Quantum Monte Carlo Assessment of the Relevance of Electronic Correlations in Defects and EOS in Metals

摘要

We have developed a highly accurate computational capability to calculate the equation of state (EOS) and defect formation energies of metallic systems. We are using a newly developed algorithm that enables the study of metallic systems with quantum Monte Carlo (QMC) methods. To date, technical limitations have restricted the application of QMC methods to semiconductors, insulators and the homogeneous electron gas. Using this new 'QMC for metals' we can determine, for the first time, the significance of correlation effects in the EOS and in the formation energies of point defects, impurities, surfaces and interfaces in metallic systems. These calculations go beyond the state-of-the-art accuracy which is currently obtained with Density Functional Theory approaches. Such benchmark calculations can provide more accurate predictions for the EOS and the formation energies of vacancies and interstitials in simple metals. These are important parameters in determining the mechanical properties as well as the micro-structural evolution of metals in irradiated materials or under extreme conditions. We describe the development of our 'QMC for metals' code, which has been adapted to run efficiently on a variety of computer architectures including BG/L. We present results of the first accurate quantum Monte Carlo calculation of an EOS of a realistic metallic system that goes beyond the homogeneous electron gas.