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      Thin silica shell coated Ag assembled nanostructures for expanding generality of SERS analytes

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          Abstract

          Surface-enhanced Raman scattering (SERS) provides a unique non-destructive spectroscopic fingerprint for chemical detection. However, intrinsic differences in affinity of analyte molecules to metal surface hinder SERS as a universal quantitative detection tool for various analyte molecules simultaneously. This must be overcome while keeping close proximity of analyte molecules to the metal surface. Moreover, assembled metal nanoparticles (NPs) structures might be beneficial for sensitive and reliable detection of chemicals than single NP structures. For this purpose, here we introduce thin silica-coated and assembled Ag NPs (SiO 2@Ag@SiO 2 NPs) for simultaneous and quantitative detection of chemicals that have different intrinsic affinities to silver metal. These SiO 2@Ag@SiO 2 NPs could detect each SERS peak of aniline or 4-aminothiophenol (4-ATP) from the mixture with limits of detection (LOD) of 93 ppm and 54 ppb, respectively. E-field distribution based on interparticle distance was simulated using discrete dipole approximation (DDA) calculation to gain insight into enhanced scattering of these thin silica coated Ag NP assemblies. These NPs were successfully applied to detect aniline in river water and tap water. Results suggest that SiO 2@Ag@SiO 2 NP-based SERS detection systems can be used as a simple and universal detection tool for environment pollutants and food safety.

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          Most cited references 62

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          Discrete-Dipole Approximation For Scattering Calculations

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            Shell-isolated nanoparticle-enhanced Raman spectroscopy.

            Surface-enhanced Raman scattering (SERS) is a powerful spectroscopy technique that can provide non-destructive and ultra-sensitive characterization down to single molecular level, comparable to single-molecule fluorescence spectroscopy. However, generally substrates based on metals such as Ag, Au and Cu, either with roughened surfaces or in the form of nanoparticles, are required to realise a substantial SERS effect, and this has severely limited the breadth of practical applications of SERS. A number of approaches have extended the technique to non-traditional substrates, most notably tip-enhanced Raman spectroscopy (TERS) where the probed substance (molecule or material surface) can be on a generic substrate and where a nanoscale gold tip above the substrate acts as the Raman signal amplifier. The drawback is that the total Raman scattering signal from the tip area is rather weak, thus limiting TERS studies to molecules with large Raman cross-sections. Here, we report an approach, which we name shell-isolated nanoparticle-enhanced Raman spectroscopy, in which the Raman signal amplification is provided by gold nanoparticles with an ultrathin silica or alumina shell. A monolayer of such nanoparticles is spread as 'smart dust' over the surface that is to be probed. The ultrathin coating keeps the nanoparticles from agglomerating, separates them from direct contact with the probed material and allows the nanoparticles to conform to different contours of substrates. High-quality Raman spectra were obtained on various molecules adsorbed at Pt and Au single-crystal surfaces and from Si surfaces with hydrogen monolayers. These measurements and our studies on yeast cells and citrus fruits with pesticide residues illustrate that our method significantly expands the flexibility of SERS for useful applications in the materials and life sciences, as well as for the inspection of food safety, drugs, explosives and environment pollutants.
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              Templated techniques for the synthesis and assembly of plasmonic nanostructures.

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                Author and article information

                Contributors
                Role: Editor
                Journal
                PLoS One
                PLoS ONE
                plos
                plosone
                PLoS ONE
                Public Library of Science (San Francisco, CA USA )
                1932-6203
                1 June 2017
                2017
                : 12
                : 6
                Affiliations
                [1 ]Department of Chemistry Education, Seoul National University, Seoul, Republic of Korea
                [2 ]Department of Bioscience and Biotechnology, Konkuk University, Seoul, Republic of Korea
                [3 ]Interdisciplinary Program in Nano-Science and Technology. Seoul National University, Seoul, Republic of Korea
                [4 ]School of Chemical and Biological Engineering, Seoul National University Seoul, Republic of Korea
                Institute of Materials Science, GERMANY
                Author notes

                Competing Interests: The authors have declared that no competing interests exist.

                • Conceptualization: MGC HMK YLK DHJ BHJ.

                • Funding acquisition: MGC HMK DHJ BHJ.

                • Investigation: MGC HMK YLK ML DHJ BHJ.

                • Methodology: MGC HMK YLK.

                • Project administration: MGC HMK DHJ BHJ.

                • Resources: MGC HMK DHJ BHJ.

                • Supervision: MGC HMK DHJ BHJ.

                • Validation: MGC HMK DHJ BHJ.

                • Visualization: MGC HMK ML DHJ BHJ.

                • Writing – original draft: MGC HMK YLK DHJ BHJ.

                • Writing – review & editing: MGC HMK YLK ML HK JK XHP THK EH YSL DHJ BHJ.

                [¤]

                Current address: Department of Radiology, Harvard Medical School and Gordon Center for Medical Imaging, Massachusetts General Hospital, Boston, Massachusetts, United States of America

                Article
                PONE-D-17-04113
                10.1371/journal.pone.0178651
                5453564
                28570633
                © 2017 Cha et al

                This is an open access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

                Page count
                Figures: 6, Tables: 0, Pages: 13
                Product
                Funding
                Funded by: funder-id http://dx.doi.org/10.13039/501100003725, National Research Foundation of Korea;
                Award ID: 2016-A423-0045
                Award Recipient :
                Funded by: Korean Health Technology R&D Project, Ministry of Health & Welfare
                Award ID: HI17C1264
                Award Recipient :
                Funded by: Korean Health Technology R&D Project, Ministry of Health & Welfare
                Award ID: HI17C1264
                Award Recipient :
                This work was supported by the Bio & Medical Technology Development Program of the National Research Foundation (NRF) & funded by the Korean government (MSIP & MOHW) (2016-A423-0045), Korean Health Technology R&D Project, Ministry of Health & Welfare (HI17C1264). The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript.
                Categories
                Research Article
                Physical Sciences
                Chemistry
                Chemical Compounds
                Organic Compounds
                Anilines
                Physical Sciences
                Chemistry
                Organic Chemistry
                Organic Compounds
                Anilines
                Earth Sciences
                Hydrology
                Surface Water
                Physical Sciences
                Chemistry
                Chemical Compounds
                Organic Compounds
                Alcohols
                Ethanol
                Physical Sciences
                Chemistry
                Organic Chemistry
                Organic Compounds
                Alcohols
                Ethanol
                Earth Sciences
                Marine and Aquatic Sciences
                Bodies of Water
                Rivers
                Ecology and Environmental Sciences
                Aquatic Environments
                Freshwater Environments
                Rivers
                Earth Sciences
                Marine and Aquatic Sciences
                Aquatic Environments
                Freshwater Environments
                Rivers
                Physical Sciences
                Chemistry
                Chemical Compounds
                Organic Compounds
                Thiols
                Physical Sciences
                Chemistry
                Organic Chemistry
                Organic Compounds
                Thiols
                Physical Sciences
                Physics
                Scattering
                Raman Scattering
                Physical sciences
                Chemistry
                Chemical physics
                Dimers (Chemical physics)
                Physical sciences
                Physics
                Chemical physics
                Dimers (Chemical physics)
                Physical Sciences
                Chemistry
                Chemical Elements
                Silver
                Custom metadata
                All relevant data are within the paper and its Supporting Information file.

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