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We demonstrate a non-monotonic evolution of in-plane thermal conductivity of large-area hexagonal boron nitride films with thickness. Wrinkles and defects/impurities are present in these films. Raman spectroscopy, an optothermal non-contact technique, is employed to probe the temperature and laser power dependence property of the Raman active E2ghigh phonon mode, which, in turn, is used to estimate the rise in the temperature of the films under different laser powers. As the conventional Fourier law of heat diffusion cannot be directly employed analytically to evaluate the thermal conductivity of these films with defects and wrinkles, finite-element modeling is used instead. In the model, average heat resistance is used to incorporate an overall near-surface defect structure, and Voronoi cells with contact resistance at the cell boundaries are constructed to mimic the wrinkled domains. The effective in-plane thermal conductivity is estimated to be 87, 55, and 117 W/m K for the 2, 10, and 30 nm-thick films, respectively. We also present a quantitative estimation of the thermal resistance by defects and wrinkles individually to the heat flow. Our study reveals that the defects/impurities render a much higher resistance to heat transfer in the films than wrinkles. [ABSTRACT FROM AUTHOR]

Wafer-scale thin films of hexagonal boron nitride have exceptional thermal and mechanical properties, which harness the potential use of these materials in two-dimensional electronic, device applications. Along with unavoidable defects, grains, and wrinkles, which develop during the growth process, underlying substrates influence the physical and mechanical properties of these films. Understanding the interactions of these large-scale films with different substrates is, thus, important for the implementation of this 2D system in device fabrication. MOVPE-grown 2 and 30 nm hBN/sapphire films of size 2 in. diameter are delaminated chemically and transferred on quartz, SiO2/Si, and sapphire substrates. The structural characteristics of these films are investigated by employing Raman spectroscopy. Our results suggest that not only the roughness but also the height modulation at the surface of the substrates play a pivotal role in determining substrate-mediated mechanical strain inhomogeneity in these films. The statistical analysis of the spectral parameters provides us with the overall characteristics of the films. Furthermore, a Stark difference in the thermal evolution of strain in these films depending on substrate materials is observed. It has been demonstrated that not only the differential thermal expansion coefficient of the substrates and the films, but also slippage of the latter during the thermal treatment determines the net strain in the films. The role of the slippage is significantly higher in 2 nm films than in 30 nm films. We believe that the observations provide crucial information on the structural characteristics of the substrate-coupled wafer-scale hBN films for their future use in technology. [ABSTRACT FROM AUTHOR]