@article{f32bafb02aa74ff89328b3dca863cb43,
title = "Surface enhanced Raman scattering artificial nose for high dimensionality fingerprinting",
abstract = "Label-free surface-enhanced Raman spectroscopy (SERS) can interrogate systems by directly fingerprinting their components{\textquoteright} unique physicochemical properties. In complex biological systems however, this can yield highly overlapping spectra that hinder sample identification. Here, we present an artificial-nose inspired SERS fingerprinting approach where spectral data is obtained as a function of sensor surface chemical functionality. Supported by molecular dynamics modeling, we show that mildly selective self-assembled monolayers can influence the strength and configuration in which analytes interact with plasmonic surfaces, diversifying the resulting SERS fingerprints. Since each sensor generates a modulated signature, the implicit value of increasing the dimensionality of datasets is shown using cell lysates for all possible combinations of up to 9 fingerprints. Reliable improvements in mean discriminatory accuracy towards 100% are achieved with each additional surface functionality. This arrayed label-free platform illustrates the wide-ranging potential of high-dimensionality artificial-nose based sensing systems for more reliable assessment of complex biological matrices.",
author = "Nayoung Kim and Thomas, {Michael R.} and Bergholt, {Mads S.} and Pence, {Isaac J.} and Hyejeong Seong and Patrick Charchar and Nevena Todorova and Anika Nagelkerke and Alexis Belessiotis-Richards and Payne, {David J.} and Amy Gelmi and Irene Yarovsky and Stevens, {Molly M.}",
note = "Funding Information: N.K. acknowledges support from the Korean Government Scholarship for Study Overseas funded by the Korean Ministry of Education. M.R.T. and M.M.S. acknowledge support from the i-sense Engineering and Physical Sciences Research Council (EPSRC) IRC in Early Warning Sensing Systems for Infectious Diseases (EP/K031953/1; EP/ R00529X/1; www.i-sense.org.uk). M.R.T. and M.M.S. acknowledge support from the Medical Research Council (MRC) grant “m-Africa” (MR/P024378/1). M.S.B. acknowledges support from the European Union{\textquoteright}s H2020 Research and Innovation programme under the Marie Sk{\l}odowska-Curie Fellowship “IMAGINE” (701713). I.J.P. Funding Information: acknowledges support from the Whitaker International Program, Institute of International Education, United States of America. H.S. acknowledges support from the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2017R1A6A3A03007397) and the European Union{\textquoteright}s H2020 Research and Innovation programme under the Marie Sk{\l}odowska-Curie Fellowship “ELECTRO NEEDLE” (797311). A.N. acknowledges support from the National Institute for Health Research (NIHR) Imperial Biomedical Research Centre and the Institute of Cancer Research, London, through the joint Cancer Research Centre of Excellence (CRCE). A.G. acknowledges support from the European Union{\textquoteright}s Horizon 2020 Research and Innovation Programme through the Marie Sk{\l}odowska-Curie Individual Fellowship “RAISED” (660757). D.J.P. acknowledges support from the Royal Society (Grants No. UF100105 and No. UF150693) and EPSRC (Grant No. EP/M028291/ 1). I.Y. and M.M.S. acknowledge the Australian Research Council Discover grants DP140101888 and DP170100511. A.B.R. acknowledges a studentship from the EPSRC CDT for the Advanced Characterisation of Materials (EP/L015277/1). P.C., N.T. and I.Y. acknowledge grant e87 for access to high performance computational resources provided by the Australian government via the NCI and Pawsey facilities. All authors would like to thank Seung Kyun Ha for helpful discussions regarding statistical analysis and its practical implementation. Publisher Copyright: {\textcopyright} 2020, The Author(s).",
year = "2020",
month = dec,
day = "1",
doi = "10.1038/s41467-019-13615-2",
language = "English (US)",
volume = "11",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",
number = "1",
}