Systematic dynamical mean-field theory study of 3d perovskite oxides with uniform Coulomb interactions

Original · EN

Strongly correlated transition-metal perovskite oxides pose a fundamental challenge for electronic-structure theory and for large-scale, data-driven materials discovery. While DFT+DMFT provides a quantitatively accurate description of such systems, its high-throughput application is hindered by the need to determine material-specific Coulomb interaction parameters (U). First-principles approaches such as the cRPA predict a highly nonlinear and non-transferable evolution of the interaction strength across chemically similar ABO₃ perovskites. Here we show that this paradigm does not extend to the large-energy-window eDMFT, which employs highly localized orbitals and treats electronic correlations and screening self-consistently within the same many-body framework. As a result, spectral properties are governed primarily by the dynamical self-energy rather than by static interaction-induced energy shifts. Recent constrained-eDMFT calculations demonstrated that, for broad classes of 3d transition-metal oxides, the self-consistently screened Coulomb interactions naturally fall within relatively narrow ranges for correlated metals and insulators. Motivated by these findings, we implement a high-throughput eDMFT framework employing physically derived interaction values of U=6 eV for metals and U=10 eV for insulators together with exact double counting. We test this framework using systematic high-throughput eDMFT calculations for ABO₃ compounds (A = Ca, Sr, La; B = V--Ni) and benchmark the resulting spectral functions against photoemission experiments, where we find overall excellent agreement. Our results establish that charge self-consistent eDMFT enables robust, parameter-tuning-free high-throughput many-body calculations for correlated oxides, opening a practical pathway toward predictive electronic-structure databases for strongly correlated materials.