Ran Adler edited workflow.tex  over 7 years ago

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The general procedure for structure prediction involves placing atoms in a unit cell and using a chosen algorithm to efficiently traverse the space of atomic configurations and cell geometries to arrive at low energy structures. This step requires having an accurate method for producing the energy of a given configuration of atoms. For weakly-correlated materials, DFT provides accurate energies, enabling successful structural prediction for novel compositions via searches within databases of known structures. This strategy was used to discover 54 new 18-valent ternary semiconductors~\cite{Gautier_2015} as well as two new structures in the Ce-Ir-In system~\cite{Fredeman_2011}. DFT has reached a high degree of stability and scalability, enabling software packages such as USPEX to implement genetic algorithms on top of DFT to successfully predict never before observed structures.  However, there are cases where DFT energies are insufficient for structure prediction: a notable failure is elemental plutonium, were where  paramagnetic DFT calculations underestimate the volume of the $\delta$ phase by roughly 25\% and magnetic calculations predict a large magnetic moment of 5$\mu_\text{B}$ which is not observed experimentally. Extending DFT by including orbital polarization--a correlation effect--brings the predictions in line with experiment. In general, for correlated materials, we argue that extensions to DFT capturing the effect of correlations on the total energy are important for structure prediction. The third step is \emph{global stability}: given the lowest energy structure of a fixed composition, check whether it is stable against decomposition to all other compositions in the chemical system. This requires knowledge of all other known stable compositions, their crystal structures and total energies, made possible by the construction of materials databases containing data in standardized computable formats, such as the Materials Project, AFLOWlib and NIMS. With this information, the energetic convex hull for a chemical system can be constructed and the target composition checked for stability.