Heterogeneities at multiple length scales in 2D layered materials: From localized defects and dopants to mesoscopic hete

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Heterogeneities at multiple length scales in 2D layered materials: From localized defects and dopants to mesoscopic heterostructures Hui Cai, Yiling Yu, Yu-Chuan Lin, Alexander A. Puretzky, David B. Geohegan, and Kai Xiao () Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 Received: 14 June 2020 / Revised: 7 August 2020 / Accepted: 10 August 2020

ABSTRACT Two-dimensional (2D) materials hold great promise for applications in optoelectronics, quantum information science, and energy conversion due to their remarkable properties imbued by their physical characteristics. Although heterogeneities in their intrinsic structure are the major challenges limiting their synthesis and predictable properties, they also provide a pathway to controllably tune the properties and broaden the potential of 2D materials. Heterogeneities that can be tailored, including defects, dopants, strain, edges, and layer stackings offer transformative opportunities in heterogeneous 2D materials through the introduction of novel properties for technological applications. This article provides a review of recent progress in studying heterogeneities in 2D materials. The review uses examples from our work to develop a strategy to understand the heterogeneities across multiple length scales to link the effect of heterogeneity at the nanoscale with the macroscale properties of 2D materials. We describe specific types of heterogeneities and explore novel synthesis and processing methods for their controlled production with example of the potential impact and applications enabled by their intriguing properties. Finally, we provide a perspective on how to extend the range of tunable properties through further engineering the heterogeneities in 2D materials.

KEYWORDS two-dimensional (2D) materials, heterogeneity, defect, strain, grain boundary, heterostructures, phase

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Introduction

Throughout the history of materials development and design, the pursuits of perfect materials via the elimination of harmful defects and impurities are goals that have been faced consistently by material scientists. The second law of thermodynamics ultimately limits such perfection in materials, so that every material inevitably contains some degree of heterogeneities. At the atomic level, these consist of point defects, dopants, impurities, and dislocations while at the mesoscopic level, there are grain boundaries, edges, stacking faults, strain, and surface adsorbates. On one hand, such heterogeneities can be debilitating for applications that rely upon the controllable, uniform, and large-scale synthesis of high-quality crystalline materials. On the other hand, when managed wisely, heterogeneities can provide opportunities to tailor material properties and functionalities and enable new and exciting applications. Perhaps the most famous example of this is the ability to dope Si as either a p-type or n-type semiconductor, enabling ge