Mass-zero constrained dynamics for density functional based ab-initio MD

The goal of this thesis is to develop the formalism for the extension of a newly developed approach to adiabatic quantum molecular dynamics, the mass-zero constrained dynamics (MaZe) method, to the framework of Kohn-Sham density functional theory (KS-DFT). Following on from this, we plan to carry out its implementation in a community code - namely Quantum Espresso - and leverage the support of GPUs by interfacing with the SIRIUS domain-specific library for electronic-structure calculations. After carrying out the implementation of MaZe within Quantum Espresso we shall perform similar tests and proof-of-principle calculations to those that have already been undertaken for the case of MaZe applied to orbital-free DFT for which there is an existing in-house code. This shall allow us to determine the extent of the computational speedup over alternative MD methods facilitated by MaZe. It is hoped that, subsequent to successful tests, we shall proceed to investigate a range of material properties via simulations that possess the ability to access longer timescales and larger system sizes than alternative methods have previously been capable of.

As an additional goal, we intend to continue with ongoing efforts to incorporate nuclear quantum effects into the orbital-free DFT based formulation of MaZe and in the future also include such capabilities in the KS-DFT version.