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<p>We present a first-principles study of the structural, electronic, magnetic, thermodynamic and thermoelectric properties of the layered rare-earth nickelates Ce<sub>4</sub>Ni<sub>3</sub>O<sub>8</sub> and Pr<sub>4</sub>Ni<sub>3</sub>O<sub>8</sub> using the generalized gradient approximation (GGA)-Perdew–Burke–Ernzerhof (PBE) functional, modified Becke-Johnson (mBJ) functional, density functional theory with Hubbard U correction (DFT+U) and DFT with relativistic spin–orbit coupling (DFT+SOC) methods. The inclusion of on-site Coulomb interaction is essential to capture strong Ni-3d and Ce/Pr-4f correlations, leading to stabilization of a ferromagnetic metallic ground state, verified through total energy comparisons with antiferromagnetic configurations. The low-energy electronic structure is dominated by Ni-3d–O-2p hybridized states, while the rare-earth 4f states remain largely localized and are mainly affected by spin–orbit coupling. Thermodynamic properties are evaluated within the quasi-harmonic Debye model, indicating good lattice stability. Thermoelectric transport calculations using BoltzTraP2 show that ZT increases from 0.01 at 300&#xa0;K to 0.16 at 900&#xa0;K, consistent with correlated metallic behaviour. These results highlight the role of electronic correlations and magnetism in governing transport in Ce<sub>4</sub>Ni<sub>3</sub>O<sub>8</sub> and Pr<sub>4</sub>Ni<sub>3</sub>O<sub>8</sub>.</p>

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Electronic Correlations, Magnetic Ordering and Thermoelectric Properties of Rare-Earth Nickelates Ce4Ni3O8 and Pr4Ni3O8: A Theoretical Study

  • 期刊论文

  • 发表日期：

    2026年2月9日

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  • Surendra Singh Sengar,
  • Dinesh C. Gupta

摘要

We present a first-principles study of the structural, electronic, magnetic, thermodynamic and thermoelectric properties of the layered rare-earth nickelates Ce4Ni3O8 and Pr4Ni3O8 using the generalized gradient approximation (GGA)-Perdew–Burke–Ernzerhof (PBE) functional, modified Becke-Johnson (mBJ) functional, density functional theory with Hubbard U correction (DFT+U) and DFT with relativistic spin–orbit coupling (DFT+SOC) methods. The inclusion of on-site Coulomb interaction is essential to capture strong Ni-3d and Ce/Pr-4f correlations, leading to stabilization of a ferromagnetic metallic ground state, verified through total energy comparisons with antiferromagnetic configurations. The low-energy electronic structure is dominated by Ni-3d–O-2p hybridized states, while the rare-earth 4f states remain largely localized and are mainly affected by spin–orbit coupling. Thermodynamic properties are evaluated within the quasi-harmonic Debye model, indicating good lattice stability. Thermoelectric transport calculations using BoltzTraP2 show that ZT increases from 0.01 at 300 K to 0.16 at 900 K, consistent with correlated metallic behaviour. These results highlight the role of electronic correlations and magnetism in governing transport in Ce4Ni3O8 and Pr4Ni3O8.