2020/07/31 by Daniel Wines, Kayahan Saritas, Can Ataca · 39 citations
Materials Science · Physics and Astronomy · #2D Materials and Applications #Density functional theory #Excited state #Exciton #GW approximation #Ground state #Heusler alloys: electronic and magnetic properties #Iron-based superconductors research #Lattice (music) #Perturbation theory (quantum mechanics) #Quantum Monte Carlo #Quasiparticle #cond-mat.mtrl-sci
paper · pdf · doi:10.1063/5.0023223
published in The Journal of Chemical Physics 153(15), 154704 (American Institute of Physics)
openalex created_date 2020/08/03 · openalex publication_date 2020/10/19 · arxiv created 2020/10/21 · arxiv updated 2020/10/22 · openalex updated_date 2026/08/06
Two-dimensional (2D) post-transition metal chalcogenides (PTMCs) have attracted attention due to their suitable bandgaps and lower exciton binding energies, making them more appropriate for electronic, optical, and water-splitting devices than graphene and monolayer transition metal dichalcogenides. Of the predicted 2D PTMCs, GaSe has been reliably synthesized and experimentally characterized. Despite this fact, quantities such as lattice parameters and band character vary significantly depending on which density functional theory (DFT) functional is used. Although many-body perturbation theory (GW approximation) has been used to correct the electronic structure and obtain the excited state properties of 2D GaSe, and solving the Bethe-Salpeter equation (BSE) has been used to find the optical gap, we find that the results depend strongly on the starting wavefunction. In an attempt to correct these discrepancies, we employed the many-body Diffusion Monte Carlo (DMC) method to calculate the ground and excited state properties of GaSe because DMC has a weaker dependence on the trial wavefunction. We benchmark these results with available experimental data, DFT [local-density approximation, Perdew-Burke-Ernzerhof (PBE), strongly constrained and appropriately normed (SCAN) meta-GGA, and hybrid (HSE06) functionals] and GW-BSE (using PBE and SCAN wavefunctions) results. Our findings confirm that monolayer GaSe is an indirect gap semiconductor (Γ-M) with a quasiparticle electronic gap in close agreement with experiment and low exciton binding energy. We also benchmark the optimal lattice parameter, cohesive energy, and ground state charge density with DMC and various DFT methods. We aim to present a terminal theoretical benchmark for pristine monolayer GaSe, which will aid in the further study of 2D PTMCs using DMC methods.