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自上而下合成与增强石墨烯量子点器件适应性。

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

机构信息

Department of Electrical and Computer Engineering, University of Waterloo, Waterloo, Canada.

Department of Mechanical and Mechatronics Engineering, University of Waterloo, Waterloo, Canada.

出版信息

Nanotechnology. 2023 Feb 16;34(18). doi: 10.1088/1361-6528/acb7fb.

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 ·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.

摘要

量子点(QD)正在迅速进入包括光电学在内的多个应用领域,因此强烈需要关注无毒的 QD。在这项工作中,我们使用硫酸和硝酸混合物通过氧化裂解,从廉价的石墨中合成了尺寸在 1.4-4.2nm 之间的石墨烯 QD。随后使用两种热预算对后续的过氧化氢氧化步骤进行了研究,结果得到了具有优异光致发光(PL)强度的 QD。延长、更高的温度氧化会导致更小尺寸的 GQD。X 射线光电子能谱分析证实了·OH 自由基在氧化过程中的作用,拉曼分析表明,更高的热预算会导致更低的缺陷密度。为了克服由于 QD 固有的酸性而导致的器件适应性挑战,设计了一种合成后中和过程。中和后的 GQD 被制成薄膜,用作光电探测器器件的有源层。荧光衰减分析表明,由于薄膜形成过程,寿命没有明显变化。所制造的 GQD 光电探测器器件在紫外光照射下表现出高光电流,在 ±1V 的偏置电压下,ON/OFF 比为 400%。该器件的性能突显了无毒、自上而下合成的 GQD 在光电设备中的高应用潜力。

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