Topic:
We have developed chemically accurate pseudo-Hamiltonians for correlated elements that overcome localization errors in diffusion Monte Carlo (DMC). This approach offers a systematic improvement in the accuracy of many body calculations of correlated quantum materials with DMC since only fixed-node errors remain outstanding.
High-level quantum chemistry methods were used to optimize localization error-free pseudo-Hamiltonians for 3d transition metals. The potentials perform like the best state-of-the-art semi-local potentials used by quantum chemistry methods, while, in addition, removing localization errors from DMC. Effective cores of this type have the potential to become state-of-the-art in DMC calculations of correlated and topological materials and further increase the predictive power of these high-level methods in materials science. DOI: 10.1021/acs.jctc.1c00992
