A European Journal, Vol. 26, Issue 6
    • DOI: 10.1002/chem.201904518

    Ultrafast Stimulated Emission Microscopy of Single Nanocrystals
    conference, January 2020

    • Piatkowski, Lukasz; Accanto, Nicolò; Calbris, Gaetan
    • CLEO: QELS_Fundamental Science, Conference on Lasers and Electro-Optics
    • DOI: 10.1364/cleo_qels.2020.fth1q.2

    Nanoscale Discrimination between Toxic and Nontoxic Protein Misfolded Oligomers with Tip-Enhanced Raman Spectroscopy
    journal, August 2018

    • D'Andrea, Cristiano; Foti, Antonino; Cottat, Maximilien
    • Small, Vol. 14, Issue 36
    • DOI: 10.1002/smll.201800890

    Toward Precision Measurement and Manipulation of Single‐Molecule Reactions by a Confined Space
    journal, March 2019

    A joint experimental and theoretical Raman study on the interactions of pyridine adsorbed on chemically pure Ag 18 clusters
    journal, June 2019

    • An, Pan; Wu, Haiming; Pembere, Anthony M. S.
    • Journal of Raman Spectroscopy, Vol. 50, Issue 10
    • DOI: 10.1002/jrs.5653

    Integrating Sub-3 nm Plasmonic Gaps into Solid-State Nanopores
    journal, December 2017

    Stimulated Raman excited fluorescence spectroscopy and imaging
    journal, April 2019

    Advances in surface-enhanced Raman spectroscopy (SERS) substrates for lipid and protein characterization: sensing and beyond
    journal, January 2018

    • Bruzas, Ian; Lum, William; Gorunmez, Zohre
    • The Analyst, Vol. 143, Issue 17
    • DOI: 10.1039/c8an00606g

    DERS substrate based on NERS-SERS interaction in integrated microfluidic detection
    journal, January 2018

    • Xiao, Cheng; Chen, Zhibin; Qin, Mengze
    • Applied Optics, Vol. 57, Issue 12
    • DOI: 10.1364/ao.57.003172

    Nano Trek Beyond: Driving Nanocars/Molecular Machines at Interfaces
    journal, April 2018

    • Ariga, Katsuhiko; Mori, Taizo; Nakanishi, Waka
    • Chemistry - An Asian Journal, Vol. 13, Issue 10
    • DOI: 10.1002/asia.201800225

    Designed Microdevices for In Vitro Diagnostics
    journal, September 2017

    Controlled dye release from a metal–organic framework: a new luminescent sensor for water
    journal, January 2020

    • Xiao, Fan; Zhang, Jun; Gan, Jiulin
    • RSC Advances, Vol. 10, Issue 5
    • DOI: 10.1039/c9ra08753b

    Amorphous Carbon Generation as a Photocatalytic Reaction on DNA-Assembled Gold and Silver Nanostructures
    text, January 2019

    Tip-enhanced Raman spectroscopy: principles, practice, and applications to nanospectroscopic imaging of 2D materials
    journal, October 2018

    Influence of Fano resonance on SERS enhancement in Fano-plasmonic oligomers
    journal, January 2019

    • Dutta, Arpan; Alam, Khairul; Nuutinen, Tarmo
    • Optics Express, Vol. 27, Issue 21
    • DOI: 10.1364/oe.27.030031

    Materials nanoarchitectonics at two-dimensional liquid interfaces
    journal, January 2019

    • Ariga, Katsuhiko; Matsumoto, Michio; Mori, Taizo
    • Beilstein Journal of Nanotechnology, Vol. 10
    • DOI: 10.3762/bjnano.10.153

    Extending surface enhanced Raman spectroscopy (SERS) of atmospheric aerosol particles to the accumulation mode (150–800 nm)
    journal, January 2018

    • Tirella, Peter N.; Craig, Rebecca L.; Tubbs, Darrell B.
    • Environmental Science: Processes & Impacts, Vol. 20, Issue 11
    • DOI: 10.1039/c8em00276b

    How surface-specific is 2nd-order non-linear spectroscopy?
    journal, December 2019

    • Sun, Shumei; Schaefer, Jan; Backus, Ellen H. G.
    • The Journal of Chemical Physics, Vol. 151, Issue 23
    • DOI: 10.1063/1.5129108

    Spectroscopic Methods Used in Implant Material Studies
    journal, January 2020

    Towards single-molecule in situ electrochemical SERS detection with disposable substrates
    journal, January 2018

    • Martín-Yerga, Daniel; Pérez-Junquera, Alejandro; González-García, María Begoña
    • Chemical Communications, Vol. 54, Issue 45
    • DOI: 10.1039/c8cc02069h

