Hexagonal Boron Nitride on Liquid and Single-Crystal Copper: Operando X-Ray and Atomistic Insights into Growth and Interfacial Structure
Abstract
Two-dimensional (2D) hexagonal boron nitride (hBN) is a key dielectric for van der Waals nanoelectronics, however, its controlled synthesis by chemical vapor deposition remains challenging and poorly understood. In this context, the growth of hBN on liquid metal catalysts is promising, as the atomically flat liquid surfaces are assumed to promote high-quality 2D growth, an expectation largely informed by graphene. Here, we implement an involved operando methodology to monitor and quantify hBN growth on molten copper (Liq-Cu) and re-solidified single-crystal copper (SC-Cu) under near-ambient-pressure conditions, enabling real-time identification of growth stages, morphology, and interfacial structure. Contrary to expectation, Liq-Cu promotes multilayer and three-dimensional domain formation, whereas SC-Cu predominantly yields monolayer-limited growth. This substrate-phase dependence correlates with a larger adsorption height of hBN on Liq-Cu than on SC-Cu, as determined by X-ray reflectivity and supported by machine-learning-accelerated molecular dynamics simulations. Direct comparison with graphene on Cu further reveals a distinct directional bonding character at the hBN/Cu interface, which rationalizes the observed adsorption-height trends. More generally, these trends across 2D materials and substrates identify the resulting interfacial stabilization – together with macroscopic factors such as precursor solubility – as a key design parameter governing mono- versus multilayer growth in 2D material synthesis.
Authors 17
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Leiden University · European Synchrotron Radiation Facility
Affiliation as printed
Leiden Institute of Chemistry
Leiden University
The European Synchrotron Radiation Facility (ESRF)
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European Synchrotron Radiation Facility
Affiliation as printed
The European Synchrotron Radiation Facility (ESRF)
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Fritz Haber Institute of the Max Planck Society
Affiliation as printed
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin, Germany, D-14195
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Affiliation as printed
School of Chemistry
University of Bristol
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European Synchrotron Radiation Facility · Université Grenoble Alpes
Affiliation as printed
The European Synchrotron Radiation Facility (ESRF)
Université Grenoble Alpes
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Commissariat à l'Énergie Atomique et aux Énergies Alternatives · Institut de Recherche Interdisciplinaire de Grenoble · Université Grenoble Alpes
Affiliation as printed
CEA
IRIG/MEM/NRS
Université Grenoble Alpes
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European Synchrotron Radiation Facility
Affiliation as printed
The European Synchrotron Radiation Facility (ESRF)
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Commissariat à l'Énergie Atomique et aux Énergies Alternatives · Laboratoire d'Électronique des Technologies de l'Information · Université Grenoble Alpes
Affiliation as printed
CEA
LETI
Université Grenoble Alpes
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University of Patras · Foundation for Research and Technology Hellas
Affiliation as printed
Department of Chemical Engineering
Foundation of Research and Technology Hellas
Institute of Chemical Engineering Sciences
University of Patras
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University of Patras · Foundation for Research and Technology Hellas
Affiliation as printed
Department of Chemical Engineering
Foundation of Research and Technology Hellas
Institute of Chemical Engineering Sciences
University of Patras
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European Synchrotron Radiation Facility
Affiliation as printed
The European Synchrotron Radiation Facility (ESRF)
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Commissariat à l'Énergie Atomique et aux Énergies Alternatives · Institut de Recherche Interdisciplinaire de Grenoble · Université Grenoble Alpes
Affiliation as printed
CEA
IRIG/MEM/NRS
Université Grenoble Alpes
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National Centre of Scientific Research "Demokritos"
Affiliation as printed
National Centre for Scientific Research Demokritos
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Fritz Haber Institute of the Max Planck Society
Affiliation as printed
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin, Germany, D-14195
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European Synchrotron Radiation Facility
Affiliation as printed
The European Synchrotron Radiation Facility (ESRF)
-
Fritz Haber Institute of the Max Planck Society
Affiliation as printed
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin, Germany, D-14195
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Affiliation as printed
Leiden Institute of Chemistry
Leiden University
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