Heat reflux sonochemical synthesis of Cu3BiS3 quantum dots: Experimental and first-principles investigation of spin–orbit coupling on structural, electronic, and optical properties

Abstract

Semiconductor quantum dots (QD) exhibit promising electrical and optical properties in photovoltaic cells by improving their stability and efficiency enhancement. Therefore, in this study, novel Cu3BiS3 (CBS) ultrafine QDs were synthesized to function as effective solar absorbers, using a facile heat reflux sonochemical synthesis process under inert (N2) atmosphere. Using high-resolution transmission electron microscopy (HRTEM) analysis, the size of CBS QDs was found to be in the range of 3–8 nm. Furthermore, the crystallite size (D), strain (ε), and dislocation density (δ) of the QDs were investigated in detail by confirming the orthorhombic wittichenite structure. The photocurrent density (PCD) of CBS QDs obtained at a voltage range of 0.5–1 V was found between 0.2 and 0.6 mA/cm2 under illumination; otherwise, it has a linear nature and good ohmic behavior in the range of − 0.1 V to + 0.1 V. In additionally, the spin–orbit coupling (SOC) interaction was computed using the Perdew–Burke–Ernzerhof (PBE) and Tran-Blaha-modified Becke–Johnson (TB-mBJ) functionals in the density functional theory (DFT) framework. The results showed a bandgap transition from direct to indirect with the inclusion of SOC, as confirmed by the electronic band structure. Moreover, the DFT-calculated bandgap using the TB-mBJ functional (∼1 eV) achieved near consistency with the experimentally obtained bandgap (∼1.4 eV). Therefore, based on the experimental and computational results, this study can pave the way toward developing novel copper chalcogenide QDs for application in future photovoltaic cells.