Tuning the electronic properties of MoSi2N4 by molecular doping: A first principles investigation

MoSi2N4 is a recently developed 2D material that exhibits remarkable thermal, mechanical, electronic, and optical properties. We used first principles calculations to study the structural and electronic properties of organic molecule doped MoSi2N4 monolayers. Effective p-doping was achieved by molecular doping with tetracyanoquinodimethane and tetracyanoethylene, while n-doping was achieved by molecular doping with tetrathiafulvalene. The doping gap of tetrathiafulvalene-doped MoSi2N4 was successfully modulated by the application of an external electric field, which resulted in effective n-doping. Furthermore, molecular doping injects additional carriers into the host, which is beneficial for enhancing the performance of MoSi2N4 in nanoelectronic devices. Our results demonstrate the importance of molecular doping in tuning the electronic properties of MoSi2N4 and broadening its applications.