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      In-situ plasmon-driven chemical reactions revealed by high vacuum tip-enhanced Raman spectroscopy

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      Scientific Reports
      Nature Publishing Group

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          Abstract

          With strong surface plasmons excited at the metallic tip, tip-enhanced Raman spectroscopy (TERS) has both high spectroscopic sensitivity and high spatial resolution, and is becoming an essential tool for chemical analysis. It is a great challenge to combine TERS with a high vacuum system due to the poor optical collection efficiency. We used our innovatively designed home-built high vacuum TERS (HV-TERS) to investigate the plasmon-driven in-situ chemical reaction of 4-nitrobenzenethiol dimerizing to dimercaptoazobenzene. The chemical reactions can be controlled by the plasmon intensity, which in turn can be controlled by the incident laser intensity, tunneling current and bias voltage. The temperature of such a chemical reaction can also be obtained by the clearly observed Stokes and Anti-Stokes HV-TERS peaks. Our findings offer a new way to design a highly efficient HV-TERS system and its applications to chemical catalysis and synthesis of molecules, and significantly extend the studies of chemical reactions.

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          Most cited references15

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          Photodetection with active optical antennas.

          Nanoantennas are key optical components for light harvesting; photodiodes convert light into a current of electrons for photodetection. We show that these two distinct, independent functions can be combined into the same structure. Photons coupled into a metallic nanoantenna excite resonant plasmons, which decay into energetic, "hot" electrons injected over a potential barrier at the nanoantenna-semiconductor interface, resulting in a photocurrent. This dual-function structure is a highly compact, wavelength-resonant, and polarization-specific light detector, with a spectral response extending to energies well below the semiconductor band edge.
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            When the signal is not from the original molecule to be detected: chemical transformation of para-aminothiophenol on Ag during the SERS measurement.

            Surface-enhanced Raman spectroscopy (SERS) has long been considered as a noninvasive technique that can obtain the fingerprint vibrational information of surface species. We demonstrated in this paper that a laser with a power level considered to be low in the traditional SERS measurement can already lead to a significant surface reaction. para-Aminothiophenol, an important probe molecule in SERS, was found to be oxidized to form 4,4'-dimercaptoazobenzene (DMAB) on a roughened silver surface during the SERS measurement. The assumption was confirmed experimentally by surface mass spectroscopy and SERS as well as electrochemistry of the synthesized DMAB, which agrees well with theoretical calculations. A defocusing method was used to avoid the laser induced surface reaction and perform reliable SERS characterization and identification, which can effectively avoid erroneous interpretation of the distorted experimental result.
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              Tip-enhanced Raman scattering.

              Tip-enhanced Raman scattering (TERS) is a technique that provides molecular information on the nanometre scale. Using a nanometre-sized metal particle results in a strong signal enhancement and a lateral resolution similar to the dimensions of the particle. As TERS is in a way the ultimate SERS experiment, the theoretical background will be briefly discussed with respect to the unique features and the specific effects that occur when only a single nanoparticle is used as a probe. All the major parts of the instrument will be revealed and the specific advantages of the different instrumental set ups will be investigated with respect to the particular requirements of the sample. Selected examples ranging from material science to cell biological applications demonstrate the capabilities and the potential of TERS in this tutorial review.
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                Author and article information

                Journal
                Sci Rep
                Sci Rep
                Scientific Reports
                Nature Publishing Group
                2045-2322
                11 September 2012
                2012
                : 2
                : 647
                Affiliations
                [1 ]simpleBeijing National Laboratory for Condensed Matter Physics, Institute of Physics , Chinese Academy of Sciences, P. O. Box 603-146, Beijing, 100190, People's Republic of China
                [2 ]simpleCollege of Physics and Information Technology, Shaanxi Normal University , Xi'an, 710062, People's Republic of China
                Author notes
                Article
                srep00647
                10.1038/srep00647
                3438462
                22970339
                ba6e395d-7c87-4434-b71b-d1967490049b
                Copyright © 2012, Macmillan Publishers Limited. All rights reserved

                This work is licensed under a Creative Commons Attribution-NonCommercial-ShareALike 3.0 Unported License. To view a copy of this license, visit http://creativecommons.org/licenses/by-nc-sa/3.0/

                History
                : 29 May 2012
                : 16 August 2012
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