Correction to:npj Computational Materials https://doi.org/10.1038/s41524-023-01120-6,published online 21 October 2023 Current caption to Fig.4 reads“P–T phase diagram of MgSiO_(3)”.The correct caption should be“P...Correction to:npj Computational Materials https://doi.org/10.1038/s41524-023-01120-6,published online 21 October 2023 Current caption to Fig.4 reads“P–T phase diagram of MgSiO_(3)”.The correct caption should be“P–T phase diagram of Al”.The original article has been corrected.展开更多
Crystal structure prediction is a central problem of crystallography and materials science, which until mid-2000s was consideredintractable. Several methods, based on either energy landscape exploration or, more commo...Crystal structure prediction is a central problem of crystallography and materials science, which until mid-2000s was consideredintractable. Several methods, based on either energy landscape exploration or, more commonly, global optimization, largely solvedthis problem and enabled fully non-empirical computational materials discovery. A major shortcoming is that, to avoid expensivecalculations of the entropy, crystal structure prediction was done at zero Kelvin, reducing to the search for the global minimum ofthe enthalpy rather than the free energy. As a consequence, high-temperature phases (especially those which are not quenchableto zero temperature) could be missed. Here we develop an accurate and affordable solution, enabling crystal structure prediction atfinite temperatures. Structure relaxation and fully anharmonic free energy calculations are done by molecular dynamics with aforcefield (which can be anything from a parametric forcefield for simpler cases to a trained on-the-fly machine learning interatomicpotential), the errors of which are corrected using thermodynamic perturbation theory to yield accurate results with full ab initioaccuracy. We illustrate this method by applications to metals (probing the P–T phase diagram of Al and Fe), a refractory covalentsolid (WB), an Earth-forming silicate MgSiO_(3) (at pressures and temperatures of the Earth’s lower mantle), and ceramic oxide HfO_(2).展开更多
文摘Correction to:npj Computational Materials https://doi.org/10.1038/s41524-023-01120-6,published online 21 October 2023 Current caption to Fig.4 reads“P–T phase diagram of MgSiO_(3)”.The correct caption should be“P–T phase diagram of Al”.The original article has been corrected.
基金I.A.K.gratefully acknowledges the financial support from the Ministry of Science and Higher Education(Agreement No.075-15-2021-606)and from the Foundation for Assistance to Small Innovative Enterprises in Science and Technology(the UMNIK program)A.B.M.thanks the Russian Science Foundation(grant No.19-73-00237)for financial supportThe work of A.R.O.is supported by the Russian Science Foundation(grant 19-72-30043).
文摘Crystal structure prediction is a central problem of crystallography and materials science, which until mid-2000s was consideredintractable. Several methods, based on either energy landscape exploration or, more commonly, global optimization, largely solvedthis problem and enabled fully non-empirical computational materials discovery. A major shortcoming is that, to avoid expensivecalculations of the entropy, crystal structure prediction was done at zero Kelvin, reducing to the search for the global minimum ofthe enthalpy rather than the free energy. As a consequence, high-temperature phases (especially those which are not quenchableto zero temperature) could be missed. Here we develop an accurate and affordable solution, enabling crystal structure prediction atfinite temperatures. Structure relaxation and fully anharmonic free energy calculations are done by molecular dynamics with aforcefield (which can be anything from a parametric forcefield for simpler cases to a trained on-the-fly machine learning interatomicpotential), the errors of which are corrected using thermodynamic perturbation theory to yield accurate results with full ab initioaccuracy. We illustrate this method by applications to metals (probing the P–T phase diagram of Al and Fe), a refractory covalentsolid (WB), an Earth-forming silicate MgSiO_(3) (at pressures and temperatures of the Earth’s lower mantle), and ceramic oxide HfO_(2).
