Quasiparticle and optical properties of phthalocyanine-TMD interfaces from first-principles GW-BSE

Heterogeneous interfaces formed between (metallo)phthalocyanine molecules and transition-metal dichalcogenides (TMDs) are both promising energy materials and excellent platforms for studying mixed-dimensional molecule-semiconductor heterostructures. First-principles calculations of the quasiparticle electronic structure and the optical properties at these interfaces are desired for a fundamental understanding of the energy and charge transfer. In this work, we employ the first-principles GW-BSE formalism to accurately characterize the quasiparticle and optical properties of a series of phthalocyanine-TMD interfaces. To reduce the computational cost, we leverage the substrate screening approximation and carry out dielectric embedding GW-BSE calculations. We discuss the dielectric screening effects of typical substrates used in experiments and the structure-property relationships derived from our calculations. Our results provide a microscopic description of the energy and charge transfer at these interfaces and benchmarks for future experimental and theoretical studies.