    Coherent Raman scattering with plasmonic antennas
    journal, May 2019

    Quantum description of surface-enhanced resonant Raman scattering within a hybrid-optomechanical model
    journal, October 2019

    Review—Surface-Enhanced Raman Scattering Sensors for Food Safety and Environmental Monitoring
    journal, January 2018

    • Tang, Haibin; Zhu, Chuhong; Meng, Guowen
    • Journal of The Electrochemical Society, Vol. 165, Issue 8
    • DOI: 10.1149/2.0161808jes

    Label-Free Optical Single-Molecule Micro- and Nanosensors
    journal, August 2018

    • Subramanian, Sivaraman; Wu, Hsin-Yu; Constant, Tom
    • Advanced Materials, Vol. 30, Issue 51
    • DOI: 10.1002/adma.201801246

    Lotus Seedpod Inspired SERS Substrates: A Novel Platform Consisting of 3D Sub-10 nm Annular Hot Spots for Ultrasensitive SERS Detection
    journal, April 2018

    On-demand quantitative SERS bioassays facilitated by surface-tethered ratiometric probes
    journal, January 2018

    • Zhang, Kun; Wang, Yuning; Wu, Meiling
    • Chemical Science, Vol. 9, Issue 42
    • DOI: 10.1039/c8sc03263g

    Enhancement of Single Molecule Raman Scattering using Sprouted Potato Shaped Bimetallic Nanoparticles
    journal, July 2019

    Kinetic investigation of a chemical process in single-molecule junction
    journal, January 2020

    • Hasegawa, Yusuke; Harashima, Takanori; Jono, Yuki
    • Chemical Communications, Vol. 56, Issue 2
    • DOI: 10.1039/c9cc08383a

    Surface-enhanced spectroscopy: Toward practical analysis probe
    journal, April 2018

    Amorphous Carbon Generation as a Photocatalytic Reaction on DNA-Assembled Gold and Silver Nanostructures
    journal, June 2019

    Hollow transition metal hydroxide octahedral microcages for single particle surface-enhanced Raman spectroscopy
    journal, January 2019

    • Gao, Mansha; Miao, Peng; Han, Xijiang
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 9
    • DOI: 10.1039/c9qi00579j

    Ultrafast stimulated emission microscopy of single nanocrystals
    journal, December 2019

    • Piatkowski, Lukasz; Accanto, Nicolò; Calbris, Gaëtan
    • Science, Vol. 366, Issue 6470
    • DOI: 10.1126/science.aay1821

    Fabrication of Ag–Pd concave nanocrystals through facet-selective oxidation of Ag atoms
    journal, January 2019

    Near- and far-field Raman spectroscopic studies of nanodiamond composite films deposited by coaxial arc plasma
    journal, January 2020

    • M. Ali, Ali; Deckert-Gaudig, Tanja; Egiza, Mohamed
    • Applied Physics Letters, Vol. 116, Issue 4
    • DOI: 10.1063/1.5142198

    Advanced Characterization Methods for Electrical and Sensoric Components and Devices at the Micro and Nano Scales
    journal, October 2019

    • Sheremet, Evgeniya; Meszmer, Peter; Blaudeck, Thomas
    • physica status solidi (a), Vol. 216, Issue 19
    • DOI: 10.1002/pssa.201970061

    Advanced space- and time-resolved techniques for photocatalyst studies
    journal, January 2020

    • Gao, Yuying; Nie, Wei; Wang, Xiuli
    • Chemical Communications, Vol. 56, Issue 7
    • DOI: 10.1039/c9cc07128h

    Mastering high resolution tip-enhanced Raman spectroscopy: towards a shift of perception
    journal, January 2017

    • Richard-Lacroix, Marie; Zhang, Yao; Dong, Zhenchao
    • Chemical Society Reviews, Vol. 46, Issue 13
    • DOI: 10.1039/c7cs00203c

    Surface-Enhanced Raman Scattering (SERS) in Microbiology: Illumination and Enhancement of the Microbial World
    journal, March 2018

    • Chisanga, Malama; Muhamadali, Howbeer; Ellis, David I.
    • Applied Spectroscopy, Vol. 72, Issue 7
    • DOI: 10.1177/0003702818764672

    Preparation and Use of Chemically Modified Noble Metal Nanoparticles
    journal, September 2018

    Advanced Nanoscale Approaches to Single-(Bio)entity Sensing and Imaging
    journal, October 2018

    Near-field depolarization of tip-enhanced Raman scattering by single azo-chromophores
    journal, January 2018

    • Kharintsev, Sergey S.; Gazizov, Almaz R.; Salakhov, Myakzyum Kh.
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 37
    • DOI: 10.1039/c8cp04887h

