Possibility of Combining Carbon Dots and Liquid Exfoliated Graphene as a Carbon-Based Light Addressable Potentiometric Sensor

A light addressable potentiometric sensor (LAPS) is a versatile sensing platform for bioassay. However, the lack of carbon-based LAPS (C-LAPS) is a bottleneck for its sustainable development in a carbon electronic era. Herein, a study of C-LAPS based on the combinations of carbon dots (CDs) and liquid exfoliated graphene (LEG) is presented. Devices of C-LAPS are first fabricated by self-assembling the hydrothermally synthesized CDs and the cosolvent ultrasonic delaminated LEG on poly(diallyldimethylammonium chloride) (PDDA)-modified indium tin oxide (ITO) glasses. According to the stacking orders of CDs and LEG, C-LAPS are named as CDs/LEG@PDDA/ITO and LEG/CDs@PDDA/ITO. Then, their electronic and photoelectronic features are measured and compared with the pure CD- and pure LEG-decorated ITO electrodes. Furthermore, working mechanisms are proposed by means of the classical theories of energy band bending and built-in electric field at the heterojunction of CDs and LEG. The resemblances of CDs/LEG@PDDA/ITO-based C-LAPS with Si-based LAPS (Si-LAPS) are confirmed from the points of view of production and separation of the photogenerated carriers, the formation of photocurrent, and the distinction with LEG/CDs@PDDA/ITO. Finally, its feasibility for biological application is justified by using the immune reaction of 5-methylcytosine (5mC) and its antibody (anti-5mC) as a proof of concept. The improved linear responses are evidenced by the comparisons with Si-LAPS' results. Conclusively, the proposed C-LAPS is believed to be a candidate for traditional semiconductor-based LAPS, with the merit of solution-processable. Meanwhile, the theoretical deductions about C-LAPS' principle can also pave the way for developing similar carbon-based sensors.