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2D materials have attracted broad attention from researchers for their unique electronic proper-ties, which may be been further enhanced by combining 2D layers into vertically stacked van der Waals heterostructures. Among the superlative properties of 2D systems, thermoelectric energy (TE) conversion promises to enable targeted energy conversion, localized thermal management, and thermal sensing. However, TE conversion efficiency remains limited by the inherent tradeoff between conductivity and thermopower. In this paper, we use first-principles calculation to study graphene-based van der Waals heterostructures (vdWHs) composed of graphene layers and hexagonal boron nitride (h-BN). We compute the electronic band structures of heterostructured systems using Quantum Espresso and their thermoelectric (TE) properties using BoltzTrap2. Our results have shown that stacking layers of these 2D materials opens a bandgap, increasing it with the number of h-BN interlayers, which significantly improves the power factor (PF). We predict a PF of ~1.0x10 11 W/K 2 .m.s for the vdWHs, nearly double compared to 5x10 10 W/K 2 .m.s that we obtained for single-layer graphene. This study gives important information on the effect of stacking layers of 2D materials and points toward new avenues to optimize the TE properties of vdWHs. 

Abstract Owing to its superlative carrier mobility and atomic thinness, graphene exhibits great promise for interconnects in future nanoelectronic integrated circuits. Chemical vapor deposition (CVD), the most popular method for wafer-scale growth of graphene, produces monolayers that are polycrystalline, where misoriented grains are separated by extended grain boundaries (GBs). Theoretical models of GB resistivity focused on small sections of an extended GB, assuming it to be a straight line, and predicted a strong dependence of resistivity on misorientation angle. In contrast, measurements produced values in a much narrower range and without a pronounced angle dependence. Here we study electron transport across rough GBs, which are composed of short straight segments connected together into an extended GB. We found that, due to the zig-zag nature of rough GBs, there always exist a few segments that divide the crystallographic angle between two grains symmetrically and provide a highly conductive path for the current to flow across the GBs. The presence of highly conductive segments produces resistivity between 10 2 to 10 4 Ω μ m regardless of misorientation angle. An extended GB with large roughness and small correlation length has small resistivity on the order of 10 3 Ω μ m, even for highly mismatched asymmetric GBs. The effective slope of the GB, given by the ratio of roughness and lateral correlation length, is an effective universal quantifier for GB resistivity. Our results demonstrate that the probability of finding conductive segments diminishes in short GBs, which could cause a large variation in the resistivity of narrow ribbons etched from polycrystalline graphene. We also uncover spreading resistance due to the current bending in the grains to flow through the conductive segments of the GB and show that it scales linearly with the grain resistance. Our results will be crucial for designing graphene-based interconnects for future integrated circuits.