Why a Diffusing Single-Molecule can be Detected in Few Minutes by a Large Capturing Bioelectronic Interface

Eleonora Macchia; Liberato De Caro; Fabrizio Torricelli; Cinzia Di Franco; Giuseppe Felice Mangiatordi; Gaetano Scamarcio; Luisa Torsi

doi:10.1002/advs.202104381

Why a Diffusing Single-Molecule can be Detected in Few Minutes by a Large Capturing Bioelectronic Interface

Eleonora Macchia, Liberato De Caro, Fabrizio Torricelli, Cinzia Di Franco, Giuseppe Felice Mangiatordi, Gaetano Scamarcio^*, Luisa Torsi ^*

^*Corresponding author for this work

Physics

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

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Abstract

Single-molecule detection at a nanometric interface in a femtomolar solution, can take weeks as the encounter rate between the diffusing molecule to be detected and the transducing nanodevice is negligibly small. On the other hand, several experiments prove that macroscopic label-free sensors based on field-effect-transistors, engaging micrometric or millimetric detecting interfaces are capable to assay a single-molecule in a large volume within few minutes. The present work demonstrates why at least a single molecule out of a few diffusing in a 100 µL volume has a high probability to hit a large capturing and detecting electronic interface. To this end, sensing data, measured with an electrolyte-gated FET whose gate is functionalized with 10¹² capturing anti-immunoglobulin G, are here provided along with a Brownian diffusion-based modeling. The EG-FET assays solutions down to some tens of zM in concentrations with volumes ranging from 25 µL to 1 mL in which the functionalized gates are incubated for times ranging from 30 s to 20 min. The high level of accordance between the experimental data and a model based on the Einstein's diffusion-theory proves how the single-molecule detection process at large-capturing interfaces is controlled by Brownian diffusion and yet is highly probable and fast.

Original language	English
Article number	2104381
Journal	Advanced Science
Volume	9
Issue number	20
DOIs	https://doi.org/10.1002/advs.202104381
Publication status	Published - 6 May 2022
MoE publication type	A1 Journal article-refereed

Funding

E.M. and L.D.C. contributed equally to this work. David Walt is acknowledged for useful discussions. SiMBiT – Single molecule bio‐electronic smart system array for clinical testing (Grant Agreement ID: MIUR PON grants e‐DESIGN (ARS01_01158); PMGB (ARS01_01195); IDF SHARID (ARS01_01270) 824946), Academy of Finland Project Nos. 316881 and 316883 “‘Spatiotemporal control of Cell Functions,’” No. 332106 “ProSiT – Protein Detection at the Single‐Molecule Limit with a Self‐powered Organic Transistor for HIV early diagnosis,” Åbo Akademi University CoE “Bioelectronic activation of cell functions,” “A binary sensor with single‐molecule digit to discriminate biofluids enclosing zero or at least one biomarker” (NoOne) (Grant Agreement ID 101040383), and CSGI are acknowledged for partial financial support.

Keywords

electrolyte-gated field-effect transistor
large-capturing interface
organic bioelectronics
single-molecule detection

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Advanced Science - 2022 - Macchia - Why a Diffusing Single‐Molecule can be Detected in Few Minutes by a Large CapturingFinal published version, 826 KBLicence: CC BY

https://urn.fi/URN:NBN:fi-fe2023021627450

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abstract = "Single-molecule detection at a nanometric interface in a femtomolar solution, can take weeks as the encounter rate between the diffusing molecule to be detected and the transducing nanodevice is negligibly small. On the other hand, several experiments prove that macroscopic label-free sensors based on field-effect-transistors, engaging micrometric or millimetric detecting interfaces are capable to assay a single-molecule in a large volume within few minutes. The present work demonstrates why at least a single molecule out of a few diffusing in a 100 µL volume has a high probability to hit a large capturing and detecting electronic interface. To this end, sensing data, measured with an electrolyte-gated FET whose gate is functionalized with 1012 capturing anti-immunoglobulin G, are here provided along with a Brownian diffusion-based modeling. The EG-FET assays solutions down to some tens of zM in concentrations with volumes ranging from 25 µL to 1 mL in which the functionalized gates are incubated for times ranging from 30 s to 20 min. The high level of accordance between the experimental data and a model based on the Einstein's diffusion-theory proves how the single-molecule detection process at large-capturing interfaces is controlled by Brownian diffusion and yet is highly probable and fast.",

