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Abstract

Borophene-based van der Waals heterostructures have demonstrated enormous potential in the realm of optoelectronic and photovoltaic devices, which has sparked a wide range of interest. However, a thorough understanding of the microscopic excited-state electronic dynamics at interfaces is lacking, which is essential for determining the macroscopic optoelectronic and photovoltaic performance of borophene-based devices. In this study, photoexcited carrier dynamics of β₁₂, χ₃, and α΄ borophene/MoS2 heterostructures are systematically studied based on time-domain nonadiabatic molecular dynamics simulations. Different Schottky contacts are found in borophene/semiconductor heterostructures. The interplay between Schottky barriers, electronic coupling, and the involvement of different phonon modes collectively contribute to the unique carrier dynamics in borophene-based heterostructures. The diverse borophene allotropes within the heterostructures exhibit distinct and selective carrier transfer behaviors on an ultrafast timescale: electrons tunnel into α΄ borophene with an ultrafast transfer rate (≈29 fs) in α΄/MoS₂ heterostructures, whereas β₁₂ borophene only allows holes to migrate with a lifetime of 176 fs. The feature enables efficient charge separation and offers promising avenues for applications in optoelectronic and photovoltaic devices. This study provides insight into the interfacial carrier dynamics in borophene-based heterostructures, which is helpful in further design of advanced 2D boron-based optoelectronic and photovoltaic devices.