Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles

Paul Williamson; Petteri Piskunen; Heini Ijäs; Adrian Butterworth; Veikko Linko; Damion K. Corrigan

doi:10.1021/acssensors.2c02469

Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles

Paul Williamson, Petteri Piskunen, Heini Ijäs, Adrian Butterworth, Veikko Linko^*, Damion K. Corrigan^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Scientific › peer-review

49 Citations (Scopus)

93 Downloads (Pure)

Abstract

Electrochemical DNA (e-DNA) biosensors are feasible tools for disease monitoring, with their ability to translate hybridization events between a desired nucleic acid target and a functionalized transducer, into recordable electrical signals. Such an approach provides a powerful method of sample analysis, with a strong potential to generate a rapid time to result in response to low analyte concentrations. Here, we report a strategy for the amplification of electrochemical signals associated with DNA hybridization, by harnessing the programmability of the DNA origami method to construct a sandwich assay to boost charge transfer resistance (R_CT) associated with target detection. This allowed for an improvement in the sensor limit of detection by two orders of magnitude compared to a conventional label-free e-DNA biosensor design and linearity for target concentrations between 10 pM and 1 nM without the requirement for probe labeling or enzymatic support. Additionally, this sensor design proved capable of achieving a high degree of strand selectivity in a challenging DNA-rich environment. This approach serves as a practical method for addressing strict sensitivity requirements necessary for a low-cost point-of-care device.

Original language	English
Pages (from-to)	1471–1480
Number of pages	10
Journal	ACS Sensors
Volume	8
Issue number	4
Early online date	13 Mar 2023
DOIs	https://doi.org/10.1021/acssensors.2c02469
Publication status	Published - 28 Apr 2023
MoE publication type	A1 Journal article-refereed

Funding

Financial support from EPSRC DTP (grant EP/R513349/1), the Emil Aaltonen Foundation, the Sigrid Jusélius Foundation, the Jane and Aatos Erkko Foundation, the Finnish Cultural Foundation (Kalle and Dagmar Välimaa Fund), the Magnus Ehrnrooth Foundation, and ERA Chair MATTER from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 856705 is gratefully acknowledged. This work was carried out under the Academy of Finland Centers of Excellence Program (2022–2029) in Life-Inspired Hybrid Materials (LIBER), project number 346110. We acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities, OtaNano Nanomicroscopy Center (Aalto-NMC), and Micronova Nanofabrication Center.

Keywords

antimicrobial resistance gene
DNA hybridization
DNA nanotechnology
electrochemical impedance spectroscopy
point-of-care devices
sensitivity enhancement
target selectivity

Access to Document

10.1021/acssensors.2c02469Licence: CC BY

CHEM_Williamson_et_al_Signal_Amplification_2023_ACS_SensorsFinal published version, 3.56 MBLicence: CC BY

Cite this

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title = "Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles",

abstract = "Electrochemical DNA (e-DNA) biosensors are feasible tools for disease monitoring, with their ability to translate hybridization events between a desired nucleic acid target and a functionalized transducer, into recordable electrical signals. Such an approach provides a powerful method of sample analysis, with a strong potential to generate a rapid time to result in response to low analyte concentrations. Here, we report a strategy for the amplification of electrochemical signals associated with DNA hybridization, by harnessing the programmability of the DNA origami method to construct a sandwich assay to boost charge transfer resistance (RCT) associated with target detection. This allowed for an improvement in the sensor limit of detection by two orders of magnitude compared to a conventional label-free e-DNA biosensor design and linearity for target concentrations between 10 pM and 1 nM without the requirement for probe labeling or enzymatic support. Additionally, this sensor design proved capable of achieving a high degree of strand selectivity in a challenging DNA-rich environment. This approach serves as a practical method for addressing strict sensitivity requirements necessary for a low-cost point-of-care device.",

keywords = "antimicrobial resistance gene, DNA hybridization, DNA nanotechnology, electrochemical impedance spectroscopy, point-of-care devices, sensitivity enhancement, target selectivity",

author = "Paul Williamson and Petteri Piskunen and Heini Ij{\"a}s and Adrian Butterworth and Veikko Linko and Corrigan, \{Damion K.\}",

note = "Funding Information: Financial support from EPSRC DTP (grant EP/R513349/1), the Emil Aaltonen Foundation, the Sigrid Jus{\'e}lius Foundation, the Jane and Aatos Erkko Foundation, the Finnish Cultural Foundation (Kalle and Dagmar V{\"a}limaa Fund), the Magnus Ehrnrooth Foundation, and ERA Chair MATTER from the European Union{\textquoteright}s Horizon 2020 research and innovation program under grant agreement no. 856705 is gratefully acknowledged. This work was carried out under the Academy of Finland Centers of Excellence Program (2022–2029) in Life-Inspired Hybrid Materials (LIBER), project number 346110. We acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities, OtaNano Nanomicroscopy Center (Aalto-NMC), and Micronova Nanofabrication Center. Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

