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Main Authors: Liang, Renhong, Ye, Mao, Zheng, Renkui, Hao, Jianhua, Huang, Haitao, Shu, Longlong, Ke, Shanming
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2512.21833
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author Liang, Renhong
Ye, Mao
Zheng, Renkui
Hao, Jianhua
Huang, Haitao
Shu, Longlong
Ke, Shanming
author_facet Liang, Renhong
Ye, Mao
Zheng, Renkui
Hao, Jianhua
Huang, Haitao
Shu, Longlong
Ke, Shanming
contents van der Waals (vdW) epitaxy is conventionally regarded as a rotation-free and strain-free growth mode driven by weak, isotropic interactions, yet many interfaces paradoxically exhibit strictly locked orientations that defy standard surface-energy models. We resolve this inconsistency by establishing a unified quantitative framework for 2D-3D systems, in which strong electrostatic and chemical interactions compete with entropic forces. We introduce a two-tier descriptor set-the predictive index (I_pre) and the thermodynamic locking criterion (I_lock)-to quantify the energetic sufficiency for locked epitaxy. Our theory accurately predicted the competitive interactions at the interface within the 2D-3D system, precisely characterized whether the epitaxial layer underwent free growth or was constrained in a locked growth mode, demonstrating robust consistency with diverse experimental observations. This framework unifies orientation selection in 3D-on-2D films and rotational locking in 2D-on-3D layers within a single-phase diagram. Our work provides a generalizable, predictive route to controlling epitaxial orientation across a broad spectrum of layered heterostructure
format Preprint
id arxiv_https___arxiv_org_abs_2512_21833
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Universal thermodynamic framework for quasi-van der Waals epitaxy
Liang, Renhong
Ye, Mao
Zheng, Renkui
Hao, Jianhua
Huang, Haitao
Shu, Longlong
Ke, Shanming
Materials Science
van der Waals (vdW) epitaxy is conventionally regarded as a rotation-free and strain-free growth mode driven by weak, isotropic interactions, yet many interfaces paradoxically exhibit strictly locked orientations that defy standard surface-energy models. We resolve this inconsistency by establishing a unified quantitative framework for 2D-3D systems, in which strong electrostatic and chemical interactions compete with entropic forces. We introduce a two-tier descriptor set-the predictive index (I_pre) and the thermodynamic locking criterion (I_lock)-to quantify the energetic sufficiency for locked epitaxy. Our theory accurately predicted the competitive interactions at the interface within the 2D-3D system, precisely characterized whether the epitaxial layer underwent free growth or was constrained in a locked growth mode, demonstrating robust consistency with diverse experimental observations. This framework unifies orientation selection in 3D-on-2D films and rotational locking in 2D-on-3D layers within a single-phase diagram. Our work provides a generalizable, predictive route to controlling epitaxial orientation across a broad spectrum of layered heterostructure
title Universal thermodynamic framework for quasi-van der Waals epitaxy
topic Materials Science
url https://arxiv.org/abs/2512.21833