Performance of the r2SCAN Functional in Transition Metal Oxides

Abstract

We assess the accuracy and computational efficiency of the recently developed meta-generalized gradient approximation (metaGGA) functional, restored regularized strongly constrained and appropriately normed (r²SCAN), in transition metal oxide (TMO) systems and compare its performance against SCAN. Specifically, we benchmark the r²SCAN-calculated oxidation enthalpies, lattice parameters, on-site magnetic moments, and band gaps of binary 3d TMOs against the SCAN-calculated and experimental values. Additionally, we evaluate the optimal Hubbard U correction required for each transition metal (TM) to improve the accuracy of the r²SCAN functional, based on experimental oxidation enthalpies, and verify the transferability of the U values by comparing against experimental properties on other TM-containing oxides. Notably, including the U-correction with r²SCAN increases the lattice parameters, on-site magnetic moments, and band gaps of TMOs, apart from an improved description of the ground state electronic state in narrow band gap TMOs. The r²SCAN and r²SCAN+U calculated oxidation enthalpies follow the qualitative trends of SCAN and SCAN+U, with r²SCAN and r²SCAN+U predicting marginally larger lattice parameters, smaller magnetic moments, and lower band gaps compared to SCAN and SCAN+U, respectively. We observe the overall computational time (i.e., for all ionic+electronic steps) required for r²SCAN(+U) to be lower than SCAN(+U). Thus, the r²SCAN(+U) framework can offer a reasonably accurate description of the ground state properties of TMOs with better computational efficiency than SCAN(+U).