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Main Authors: Liang, Renhong, Ye, Mao, Ying, Yiran, Shu, Longlong, Zheng, Renkui, Huang, Haitao, Hao, Jianhua, Tong, Shuk-Yin, Ke, Shanming
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2603.09225
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author Liang, Renhong
Ye, Mao
Ying, Yiran
Shu, Longlong
Zheng, Renkui
Huang, Haitao
Hao, Jianhua
Tong, Shuk-Yin
Ke, Shanming
author_facet Liang, Renhong
Ye, Mao
Ying, Yiran
Shu, Longlong
Zheng, Renkui
Huang, Haitao
Hao, Jianhua
Tong, Shuk-Yin
Ke, Shanming
contents Controlling crystallographic orientation in quasi-van der Waals (vdW) epitaxy remains a fundamental challenge, especially for material systems located near the boundary between weakly and strongly coupled growth regimes. In such marginal systems, epitaxial selection is governed by a delicate thermodynamic competition between surface-energy penalties and interfacial interaction gains, giving rise to two archetypal limits: vdW-dominated free-epitaxy and strong interfacial coupling dominated locked-epitaxy. However, dynamically driving transitions between these regimes has remained elusive. Here, we demonstrate that external light irradiation can deterministically induce such a transition. Using the thermodynamically frustrated Fe4N/mica interface as a model system, we show that photo-excited carriers act as a chemical potentiator, significantly enhancing the interfacial chemical affinity. Within a quantitative thermodynamic description, this optical modulation increases the locking criterion (I_lock)-defined as the ratio of interfacial energy gain to surface-energy cost-beyond its critical threshold. As a result, the system switches from vdW-dominated free-epitaxy with (001) orientation to chemically locked-epitaxy with (111) orientation. Our findings establish light as a non-invasive and switchable control knob to dynamically reconfigure the interfacial energy landscape in quasi-vdW epitaxy, enabling programmable access to distinct epitaxial states beyond intrinsic material limitations.
format Preprint
id arxiv_https___arxiv_org_abs_2603_09225
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Optically driven thermodynamic transition from free- to locked-epitaxy
Liang, Renhong
Ye, Mao
Ying, Yiran
Shu, Longlong
Zheng, Renkui
Huang, Haitao
Hao, Jianhua
Tong, Shuk-Yin
Ke, Shanming
Materials Science
Controlling crystallographic orientation in quasi-van der Waals (vdW) epitaxy remains a fundamental challenge, especially for material systems located near the boundary between weakly and strongly coupled growth regimes. In such marginal systems, epitaxial selection is governed by a delicate thermodynamic competition between surface-energy penalties and interfacial interaction gains, giving rise to two archetypal limits: vdW-dominated free-epitaxy and strong interfacial coupling dominated locked-epitaxy. However, dynamically driving transitions between these regimes has remained elusive. Here, we demonstrate that external light irradiation can deterministically induce such a transition. Using the thermodynamically frustrated Fe4N/mica interface as a model system, we show that photo-excited carriers act as a chemical potentiator, significantly enhancing the interfacial chemical affinity. Within a quantitative thermodynamic description, this optical modulation increases the locking criterion (I_lock)-defined as the ratio of interfacial energy gain to surface-energy cost-beyond its critical threshold. As a result, the system switches from vdW-dominated free-epitaxy with (001) orientation to chemically locked-epitaxy with (111) orientation. Our findings establish light as a non-invasive and switchable control knob to dynamically reconfigure the interfacial energy landscape in quasi-vdW epitaxy, enabling programmable access to distinct epitaxial states beyond intrinsic material limitations.
title Optically driven thermodynamic transition from free- to locked-epitaxy
topic Materials Science
url https://arxiv.org/abs/2603.09225