Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors

Abstract Peptide-based liquid-liquid phase separated domains, or coacervates, are a biomaterial gaining new interest due to their exciting potential in fields ranging from biosensing to drug delivery. In this study, we demonstrate that coacervates provide a simple and biocompatible medium to improve...

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Main Authors: Christopher M. Green, Deborah Sementa, Divita Mathur, Joseph S. Melinger, Priyasha Deshpande, Shana Elbaum-Garfinkle, Igor L. Medintz, Rein V. Ulijn, Sebastián A. Díaz
Format: Article
Language:English
Published: Nature Portfolio 2024-02-01
Series:Communications Chemistry
Online Access:https://doi.org/10.1038/s42004-024-01124-3
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author Christopher M. Green
Deborah Sementa
Divita Mathur
Joseph S. Melinger
Priyasha Deshpande
Shana Elbaum-Garfinkle
Igor L. Medintz
Rein V. Ulijn
Sebastián A. Díaz
author_facet Christopher M. Green
Deborah Sementa
Divita Mathur
Joseph S. Melinger
Priyasha Deshpande
Shana Elbaum-Garfinkle
Igor L. Medintz
Rein V. Ulijn
Sebastián A. Díaz
author_sort Christopher M. Green
collection DOAJ
description Abstract Peptide-based liquid-liquid phase separated domains, or coacervates, are a biomaterial gaining new interest due to their exciting potential in fields ranging from biosensing to drug delivery. In this study, we demonstrate that coacervates provide a simple and biocompatible medium to improve nucleic acid biosensors through the sequestration of both the biosensor and target strands within the coacervate, thereby increasing their local concentration. Using the well-established polyarginine (R9) – ATP coacervate system and an energy transfer-based DNA molecular beacon we observed three key improvements: i) a greater than 20-fold reduction of the limit of detection within coacervates when compared to control buffer solutions; ii) an increase in the kinetics, equilibrium was reached more than 4-times faster in coacervates; and iii) enhancement in the dye fluorescent quantum yields within the coacervates, resulting in greater signal-to-noise. The observed benefits translate into coacervates greatly improving bioassay functionality.
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spelling doaj.art-17560a3af1604411ac2b319cd3bed36b2024-03-05T17:55:30ZengNature PortfolioCommunications Chemistry2399-36692024-02-01711910.1038/s42004-024-01124-3Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensorsChristopher M. Green0Deborah Sementa1Divita Mathur2Joseph S. Melinger3Priyasha Deshpande4Shana Elbaum-Garfinkle5Igor L. Medintz6Rein V. Ulijn7Sebastián A. Díaz8Center for Bio/Molecular Science and Engineering Code 6900, U.S. Naval Research LaboratoryNanoscience Initiative at Advanced Science Research Center, Graduate Center of the City University of New YorkDepartment of Chemistry, Case Western Reserve UniversityElectronics Sciences and Technology Division Code 6816, U.S. Naval Research LaboratoryStructural Biology Initiative at Advanced Science Research Center, Graduate Center of the City University of New YorkStructural Biology Initiative at Advanced Science Research Center, Graduate Center of the City University of New YorkCenter for Bio/Molecular Science and Engineering Code 6900, U.S. Naval Research LaboratoryNanoscience Initiative at Advanced Science Research Center, Graduate Center of the City University of New YorkCenter for Bio/Molecular Science and Engineering Code 6900, U.S. Naval Research LaboratoryAbstract Peptide-based liquid-liquid phase separated domains, or coacervates, are a biomaterial gaining new interest due to their exciting potential in fields ranging from biosensing to drug delivery. In this study, we demonstrate that coacervates provide a simple and biocompatible medium to improve nucleic acid biosensors through the sequestration of both the biosensor and target strands within the coacervate, thereby increasing their local concentration. Using the well-established polyarginine (R9) – ATP coacervate system and an energy transfer-based DNA molecular beacon we observed three key improvements: i) a greater than 20-fold reduction of the limit of detection within coacervates when compared to control buffer solutions; ii) an increase in the kinetics, equilibrium was reached more than 4-times faster in coacervates; and iii) enhancement in the dye fluorescent quantum yields within the coacervates, resulting in greater signal-to-noise. The observed benefits translate into coacervates greatly improving bioassay functionality.https://doi.org/10.1038/s42004-024-01124-3
spellingShingle Christopher M. Green
Deborah Sementa
Divita Mathur
Joseph S. Melinger
Priyasha Deshpande
Shana Elbaum-Garfinkle
Igor L. Medintz
Rein V. Ulijn
Sebastián A. Díaz
Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
Communications Chemistry
title Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
title_full Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
title_fullStr Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
title_full_unstemmed Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
title_short Sequestration within peptide coacervates improves the fluorescence intensity, kinetics, and limits of detection of dye-based DNA biosensors
title_sort sequestration within peptide coacervates improves the fluorescence intensity kinetics and limits of detection of dye based dna biosensors
url https://doi.org/10.1038/s42004-024-01124-3
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