<p>Confinement epitaxy beneath graphene stabilizes exotic material phases by restricting vertical growth and altering lateral diffusion, conditions unattainable on bare substrates. However, achieving long-range interfacial order while maintaining high-quality graphene remains a significant challenge. Here, we demonstrate the synthesis of large-area quasi-free-standing monolayer graphene (QFMLG) via the intercalation of two-dimensional (2D) Sn. While the triangular Sn(1 × 1) interface exhibits a robust metallic band structure, the decoupled QFMLG maintains charge neutrality, confirmed by photoemission spectroscopy. Using high-resolution Raman spectroscopy and microscopy, we distinguish between direct intercalation and diffusion-driven expansion, identifying the latter as the critical pathway to superior QFMLG crystalline quality. Temperature-dependent analysis reveals dynamical structural coupling between the decoupled QFMLG and the Sn interface, providing a novel degree of freedom for strain engineering. Beyond uncovering the diffusion-driven mechanism, this work establishes metal intercalation as an effective strategy for tailoring durable graphene-metal heterostructures with tunable properties for next-generation quantum materials platforms.</p><p></p>

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Confinement epitaxy of large-area two-dimensional Sn at the graphene-SiC interface

  • Zamin Mamiyev,
  • Niclas Tilgner,
  • Narmina O. Balayeva,
  • Dietrich R. T. Zahn,
  • Thomas Seyller,
  • Christoph Tegenkamp

摘要

Confinement epitaxy beneath graphene stabilizes exotic material phases by restricting vertical growth and altering lateral diffusion, conditions unattainable on bare substrates. However, achieving long-range interfacial order while maintaining high-quality graphene remains a significant challenge. Here, we demonstrate the synthesis of large-area quasi-free-standing monolayer graphene (QFMLG) via the intercalation of two-dimensional (2D) Sn. While the triangular Sn(1 × 1) interface exhibits a robust metallic band structure, the decoupled QFMLG maintains charge neutrality, confirmed by photoemission spectroscopy. Using high-resolution Raman spectroscopy and microscopy, we distinguish between direct intercalation and diffusion-driven expansion, identifying the latter as the critical pathway to superior QFMLG crystalline quality. Temperature-dependent analysis reveals dynamical structural coupling between the decoupled QFMLG and the Sn interface, providing a novel degree of freedom for strain engineering. Beyond uncovering the diffusion-driven mechanism, this work establishes metal intercalation as an effective strategy for tailoring durable graphene-metal heterostructures with tunable properties for next-generation quantum materials platforms.