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author = "Eleonora Macchia and \{De Caro\}, Liberato and Fabrizio Torricelli and Franco, \{Cinzia Di\} and Mangiatordi, \{Giuseppe Felice\} and Gaetano Scamarcio and Luisa Torsi",

note = "Funding Information: E.M. and L.D.C. contributed equally to this work. David Walt is acknowledged for useful discussions. SiMBiT – Single molecule bio‐electronic smart system array for clinical testing (Grant Agreement ID: MIUR PON grants e‐DESIGN (ARS01\_01158); PMGB (ARS01\_01195); IDF SHARID (ARS01\_01270) 824946), Academy of Finland Project Nos. 316881 and 316883 “{\textquoteleft}Spatiotemporal control of Cell Functions,{\textquoteright}” No. 332106 “ProSiT – Protein Detection at the Single‐Molecule Limit with a Self‐powered Organic Transistor for HIV early diagnosis,” {\AA}bo Akademi University CoE “Bioelectronic activation of cell functions,” “A binary sensor with single‐molecule digit to discriminate biofluids enclosing zero or at least one biomarker” (NoOne) (Grant Agreement ID 101040383), and CSGI are acknowledged for partial financial support. Publisher Copyright: {\textcopyright} 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.",

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AU - Franco, Cinzia Di

AU - Mangiatordi, Giuseppe Felice

AU - Scamarcio, Gaetano

AU - Torsi , Luisa

N1 - Funding Information: E.M. and L.D.C. contributed equally to this work. David Walt is acknowledged for useful discussions. SiMBiT – Single molecule bio‐electronic smart system array for clinical testing (Grant Agreement ID: MIUR PON grants e‐DESIGN (ARS01_01158); PMGB (ARS01_01195); IDF SHARID (ARS01_01270) 824946), Academy of Finland Project Nos. 316881 and 316883 “‘Spatiotemporal control of Cell Functions,’” No. 332106 “ProSiT – Protein Detection at the Single‐Molecule Limit with a Self‐powered Organic Transistor for HIV early diagnosis,” Åbo Akademi University CoE “Bioelectronic activation of cell functions,” “A binary sensor with single‐molecule digit to discriminate biofluids enclosing zero or at least one biomarker” (NoOne) (Grant Agreement ID 101040383), and CSGI are acknowledged for partial financial support. Publisher Copyright: © 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.

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N2 - Single-molecule detection at a nanometric interface in a femtomolar solution, can take weeks as the encounter rate between the diffusing molecule to be detected and the transducing nanodevice is negligibly small. On the other hand, several experiments prove that macroscopic label-free sensors based on field-effect-transistors, engaging micrometric or millimetric detecting interfaces are capable to assay a single-molecule in a large volume within few minutes. The present work demonstrates why at least a single molecule out of a few diffusing in a 100 µL volume has a high probability to hit a large capturing and detecting electronic interface. To this end, sensing data, measured with an electrolyte-gated FET whose gate is functionalized with 1012 capturing anti-immunoglobulin G, are here provided along with a Brownian diffusion-based modeling. The EG-FET assays solutions down to some tens of zM in concentrations with volumes ranging from 25 µL to 1 mL in which the functionalized gates are incubated for times ranging from 30 s to 20 min. The high level of accordance between the experimental data and a model based on the Einstein's diffusion-theory proves how the single-molecule detection process at large-capturing interfaces is controlled by Brownian diffusion and yet is highly probable and fast.

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Why a Diffusing Single-Molecule can be Detected in Few Minutes by a Large Capturing Bioelectronic Interface

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