Abstract

We report the growth and transfer of centimeter-sized, epitaxial hexagonal boron nitride (h-BN) few-layer films using Ni(111) single-crystal substrates. The h-BN films were heteroepitaxially grown on 10 × 10 mm2 or 20 × 20 mm2 Ni(111) substrates using atmospheric pressure chemical vapor deposition with a single ammonia-borane precursor. The grown films were transferred to arbitrary substrates via an electrochemical delamination technique, and the remaining Ni(111) substrates were repeatedly re-used. A careful analysis of the growth parameters revealed that the crystallinity and area coverage of the h-BN films were mostly sensitive to the sublimation temperature of the ammonia-borane source. Moreover, various physical characterizations confirmed that the grown films exhibited the typical characteristics of hexagonal boron nitride layers over the entire area. Furthermore, the heteroepitaxial relationship between h-BN and Ni(111) and the overall crystallinity of the film were thoroughly investigated using a synchrotron radiation X-ray diffraction analysis including θ–2θ scans, grazing incident diffraction, and reciprocal space mapping. The crystallinity at the microscopic scale was further investigated using transmission electron microscopy (TEM)-based techniques, including selective area electron diffraction pattern mapping, electron back-scattered diffraction, and high-resolution TEM. Transparent and flexible ceramic films for electronic devices can now be made at centimetre scales by a low-cost technique. Hexagonal boron nitride (h-BN) crystals are attractive platforms for building next-generation circuits because their flat, graphite-like surfaces resist mechanical and chemical damage while offering excellent signal isolation. Gyu-Chul Yi from Seoul National University and colleagues have developed a way to improve large-scale manufacturing of these films using a reusable nickel template. Nickel has a surface structure that helps h-BN films grow with high crystallinity following chemical vapor deposition, but detaching the resulting ceramic layer has always proved troublesome. The Korean team solved this problem through an electrochemical delamination process that seamlessly separates h-BN films with dimensions up to 20 × 20 square millimetres using a stream of hydrogen bubbles. Centimeter-sized, epitaxial hexagonal boron nitride (h-BN) few-layer films were heteroepitaxially grown on Ni(111) single-crystal substrates using atmospheric pressure chemical vapor deposition with ammonia-borane single precursor. The grown films were transferred to arbitrary substrates via an electrochemical delamination technique, and the remaining Ni(111) substrates were repeatedly re-used. Over repeated growth and transfer after the initial annealing, no significant degradation of Ni(111) substrates was observed and the crystallinity of h-BN layers was reproduced reliably. The grown h-BN films showed typical physical characteristics of h-BN, with a high uniformity over a wide area. The large-area synthesis and transfer of atomically thin uniform epitaxial h-BN layers can be applied in various fields where high quality two-dimensional insulating layers are required.

Highlights

  • Hexagonal boron nitride (h-BN) is a dielectric insulator with a twodimensional layered structure

  • The as-grown h-BN films were spin-coated with poly(methyl methacrylate) (PMMA) and transferred onto foreign substrates using the electrochemical delamination method.[14,31]

  • The optimal source sublimation and growth temperatures were found to be important for synthesizing few-layered h-BN with full coverage and high crystallinity, while the cooling rate had a negligible role

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Summary

Introduction

Hexagonal boron nitride (h-BN) is a dielectric insulator with a twodimensional layered structure. The large-area h-BN layers prepared by chemical vapor deposition usually exhibit polycrystalline structures with a typical average grain size of several microns[12,13,14] or tens of microns.[15,16] Grain boundaries or dislocations in polycrystalline h-BN can affect its electronic or mechanical properties, resulting in a lower band gap energy, higher leakage current and poorer mechanical strength.[17,18,19,20] large-area single crystalline h-BN layers are desired to fully realize the potential advantages of h-BN in device applications To this end, efforts on controlling the size and direction of individual domains of h-BN have been reported;[15,16,21,22] obtaining large-scale single crystalline h-BN films remains challenging. We report the synthesis of epitaxial h-BN films on the centimeter scale while maintaining a low cost of production by re-using the Ni(111) substrates via electrochemical delamination

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