Quasicrystal bulk and surface energies from density functional theory

Abstract

Are quasicrystals stable or metastable? Density functional theory (DFT) is often used to evaluate thermodynamic stability, but quasicrystals are long-range aperiodic and their energies cannot be calculated using conventional ab initio methods. Here, we perform first-principles calculations on quasicrystal nanoparticles of increasing sizes, from which we can directly extrapolate their bulk and surface energies. Using this technique, we determine with high confidence that the icosahedral quasicrystals ScZn7.33 and YbCd5.7 are ground-state phases--revealing that translational symmetry is not a necessary condition for the T = 0 K stability of inorganic solids. Although we find the ScZn7.33 quasicrystal to be thermodynamically stable, we show on a mixed thermodynamic and kinetic phase diagram that its solidification from the melt is nucleation-limited, which illustrates why even stable materials may be kinetically challenging to grow. Our techniques here broadly open the door to first-principles investigations into the structure-bonding-stability relationships of aperiodic materials.

References in corpus (17)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Optimized norm-conserving Vanderbilt pseudopotentials
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• A Performance and Cost Assessment of Machine Learning Interatomic Potentials
• Precision and efficiency in solid-state pseudopotential calculations
• DynaPhoPy: A code for extracting phonon quasiparticles from molecular dynamics simulations
• DFT-FE -- A massively parallel adaptive finite-element code for large-scale density functional theory calculations
• Superconductivity and strong interactions in a tunable moiré quasiperiodic crystal
• Higher-order adaptive finite-element methods for Kohn-Sham density functional theory
• ESPEI for efficient thermodynamic database development, modification, and uncertainty quantification: application to Cu-Mg
• Discussion on clusters, phasons, and quasicrystal stabilisation
• Discovery of a binary icosahedral quasicrystal in Sc${}_{1}2$Zn${}_{8}8$
• Hidden Multiscale Order in the Primes
• Configurational forces in electronic structure calculations using Kohn-Sham density functional theory
• Spontaneous formation of thermodynamically stable Al--Cu--Fe icosahedral quasicrystal from realistic atomistic simulations
• A hard-sphere quasicrystal stabilized by configurational entropy
• Atomic diffusion due to hyperatomic fluctuation for quasicrystals