Tuning the Surface Molecular Charge of Organic Photoelectrochemical Transistors with Significantly Improved Signal Resolution: A General Strategy toward Sensitive Bioanalysis

Abstract

Nature makes use of molecular charges to operate specific biological synthesis and reactions. Targeting advanced opto-bioelectronic sensors, organic photoelectrochemical transistors (OPECTs), taking advantage of the light fuel substituting an external gate potential, is now debuting and expected to serve as a universal platform for studying the rich light–biomatter interplay for new bioanalytics. Given the ubiquity of charged biomolecules in nature, molecular charge manipulation should underpin a generic route for innovative OPECT regulation and operation, which nevertheless has remained unachieved. Herein, this work manifests the biological tuning of surface charge toward the OPECT biosensor, which was exemplified by a light-sensitive CdS quantum dot (QD) gate electrode interfaced by a smart DNA superstructure with adenosine triphosphate (ATP) responsiveness. Highly negative-charged supramolecular DNA concatemers were self-assembled via sequential hybridization, and the ATP-triggered disassembly of the DNA concatemers would cause a tandem change of the effective gate voltage and transfer characteristics with significantly improved resolution. The present opto-bioelectronic device translates the events of charged molecules into amplified electrical signals and outlines a generic format for the future exploitation of rich biological tunability and light–biomatter interplay for innovative bioanalytics and beyond.

Dual Functional Conjugated Acetylenic Polymers: High-Efficacy Modulation for Organic Photoelectrochemical Transistors and Structural Evolution for Bioelectronic Detection

“…6.8 × 10 3 , which was higher than that of the previously reported OECT biosensors. 29,30,39,49,50 Such a high gain indicated the superior modulation effect of pDEB/NiO/FTO gate against the DETA de-doped PE-DOT:PSS channel and thus its remarkable capability to amplify the gate signals. To further unveil the gating effect, the transfer characteristics of pDEB/NiO/FTO and S-pDEB/ NiO/FTO were addressed.…”

Metallointercalated-DNA Nanotubes as Functional Light Antenna for Organic Photoelectrochemical Transistor Biosensor with Minimum Background

“…Photoelectrochemistry (PEC) has been a burgeoning technology in the field of advanced biosensing. − The intense interest in this arena arises from the advantages of semiconducting materials interfacing biological systems, the versatile interfacial interactions, and the reduced background due to the total separation and different energy types of the input (photons) and output (electrons) signals. Recent exploration of light-semiconductor-OECT interactions − has opened the light-controllable OECT with many new implementations and unknown possibilities. Among them, one of particular interest is the fusion between PEC and the OECT to realize an organic photoelectrochemical transistor (OPECT) with a minimum background, in which the rational light-matter interplay is of vital importance.…”

Biomolecules‐Incorporated Metal‐Organic Frameworks Gated Light‐Sensitive Organic Photoelectrochemical Transistor for Biodetection

“…Rational integration between the organic electrochemical transistor (OECT) [ 1–6 ] and photoelectrochemistry (PEC) [ 7–11 ] taking place in organic optoelectronics leads to the advanced light‐sensitive organic photoelectrochemical transistor (OPECT), which has been shown to be a versatile platform to study the rich light‐material‐bio interaction and to develop new light‐sensitive biosensors, [ 12–16 ] bioelectronics [ 17 ] and opto‐logics. [ 18 ] In such devices, semiconducting interfacial properties of light‐harvesting gates have been proven to be of intimate relevance to the potentiometric performance of devices, while the high accessibility of the semiconductors provides the possibility for biological interfacing.…”