Orbital-free density functional theory (OFDFT) simulations are orders of magnitude faster than those based on Kohn-Sham density functional theory because of the theoretical simplicity of the former that merely involves variationally optimizing the electron density rather than wavefunctions. However, the lack of one-electron wavefunctions (orbitals) in practice limits the accuracy of OFDFT because of the need to employ (i) a kinetic energy density functional (KEDF) to evaluate the kinetic energy of the electrons and (ii) normally a local pseudopotential (LPS) to account for the electron-ion (screened nucleus) interaction. We start with a bit of history of our earlier contributions to improve the accuracy, generality, and speed of OFDFT implementations, followed updates on recent advances, including a global optimization algorithm to efficiently construct LPSs, an open-source library of KEDFs that work with gpus as well as cpus, and new approaches to KEDFs and angular-momentum-dependent OFDFT.

Advances in orbital-free density functional theory simulations of materials

255th National Meeting (2018)

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