    Surface Enhanced Raman Spectroscopy for Single Molecule Protein Detection
    journal, August 2019

    • Almehmadi, Lamyaa M.; Curley, Stephanie M.; Tokranova, Natalya A.
    • Scientific Reports, Vol. 9, Issue 1
    • DOI: 10.1038/s41598-019-48650-y

    Identifying surface reaction intermediates with photoemission tomography
    journal, July 2019

    Plasmon-enhanced stimulated Raman scattering microscopy with single-molecule detection sensitivity
    journal, November 2019

    Mesoscopic and Microscopic Strategies for Engineering Plasmon-Enhanced Raman Scattering
    journal, June 2018

    Chemically Modified Silver and Gold Nanoparticles in Spectrometric Analysis
    journal, April 2019

    3D aluminum/silver hierarchical nanostructure with large areas of dense hot spots for surface‐enhanced raman scattering
    journal, October 2019

    Fermi level-tuned optics of graphene for attocoulomb-scale quantification of electron transfer at single gold nanoparticles
    journal, August 2019

    Hybrid nanostructure of SiO 2 @Si with Au-nanoparticles for surface enhanced Raman spectroscopy
    journal, January 2019

    • Yang, Huan; Li, Ben Q.; Jiang, Xinbing
    • Nanoscale, Vol. 11, Issue 28
    • DOI: 10.1039/c9nr03813b

    Multiscale modelling of photoinduced processes in composite systems
    journal, April 2019

    Spectroelectrochemical Sensing: Current Trends and Challenges
    journal, November 2018

    • Garoz‐Ruiz, Jesus; Perales‐Rondon, Juan Victor; Heras, Aranzazu
    • Electroanalysis, Vol. 31, Issue 7
    • DOI: 10.1002/elan.201900075

    Methods to probe the formation of biofilms: applications in foods and related surfaces
    journal, January 2020

    • Huang, Yating; Chakraborty, Sayak; Liang, Hong
    • Analytical Methods, Vol. 12, Issue 4
    • DOI: 10.1039/c9ay02214g

    Surface-Enhanced Raman Spectroscopy Based on a Silver-Film Semi-Coated Nanosphere Array
    journal, September 2019

    • Zhang, Wending; Xue, Tianyang; Zhang, Lu
    • Sensors, Vol. 19, Issue 18
    • DOI: 10.3390/s19183966

    Non-adiabatic molecular dynamics of molecules in the presence of strong light-matter interactions
    journal, October 2019

    • Zhang, Yu; Nelson, Tammie; Tretiak, Sergei
    • The Journal of Chemical Physics, Vol. 151, Issue 15
    • DOI: 10.1063/1.5116550

    Fabrication and simulation of V-shaped Ag nanorods as high-performance SERS substrates
    journal, January 2018

    • Li, Jianghao; Fan, Yihang; Xue, Xiaotian
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 40
    • DOI: 10.1039/c8cp05533e

    Vibrational spectroscopy of compound semiconductor nanocrystals
    journal, September 2018

    • Dzhagan, V. M.; Azhniuk, Yu M.; Milekhin, A. G.
    • Journal of Physics D: Applied Physics, Vol. 51, Issue 50
    • DOI: 10.1088/1361-6463/aada5c

    Probe design for super-multiplexed vibrational imaging
    journal, April 2019

    Volume‐Enhanced Raman Scattering Detection of Viruses
    journal, February 2019

    Morphology dependent near-field response in atomistic plasmonic nanocavities
    journal, January 2018

    Electrodeposited surfaces with reversibly switching interfacial properties
    journal, November 2019

    Bioscaffold arrays decorated with Ag nanoparticles as a SERS substrate for direct detection of melamine in infant formula
    journal, January 2019

    • Zhao, Nan; Li, Hefu; Tian, Cunwei
    • RSC Advances, Vol. 9, Issue 38
    • DOI: 10.1039/c9ra01862j

    Low cost tips for tip-enhanced Raman spectroscopy fabricated by two-step electrochemical etching of 125 µm diameter gold wires
    journal, January 2018

    • Foti, Antonino; Barreca, Francesco; Fazio, Enza
    • Beilstein Journal of Nanotechnology, Vol. 9
    • DOI: 10.3762/bjnano.9.254

    Transforming Noble‐Metal Nanocrystals into Complex Nanostructures through Facet‐Selective Etching and Deposition
    journal, August 2019

    Modulating and probing the dynamic intermolecular interactions in plasmonic molecule-pair junctions
    journal, January 2019

    • Ma, Tao; Guo, Jing; Chang, Shuai
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 29
    • DOI: 10.1039/c9cp02030f

    Identifying surface reaction intermediates with photoemission tomography
    text, January 2019

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