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Plasmonic Liquid Marbles: A Miniature Substrate-less SERS Platform for Quantitative and Multiplex Ultratrace Molecular Detection

Authors

  • Hiang Kwee Lee,

    1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 50 Nanyang Ave, Singapore 637371 (Singapore)
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  • Dr. Yih Hong Lee,

    1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 50 Nanyang Ave, Singapore 637371 (Singapore)
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  • Dr. In Yee Phang,

    1. Institute of Materials Research and Engineering, A*STAR (Agency for Science, Technology and Research), 3 Research Link, Singapore 117602 (Singapore)
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  • Jiaqi Wei,

    1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 50 Nanyang Ave, Singapore 637371 (Singapore)
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  • Yue-E Miao,

    1. State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433 (P.R. China)
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  • Prof. Tianxi Liu,

    1. State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433 (P.R. China)
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  • Prof. Xing Yi Ling

    Corresponding author
    1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 50 Nanyang Ave, Singapore 637371 (Singapore)
    • Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 50 Nanyang Ave, Singapore 637371 (Singapore)===

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  • X.Y.L. thanks the National Research Foundation, Singapore (NRF-NRFF2012-04) for support and Nanyang Technological University for a start-up grant. H.K.L. thanks A*STAR, Singapore for an A*STAR Graduate Scholarship. SERS=surface-enhanced Raman spectroscopy.

Abstract

Inspired by aphids, liquid marbles have been studied extensively and have found application as isolated microreactors, as micropumps, and in sensing. However, current liquid-marble-based sensing methodologies are limited to qualitative colorimetry-based detection. Herein we describe the fabrication of a plasmonic liquid marble as a substrate-less analytical platform which, when coupled with ultrasensitive SERS, enables simultaneous multiplex quantification and the identification of ultratrace analytes across separate phases. Our plasmonic liquid marble demonstrates excellent mechanical stability and is suitable for the quantitative examination of ultratrace analytes, with detection limits as low as 0.3 fmol, which corresponds to an analytical enhancement factor of 5×108. The results of our simultaneous detection scheme based on plasmonic liquid marbles and an aqueous–solid–organic interface quantitatively tally with those found for the individual detection of methylene blue and coumarin.

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