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doi = "10.1021/acssensors.2c02469",

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AU - Piskunen, Petteri

AU - Ijäs, Heini

AU - Butterworth, Adrian

AU - Linko, Veikko

AU - Corrigan, Damion K.

N1 - Funding Information: Financial support from EPSRC DTP (grant EP/R513349/1), the Emil Aaltonen Foundation, the Sigrid Jusélius Foundation, the Jane and Aatos Erkko Foundation, the Finnish Cultural Foundation (Kalle and Dagmar Välimaa Fund), the Magnus Ehrnrooth Foundation, and ERA Chair MATTER from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 856705 is gratefully acknowledged. This work was carried out under the Academy of Finland Centers of Excellence Program (2022–2029) in Life-Inspired Hybrid Materials (LIBER), project number 346110. We acknowledge the provision of facilities and technical support by Aalto University Bioeconomy Facilities, OtaNano Nanomicroscopy Center (Aalto-NMC), and Micronova Nanofabrication Center. Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.

PY - 2023/4/28

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N2 - Electrochemical DNA (e-DNA) biosensors are feasible tools for disease monitoring, with their ability to translate hybridization events between a desired nucleic acid target and a functionalized transducer, into recordable electrical signals. Such an approach provides a powerful method of sample analysis, with a strong potential to generate a rapid time to result in response to low analyte concentrations. Here, we report a strategy for the amplification of electrochemical signals associated with DNA hybridization, by harnessing the programmability of the DNA origami method to construct a sandwich assay to boost charge transfer resistance (RCT) associated with target detection. This allowed for an improvement in the sensor limit of detection by two orders of magnitude compared to a conventional label-free e-DNA biosensor design and linearity for target concentrations between 10 pM and 1 nM without the requirement for probe labeling or enzymatic support. Additionally, this sensor design proved capable of achieving a high degree of strand selectivity in a challenging DNA-rich environment. This approach serves as a practical method for addressing strict sensitivity requirements necessary for a low-cost point-of-care device.

AB - Electrochemical DNA (e-DNA) biosensors are feasible tools for disease monitoring, with their ability to translate hybridization events between a desired nucleic acid target and a functionalized transducer, into recordable electrical signals. Such an approach provides a powerful method of sample analysis, with a strong potential to generate a rapid time to result in response to low analyte concentrations. Here, we report a strategy for the amplification of electrochemical signals associated with DNA hybridization, by harnessing the programmability of the DNA origami method to construct a sandwich assay to boost charge transfer resistance (RCT) associated with target detection. This allowed for an improvement in the sensor limit of detection by two orders of magnitude compared to a conventional label-free e-DNA biosensor design and linearity for target concentrations between 10 pM and 1 nM without the requirement for probe labeling or enzymatic support. Additionally, this sensor design proved capable of achieving a high degree of strand selectivity in a challenging DNA-rich environment. This approach serves as a practical method for addressing strict sensitivity requirements necessary for a low-cost point-of-care device.

KW - antimicrobial resistance gene

KW - DNA hybridization

KW - DNA nanotechnology

KW - electrochemical impedance spectroscopy

KW - point-of-care devices

KW - sensitivity enhancement

KW - target selectivity

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SP - 1471

EP - 1480

JO - ACS Sensors

JF - ACS Sensors

IS - 4

ER -

Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles

Abstract

Funding

Keywords

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Bioeconomy Research Infrastructure

OtaNano

OtaNano - Nanofab

DNA origami boosts electrochemical biosensor performance

Aalto University Reports Findings in DNA Biosensors (Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles)

Aalto University: DNA Origami Boosts Electrochemical Biosensor Performance

Cite this

Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Equipment

Bioeconomy Research Infrastructure

OtaNano

OtaNano - Nanofab

Press/Media

DNA origami boosts electrochemical biosensor performance

Aalto University Reports Findings in DNA Biosensors (Signal Amplification in Electrochemical DNA Biosensors Using Target-Capturing DNA Origami Tiles)

Aalto University: DNA Origami Boosts Electrochemical Biosensor Performance

Cite this