Top-down synthesis and enhancing device adaptability of graphene quantum dots

Abstract

Quantum dots (QD) are rapidly making their way into several application sectors including optoelectronics, and there is a strong need to focus on non-toxic QDs. In this work, we have synthesized graphene QDs in the size range of 1.4-4.2 nm from inexpensive graphite by oxidative cleavage using a sulphuric and nitric acid mixture. A subsequent hydrogen peroxide oxidation step, investigated using two thermal budgets, has resulted in QDs with excellent photoluminescence (PL) intensity. Prolonged, higher temperature oxidation results in smaller size GQDs. X-ray photoelectron spectroscopy analysis confirmed the role of center dot OH radicals in the oxidation process and Raman analysis revealed that the higher thermal budget oxidation results in lower defect density. To overcome the challenges in device adaptability due to the inherent acidity in the QDs, a post-synthesis neutralization process was devised. The neutralized GQDs were formed into a film to be used as the active layer in a photodetector device. Fluorescence decay analysis showed there is no significant change in lifetime because of the film formation process. The fabricated GQD photodetector device exhibited high photocurrent under ultraviolet illumination with an ON/OFF ratio of 400% at an applied bias of +/- 1 V. The device performance underlines the high potential for the non-toxic, top-down synthesized GQDs for application in optoelectronic devices.