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Multivariate spectral analysis of pH SERS probes for improved sensing capabilities

Adam Williams, Kevin John Flynn, Zhidao Xia Orcid Logo, Peter Dunstan Orcid Logo

Journal of Raman Spectroscopy

Swansea University Authors: Zhidao Xia Orcid Logo, Peter Dunstan Orcid Logo

DOI (Published version): 10.1002/jrs.4910

Abstract

Appropriate functional groups adsorbed to the surface of plasmonic nanoparticles provides a platform for localised optical sensing. For example, intracellular pH nanosensors based on surface enhanced Raman spectroscopy (SERS) have been developed. However, the measurement methods and analysis of pH-S...

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Published in: Journal of Raman Spectroscopy
Published: 2016
URI: https://cronfa.swan.ac.uk/Record/cronfa26714
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fullrecord <?xml version="1.0"?><rfc1807><datestamp>2019-08-08T11:25:12.0773869</datestamp><bib-version>v2</bib-version><id>26714</id><entry>2016-03-08</entry><title>Multivariate spectral analysis of pH SERS probes for improved sensing capabilities</title><swanseaauthors><author><sid>c9307abfed1b43987a19da0c0e30d7a4</sid><ORCID>0000-0002-2047-7282</ORCID><firstname>Zhidao</firstname><surname>Xia</surname><name>Zhidao Xia</name><active>true</active><ethesisStudent>false</ethesisStudent></author><author><sid>eada15d4d33fcb3dfddcff43f1323bd6</sid><ORCID>0000-0002-4337-4307</ORCID><firstname>Peter</firstname><surname>Dunstan</surname><name>Peter Dunstan</name><active>true</active><ethesisStudent>false</ethesisStudent></author></swanseaauthors><date>2016-03-08</date><deptcode>BMS</deptcode><abstract>Appropriate functional groups adsorbed to the surface of plasmonic nanoparticles provides a platform for localised optical sensing. For example, intracellular pH nanosensors based on surface enhanced Raman spectroscopy (SERS) have been developed. However, the measurement methods and analysis of pH-SERS can greatly impact the precision and accuracy of pH calibration. This paper provides several key improvements to the performance and analysis pH nanosensors which thus transforms the performance into a useable intracellular pH sensor. We report the plasmon-induced decarboxylation of para-mercaptobenzoic acid (pMBA) pH-reporters which are bound to the gold nanoparticles, and attribute this to the laser power. This detrimental decarboxylation of pMBA has significant implications for accurate reporting and analysis due to the sensitivity and reliability of the pH sensor. The greatest implication of decarboxylation of pH sensors is inaccurate or false pH reporting, because the decarboxylation spectral signatures map directly onto those that are typically used to record pH changes. Here a unique application of the multivariate statistical technique, principal components analysis (PCA) is presented along with an optimal spectral region for pH calibration. By direct comparisons between the PCA method with the typically employed ratio-metric analysis a significant improvement in generating accurate pH sensing is demonstrated. An application of intracellular pH sensing in macrophage cells using these nanosensors promotes these step-changes in pH measurement methodology.</abstract><type>Journal Article</type><journal>Journal of Raman Spectroscopy</journal><publisher/><keywords>nanosensors, pMBA, Raman Spectroscopy, PCA</keywords><publishedDay>31</publishedDay><publishedMonth>12</publishedMonth><publishedYear>2016</publishedYear><publishedDate>2016-12-31</publishedDate><doi>10.1002/jrs.4910</doi><url/><notes>The paper represents a significant enhancement on the analysis of spectral properties relating to producing reliable nano-reporter of pH, which can be used for in-vivo studies. The paper describes an adapted analysis methodology which focussed on key spectral markers that enable better discrimination when the reporter is in a biological host. The use of pH intracellular probes has been limited but with this newly developed analysis and extended protocols, the practical use of pH nano-reporters has the opportunity to be fully exploited in biological systems. Indeed the paper then describes an application in a human macrophage cell. The work adds significantly to the field due to the improvements made at reliably identifying pH.</notes><college>COLLEGE NANME</college><department>Biomedical Sciences</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>BMS</DepartmentCode><institution>Swansea University</institution><apcterm/><lastEdited>2019-08-08T11:25:12.0773869</lastEdited><Created>2016-03-08T01:03:03.2008402</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Biosciences, Geography and Physics - Physics</level></path><authors><author><firstname>Adam</firstname><surname>Williams</surname><order>1</order></author><author><firstname>Kevin John</firstname><surname>Flynn</surname><order>2</order></author><author><firstname>Zhidao</firstname><surname>Xia</surname><orcid>0000-0002-2047-7282</orcid><order>3</order></author><author><firstname>Peter</firstname><surname>Dunstan</surname><orcid>0000-0002-4337-4307</orcid><order>4</order></author></authors><documents><document><filename>0026714-67201620714PM.pdf</filename><originalFilename>JRS_Williams_Dunstan_pH_final_submissionv2.pdf</originalFilename><uploaded>2016-06-07T14:07:14.0570000</uploaded><type>Output</type><contentLength>1733070</contentLength><contentType>application/pdf</contentType><version>Accepted Manuscript</version><cronfaStatus>true</cronfaStatus><embargoDate>2016-06-07T14:07:14.0570000</embargoDate><copyrightCorrect>true</copyrightCorrect></document></documents><OutputDurs/></rfc1807>
