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Abstract Heat dissipation is a major limitation of high‐performance electronics. This is especially important in emerging nanoelectronic devices consisting of ultra‐thin layers, heterostructures, and interfaces, where enhancement in thermal transport is highly desired. Here, ultra‐high interfacial thermal conductance in encapsulated van der Waals (vdW) heterostructures with single‐layer transition metal dichalcogenides MX₂(MoS₂, WSe₂, WS₂) sandwiched between two hexagonal boron nitride (hBN) layers is reported. Through Raman spectroscopic measurements of suspended and substrate‐supported hBN/MX₂/hBN heterostructures with varying laser power and temperature, the out‐of‐plane interfacial thermal conductance in the vertical stack is calibrated. The measured interfacial thermal conductance between MX₂and hBN reaches 74 ± 25 MW m⁻²K⁻¹, which is at least ten times higher than the interfacial thermal conductance of MX₂in non‐encapsulation structures. Molecular dynamics (MD) calculations verify and explain the experimental results, suggesting a full encapsulation by hBN layers is accounting for the high interfacial conductance. This ultra‐high interfacial thermal conductance is attributed to the double heat transfer pathways and the clean and tight vdW interface between two crystalline 2D materials. The findings in this study reveal new thermal transport mechanisms in hBN/MX₂/hBN structures and shed light on building novel hBN‐encapsulated nanoelectronic devices with enhanced thermal management. 

Two-dimensional (2-D) atomically thin graphene has exhibited overwhelming excellent properties over its bulk counterpart graphite, yet the broad applications and explorations of its unprecedented properties require a diversity of its geometric morphologies, beyond its inherently planar structures. In this study, we present a self-folding approach for converting 2-D planar free-standing graphene to 2-D and 3-D folded structures through the evaporation of its liquid solutions. This approach involves competition between the surface energy of the liquid, and the deformation energy and van der Waals energy of graphene. An energy-based theoretical model is developed to describe the self-folding process during liquid evaporation by incorporating both graphene dimensions and surface wettability. The critical elastocapillary length by liquid evaporation is extracted and exemplified by investigating three typical graphene geometries with rectangular, circular and triangular shapes. After the complete evaporation of the liquid, the critical self-folding length of graphene that can enable a stable folded pattern by van der Waals energy is also obtained. In parallel, full-scale molecular dynamics (MD) simulations are performed to monitor the evolution of deformation energies and folded patterns with liquid evaporation. The simulation results demonstrate the formation of 2-D folded racket-like and 3-D folded cone-like patterns and show remarkable agreement with theoretical predictions in both energy variations and folded patterns. This work offers quantitative guidance for controlling the self-folding of graphene and other 2-D materials into complex structures by liquid evaporation.