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Download fileRandom Structure Searching with Orbital-Free Density Functional Theory
journal contribution
posted on 2021-02-15, 15:08 authored by William C. Witt, Benjamin W. B. Shires, Chuin Wei Tan, Wojciech J. Jankowski, Chris J. PickardThe properties of
a material depend on how its atoms are arranged,
and predicting these arrangements from first principles is a longstanding
challenge. Orbital-free density functional theory provides a quantum-mechanical
model based solely on the electron density, not individual wave functions.
The resulting speedups make it attractive for random structure searching,
whereby random configurations of atoms are relaxed to local minima
in the energy landscape. We use this strategy to map the low-energy
crystal structures of Li, Na, Mg, and Al at zero pressure. For Li
and Na, our searching finds numerous close-packed polytypes of almost-equal
energy, consistent with previous efforts to understand their low-temperature
forms. For Mg and Al, the searching identifies the expected ground
state structures unambiguously, in addition to revealing other low-energy
structures. This new role for orbital-free density functional theoryparticularly
as continued advances make it accurate for more of the periodic tablewill
expedite crystal structure prediction over wide ranges of compositions
and pressures.
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ground state structuresNaAlLiRandom Structurewave functionsOrbital-Free Density Functional Theoryelectron densitylow-energy crystal structuresquantum-mechanical modelclose-packed polytypesalmost-equal energyMgOrbital-free densitycrystal structure predictionlow-energy structuresorbital-free densityenergy landscape