spelling 2019-08-08T11:25:12.0773869 v2 26714 2016-03-08 Multivariate spectral analysis of pH SERS probes for improved sensing capabilities c9307abfed1b43987a19da0c0e30d7a4 0000-0002-2047-7282 Zhidao Xia Zhidao Xia true false eada15d4d33fcb3dfddcff43f1323bd6 0000-0002-4337-4307 Peter Dunstan Peter Dunstan true false 2016-03-08 BMS Appropriate functional groups adsorbed to the surface of plasmonic nanoparticles provides a platform for localised optical sensing. For example, intracellular pH nanosensors based on surface enhanced Raman spectroscopy (SERS) have been developed. However, the measurement methods and analysis of pH-SERS can greatly impact the precision and accuracy of pH calibration. This paper provides several key improvements to the performance and analysis pH nanosensors which thus transforms the performance into a useable intracellular pH sensor. We report the plasmon-induced decarboxylation of para-mercaptobenzoic acid (pMBA) pH-reporters which are bound to the gold nanoparticles, and attribute this to the laser power. This detrimental decarboxylation of pMBA has significant implications for accurate reporting and analysis due to the sensitivity and reliability of the pH sensor. The greatest implication of decarboxylation of pH sensors is inaccurate or false pH reporting, because the decarboxylation spectral signatures map directly onto those that are typically used to record pH changes. Here a unique application of the multivariate statistical technique, principal components analysis (PCA) is presented along with an optimal spectral region for pH calibration. By direct comparisons between the PCA method with the typically employed ratio-metric analysis a significant improvement in generating accurate pH sensing is demonstrated. An application of intracellular pH sensing in macrophage cells using these nanosensors promotes these step-changes in pH measurement methodology. Journal Article Journal of Raman Spectroscopy nanosensors, pMBA, Raman Spectroscopy, PCA 31 12 2016 2016-12-31 10.1002/jrs.4910 The paper represents a significant enhancement on the analysis of spectral properties relating to producing reliable nano-reporter of pH, which can be used for in-vivo studies. The paper describes an adapted analysis methodology which focussed on key spectral markers that enable better discrimination when the reporter is in a biological host. The use of pH intracellular probes has been limited but with this newly developed analysis and extended protocols, the practical use of pH nano-reporters has the opportunity to be fully exploited in biological systems. Indeed the paper then describes an application in a human macrophage cell. The work adds significantly to the field due to the improvements made at reliably identifying pH. COLLEGE NANME Biomedical Sciences COLLEGE CODE BMS Swansea University 2019-08-08T11:25:12.0773869 2016-03-08T01:03:03.2008402 Faculty of Science and Engineering School of Biosciences, Geography and Physics - Physics Adam Williams 1 Kevin John Flynn 2 Zhidao Xia 0000-0002-2047-7282 3 Peter Dunstan 0000-0002-4337-4307 4 0026714-67201620714PM.pdf JRS_Williams_Dunstan_pH_final_submissionv2.pdf 2016-06-07T14:07:14.0570000 Output 1733070 application/pdf Accepted Manuscript true 2016-06-07T14:07:14.0570000 true
title Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
spellingShingle Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
Zhidao Xia
Peter Dunstan
title_short Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
title_full Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
title_fullStr Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
title_full_unstemmed Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
title_sort Multivariate spectral analysis of pH SERS probes for improved sensing capabilities
author_id_str_mv c9307abfed1b43987a19da0c0e30d7a4
eada15d4d33fcb3dfddcff43f1323bd6
author_id_fullname_str_mv c9307abfed1b43987a19da0c0e30d7a4_***_Zhidao Xia
eada15d4d33fcb3dfddcff43f1323bd6_***_Peter Dunstan
author Zhidao Xia
Peter Dunstan
author2 Adam Williams
Kevin John Flynn
Zhidao Xia
Peter Dunstan
format Journal article
container_title Journal of Raman Spectroscopy
publishDate 2016
institution Swansea University
doi_str_mv 10.1002/jrs.4910
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Biosciences, Geography and Physics - Physics{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Biosciences, Geography and Physics - Physics
document_store_str 1
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description Appropriate functional groups adsorbed to the surface of plasmonic nanoparticles provides a platform for localised optical sensing. For example, intracellular pH nanosensors based on surface enhanced Raman spectroscopy (SERS) have been developed. However, the measurement methods and analysis of pH-SERS can greatly impact the precision and accuracy of pH calibration. This paper provides several key improvements to the performance and analysis pH nanosensors which thus transforms the performance into a useable intracellular pH sensor. We report the plasmon-induced decarboxylation of para-mercaptobenzoic acid (pMBA) pH-reporters which are bound to the gold nanoparticles, and attribute this to the laser power. This detrimental decarboxylation of pMBA has significant implications for accurate reporting and analysis due to the sensitivity and reliability of the pH sensor. The greatest implication of decarboxylation of pH sensors is inaccurate or false pH reporting, because the decarboxylation spectral signatures map directly onto those that are typically used to record pH changes. Here a unique application of the multivariate statistical technique, principal components analysis (PCA) is presented along with an optimal spectral region for pH calibration. By direct comparisons between the PCA method with the typically employed ratio-metric analysis a significant improvement in generating accurate pH sensing is demonstrated. An application of intracellular pH sensing in macrophage cells using these nanosensors promotes these step-changes in pH measurement methodology.
published_date 2016-12-31T03:32:08Z
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score 10.972127

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