Lone pair driven anisotropy in antimony chalcogenide semiconductors

Abstract

Antimony sulfide (Sb2S3) and selenide (Sb2Se3) have emerged as promising earth-abundant alternatives among thin-film photovoltaic compounds. A distinguishing feature of these materials is their anisotropic crystal structures, which are composed of quasi-one-dimensional (1D) [Sb4X6]n ribbons. The interaction between ribbons has been reported to be van der Waals (vdW) in nature and Sb2X3 are thus commonly classified in the literature as 1D semiconductors. However, based on first-principles calculations, here we show that inter-ribbon interactions are present in Sb2X3 beyond the vdW regime. The origin of the anisotropic structures is related to the stereochemical activity of the Sb 5s lone pair according to electronic structure analysis. The impacts of structural anisotropy on the electronic and optical properties are further examined, including the presence of higher dimensional Fermi surfaces for charge carrier transport. Our study provides guidelines for optimising the performance of Sb2X3-based solar cells via device structuring based on the underlying crystal anisotropy.

References in corpus (13)

• Double-slit photoelectron interference in strong-field ionization of the neon dimer
• BoltzTraP. A code for calculating band-structure dependent quantities
• Van der Waals density functionals applied to solids
• Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
• Van der Waals bonding in layered compounds from advanced first-principles calculations
• Efficient calculation of carrier scattering rates from first principles
• Low Hole Effective Mass p-type Transparent Conducting Oxides: Identification and Design Principles
• GW quasiparticle band structures of stibnite, antimonselite, bismuthinite, and guanajuatite
• First principles prediction of the elastic, electronic, and optical properties of Sb2S3 and Sb2Se3 compounds
• High-Mobility Bismuth-based Transparent P-Type Oxide from High-throughput Material Screening
• Impact of non-parabolic electronic band structure on the optical and transport properties of photovoltaic materials
• First-principles study of the lattice dynamics of Sb2S3
• Rapid Recombination by Cadmium Vacancies in CdTe

Cited by in corpus (9)

• Identifying the ground state structures of point defects in solids
• Upper efficiency limit of Sb2Se3 solar cells
• Band Versus Polaron: Charge Transport in Antimony Chalcogenides
• Impact of metastable defect structures on carrier recombination in solar cells
• Sulfur Vacancies Limit the Open-circuit Voltage of Sb2S3 Solar Cells
• Four-electron Negative-U Vacancy Defects in Antimony Selenide
• Strong electron-phonon coupling and carrier self-trapping in Sb${}_2$S${}_3$
• Heteroepitaxial growth of highly anisotropic $S{b}_{2}S{e}_3$ films on GaAs
• Tilt-induced charge localisation in phosphide antiperovskite photovoltaics