Van der Waals template–encoded soft epitaxy of tellurium enabled by atomic layer deposition

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Abstract
Van der Waals (vdW) epitaxy can integrate lattice-mismatched crystals with atomically sharp, pristine interfaces. However, translating this concept to atomic layer deposition (ALD), a standard for low-temperature, layer-by-layer growth, remains challenging because precursors adsorb transiently on chemically inert vdW basal planes, leading to physisorption-limited nucleation and poor crystalline ordering. Here, we introduce diffusion-steered epitaxial ALD (Epi-ALD), redefining vdW surfaces as programmable kinetic-thermodynamic landscapes and demonstrate highly crystalline tellurium at 150°C. Epi-ALD couples surface-potential-encoded physisorption with long-range diffusion to promote ordered nucleation and epitaxial alignment. This “soft” pathway enables strain-free tellurium epitaxy with a pristine vdW gap (∼1.4 angstrom) despite lattice mismatch (>3.6%) and generalizes across multiple vdW templates. Retaining hallmark advantages of ALD including scalability and uniformity, we further program in-plane orientation through vdW symmetry engineering to achieve quasi-single-crystalline tellurium films with pronounced anisotropy and a chiral anomaly signature. Our work establishes a universal, low-thermal-budget approach for integrating vdW materials and expands the scope of epitaxy within the ALD paradigm.
Funding Information
  • National Science Foundation (NSF-CBET 2330110)
  • National Science Foundation (FUSE2329111, CMMI-2239545)
  • National Science Foundation (FUSE2329111, CMMI-2239545)
  • U.S. Department of Energy (DOE-SC0020653)
  • Welch Foundation (C-2065, X-C-0011)
  • Welch Foundation (C-2065, X-C-0011)
  • National Research Foundation of Korea (RS-2025-12602968, RS-2024-00336695, RS-2025-12602968, RS-2025-23323754)
  • National Research Foundation of Korea (RS-2024-00406422)
  • Applied Materials
  • Samsung Research Funding & Incubation Center of Samsung Electronics (SRFC-MA2401-01)
  • National Research Foundation of Korea (RS-202523323228)
  • National Research Council of Science and Technology (GTL24041-000)
  • National Research Council of Science and Technology (GTL24041-000)
  • National Research Foundation of Korea (RS-202523323228)

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