Underpinned exploration for magnetic structure, lattice dynamics, electronic properties, and disproportionation of yttrium nickelate

Magnetic behavior and disproportionation effect of nickelates are closely related to the nature of their ground state. In the present work, the magnetic structure, lattice dynamics, electronic properties, and disproportionation effect of yttrium nickelate (YNiO3) in its ground state P21/n structure were investigated by first-principles and phonon calculations based on density functional theory (DFT). The strong correlated interactions were treated by the DFT + U approach and the meta-generalized-gradient approximation approach implemented under the strongly constrained appropriately normed functional. The S-type antiferromagnetic insulating ground state of YNiO3 was captured well by both approaches. The disproportionation effect is quantitatively characterized through the Born effective charge, indicating the ligand-hole picture of Ni2+ → Ni2−δ+ Ni2+δ with δ = 0.3. The predicted phonon frequency at the Γ point agrees well with the measured value from infrared experiments, including the longitudinal and transverse optical splitting. The analysis based on stretching force constants indicated that the interaction between Ni and O atoms in the small nonmagnetic NiO6 octahedral clusters is stronger than that in the large magnetic NiO6 octahedral clusters.