Title: Computational Studies and Algorithmic Research of Strongly Correlated Materials
Description: Strongly correlated materials are an important class of materials for research in condensed matter physics. Other than ordinary solid-state physical systems, which can be well described and analyzed by the energy band theory, the electron-electron correlation effects in strongly correlated materials are far more significant. So it is necessary to develop theories and methods that are beyond the energy band theory to describe their rich and varied behaviors. Not only are there electron-electron correlations, typically the multiple degrees of freedom in strongly correlated materials, such as charge distribution, orbital occupancies, spin orientations, and lattice structure exhibit cooperative or competitive behaviors, giving rise to rich phase diagrams and sensitive or non-perturbative responses to changes in external parameters such as temperature, strain, electromagnetic fields, etc. This thesis is divided into two parts. In the first part, we use the density functional theory (DFT) plus U correction, i.e., the DFT+U method, to calculate the equilibrium and nonequilibrium phase transitions of LuNiO3 and VO2.

The effect of adding U is manifested in both materials as the change of band structure in response to the change of orbital occupancies of electrons, i.e., the soft band effect. This effect bring about competitions of electrons between different orbitals by lowering the occupied orbitals and raising the empty orbitals in energy, giving rise to multiple metastable states. In the second part, we study the dynamic mean field theory (DMFT) as a beyond band-theory method. This is a Green's function based theory for open quantum systems. By selecting one lattice site of an interacting lattice model as an open system, the other lattice sites as the environment are equivalently replaced by a set of non-interaction orbitals according to the hybridization function, so the whole system is transformed into an Anderson impurity model. We studied how to use the density matrix renormalization group (DMRG) method to perform real-time evolutions of the Anderson impurity model to study the non-equilibrium dynamics of a strongly correlated lattice system.

We begin in Chapter 1 with an introduction to strongly correlated materials, density functional theory (DFT) and dynamical mean-field theory (DMFT). The Kohn-Sham density functional theory and its plus U correction are discussed in detail. We also demonstrate how the DMFT reduces the lattice sites other than the impurity site as a set of non-interacting bath orbitals. Then in Chapters 2 and 3, we show material-related studies of LuNiO3 as an example of rare-earth nickelates under substrate strain, and VO2 as an example of a narrow-gap Mott insulator in a pump-probe experiment. These are two types of strongly correlated materials with localized 3d orbitals (for Ni and V). We use the DFT+U method to calculate their band structures and study the structural phase transitions in LuNiO3 and metal-insulator transitions in both materials. The competition between the charge-ordered and Jahn-Teller distorted phases of LuNiO3 is studied at various substrate lattice constants within DFT+U. A Landau energy function is constructed based on group theory to understand the competition of various distortion modes of the NiO6 octahedra.

VO2 is known for its metal-insulator transition at 68 degree C, above which temperature it's a metal and below which it's an insulator with a doubled unit cell. For VO2 in a pump-probe experiment, a metastable metal phase was found to exist in the crystal structure of the equilibrium insulating phase. Our work is to understand this novel metastable phase from a soft-band picture. We also use quantum Boltzmann equation to justify the prethermalization of electrons over the lifetime of the metastable metal, so that the photoinduced transition can be understood in a hot electron picture. Finally, in Chapters 4 and 5, we show a focused study of building a real-time solver for the Anderson impurity model out of equilibrium using the density matrix renormalization group (DMRG) method, towards the goal of building an impurity solver for nonequilibrium dynamical mean-field theory (DMFT). We study both the quenched and driven single-impurity Anderson models (SIAM) in real time, evolving the wave function written in a form with 4 matrix product states (MPS) in DMRG.

For the quenched model, we find that the computational cost is polynomial time if the bath orbitals in the MPSs are ordered in energy. The same energy-ordering scheme works for the driven model in the short driving period regime in which the Floquet-Magnus expansion converges. In the long-period regime, we find that the computational time grows exponentially with the physical time, or the number of periods reached. The computational cost reduces in the long run when the bath orbitals are quasi-energy ordered, which is discussed in further detail in the thesis.