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dc.contributor.authorGrys, David
dc.contributor.authorde Nijs, Bart
dc.contributor.authorHuang, Junyang
dc.contributor.authorScherman, Oren
dc.contributor.authorBaumberg, Jeremy
dc.date.accessioned2022-01-28T14:46:55Z
dc.date.available2022-01-28T14:46:55Z
dc.date.issued2021-12-24
dc.identifier.issn2379-3694
dc.identifier.other34882398
dc.identifier.otherPMC8715530
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/333109
dc.descriptionFunder: Isaac Newton Trust
dc.descriptionFunder: Leverhulme Trust
dc.description.abstractSurface-enhanced Raman spectroscopy (SERS) is considered an attractive candidate for quantitative and multiplexed molecular sensing of analytes whose chemical composition is not fully known. In principle, molecules can be identified through their fingerprint spectrum when binding inside plasmonic hotspots. However, competitive binding experiments between methyl viologen (MV2+) and its deuterated isomer (d8-MV2+) here show that determining individual concentrations by extracting peak intensities from spectra is not possible. This is because analytes bind to different binding sites inside and outside of hotspots with different affinities. Only by knowing all binding constants and geometry-related factors, can a model revealing accurate concentrations be constructed. To collect sufficiently reproducible data for such a sensitive experiment, we fully automate measurements using a high-throughput SERS optical system integrated with a liquid handling robot (the SERSbot). This now allows us to accurately deconvolute analyte mixtures through independent component analysis (ICA) and to quantitatively map out the competitive binding of analytes in nanogaps. Its success demonstrates the feasibility of automated SERS in a wide variety of experiments and applications.
dc.description.sponsorshipEPSRC Grants (EP/L027151/1, EP/R020965/1, EP/P029426/1) and ERC PICOFORCE (883703). EPSRC grant EP/L015889/1 for the EPSRC Centre for Doctoral Training in Sensor Technologies and Applications.
dc.languageeng
dc.publisherAmerican Chemical Society (ACS)
dc.rightsAttribution-NonCommercial-NoDerivatives 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.sourcenlmid: 101669031
dc.sourceessn: 2379-3694
dc.subjectLab Automation
dc.subjectLiquid Handling
dc.subjectCompetitive Binding
dc.subjectSurface-enhanced Raman
dc.subjectLangmuir Isotherm
dc.subjectMultiplexed Sensing
dc.subjectQuantitative Sers
dc.subjectLab Robot
dc.subjectNanogap Sequestration
dc.titleSERSbot: Revealing the Details of SERS Multianalyte Sensing Using Full Automation.
dc.typeArticle
dc.date.updated2022-01-28T14:46:54Z
prism.endingPage4514
prism.issueIdentifier12
prism.publicationNameACS Sens
prism.startingPage4507
prism.volume6
dc.identifier.doi10.17863/CAM.80533
dcterms.dateAccepted2021-11-17
rioxxterms.versionofrecord10.1021/acssensors.1c02116
rioxxterms.versionVoR
rioxxterms.licenseref.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.contributor.orcidGrys, David [0000-0002-4038-6388]
dc.contributor.orcidde Nijs, Bart [0000-0002-8234-723X]
dc.contributor.orcidHuang, Junyang [0000-0001-6676-495X]
dc.contributor.orcidScherman, Oren [0000-0001-8032-7166]
dc.contributor.orcidBaumberg, Jeremy [0000-0002-9606-9488]
dc.identifier.eissn2379-3694
pubs.funder-project-idEPSRC (1783357)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L027151/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L015889/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P029426/1)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/R020965/1)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) ERC (883703)
cam.issuedOnline2021-12-09


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Attribution-NonCommercial-NoDerivatives 4.0 International
Except where otherwise noted, this item's licence is described as Attribution-NonCommercial-NoDerivatives 4.0 International