ab initio Gutzwiller quantum molecular dynamics simulation of hydrogens under extreme conditions

Molecular dynamics (MD), a computer simulation method for studying the dynamical evolution of molecules and atoms, has achieved great success in the past decades and has been widely used in a variety of research fields. In particular, the ab initio molecular dynamics (AIMD) methods, in which the electron degrees of freedom are integrated out on the fly from first principles, have become the state-of-the-art tool for accurate modeling of physical phenomena and functional materials. In most AIMD simulations, the electronic structure problem is solved using the density functional theory (DFT). However, it is known that DFT fails to capture effects of strong electron correlation. To overcome this obstacle, here we present a novel AIMD scheme based on the Gutzwiller/slave-boson many-body technique, which has been shown to successfully describe the correlation-induced metal-insulator transitions. We applied our ab initio Gutzwiller MD to simulate the dissociation of hydrogen molecules in the high-pressure liquid phase. Our work sheds new light on the role of electron correlation in this intriguing liquid-liquid transition of hydrogens.