Ferrimagnetic semiconductor with a direct bandgap

Abstract

The direct bandgap nature of semiconductors is crucial for a wide range of optoelectronic devices and energy applications. These materials are mainly concentrated in hybrid organic–inorganic halide perovskites, III–V semiconductors, and monolayer transition metal dichalcogenides. Here, we report an AA′3B2B′2O12-type direct bandgap semiconductor CaCu3Fe2Ta2O12 using spin-polarized density functional theory calculations. The formation energy indicates that this material is thermodynamically preferred under a high-temperature and high-pressure synthetic route, similar to the analog CaCu3Fe2Nb2O12. Effective ferrimagnetic interaction occurs through the antiferromagnetic coupling between the A-site Cu and B-site Fe. More importantly, CaCu3Fe2Ta2O12 exhibits semiconducting behavior with a direct bandgap in the visible range, suggesting that AA′3B2B′2O12-type quadruple perovskites are potential candidate materials in photovoltaics as well as in optoelectronic devices.

Dielectric Relaxation and Magnetic Structure of A-Site-Ordered Perovskite Oxide Semiconductor CaCu3Fe2Ta2O12

“…To further confirm the electronic property of CaCu 3 Fe 2 Ta 2 O 12 , we measured the UV–vis diffuse reflectance spectra in Figures S1a and S1b in the Supporting Information. The experimental result suggests that CaCu 3 Fe 2 Ta 2 O 12 is a semiconductor and the band gap is approximately 1.77 eV, which is consistent with the theoretical calculation Figure S1c displays the temperature-dependent resistance and electrical resistivity of the compound.…”

Ferroelasticity, thermochromism, semi-conductivity, and ferromagnetism in a new layered perovskite: (4-fluorophenethylaminium)2[CuCl4]

“…Simultaneously, the electronic states of Cu exhibit spin characteristics that both of the spin-up and spin-down states of Cu-3d orbitals are partly occupied, confirming Cu 2+ with a 3d 9 electronic configuration. 58,59 That is, the layered Cu-Cl inorganic framework makes a dominant contribution to the energy band gap and ferromagnetism.…”

Research progress on quadruple perovskite oxides

“…128,129 When a 5d element is utilized to partially replace the B-site in quadruple perovskite oxides, generally a 3d-5d ordered distribution may be attained in the perovskite system, leading to a high spin ordering temperature. Furthermore, in contrast to the 3d electrons, the 5d electrons can result in several fascinating phenomena, such as half metallicity and high temperatures, 70,80,81 which are required for spintronic materials. Theoretical calculations have been conducted in tandem with experimental studies on quadruple perovskite oxides, enabling the theoretical analysis of their structural features and electronic structures.…”

“…The DFT based on quantum mechanics is the source of first-principles. Currently, numerous ab initio computations, including the DFT-based full potential linearized augmented plane-wave (FPLAPW) technique, 130,131 quantum Monte-Carlo simulation method, 82,132 spin-polarized first-principles calculations, 81,133,134 and DFT method with generalized gradient approximation (GGA) and GGA+U approximations, 133,135 have been developed to significant DOSs of the s, p-orbitals was found, suggesting less covalency between the Ca and O ions. 136 The computed electronic band structures and DOS with HSE06 for MnCu 3 Mn 4 O 12 are displayed in Fig.…”

“…AA′ 3 B 2 B′ 2 O 12 is an example of a quadruple perovskite that is mostly composed of FiM compounds, including CaCu 3 Mn 2 Os 2 O 12 , 32 NaCu 3 Fe 2 Os 2 O 12 (NCFOO), 80 CaCu 3 Fe 2 (Ta/Nb) 2 O 12 , 81 CCFRO, 73,82 LaCu 3 Co 2 Re 2 O 12 , 83 and LCFRO. 18 Among these perovskites, CCFRO and NCFOO have potential to be spintronic materials, showing spin-polarized properties with a transition above RT in the FiM spin magnetic structure.…”