Phase transitions of correlated systems from graph neural networks with quantum embedding techniques

Abstract

Correlated systems represent a class of materials that are difficult to describe through traditional electronic structure methods. The computational demand to simulate the structural dynamics of such systems, with correlation effects considered, is substantial. Here, we investigate the structural dynamics of $f$- and $d$-electron correlated systems by integrating quantum embedding techniques with interatomic potentials derived from graph neural networks. For Cerium, a prototypical correlated $f$-electron system, we use Density Functional Theory with the Gutzwiller approximation to generate training data due to efficiency with which correlations effects are included for large multi-orbital systems. For Nickel Oxide, a prototypical correlated $d$-electron system, advancements in computational capabilities now permit the use of full Dynamical Mean Field Theory to obtain energies and forces. We train neural networks on this data to create a model of the potential energy surface, enabling rapid and effective exploration of structural dynamics. Utilizing these potentials, we delineate transition pathways between the $\alpha$, ${\alpha }^{\prime }$, and ${\alpha }^{\prime \prime }$ phases of Cerium and predict the melting curve of Nickel Oxide. Our results demonstrate the potential of machine learning potentials to accelerate the study of strongly correlated systems, offering a scalable approach to explore and understand the complex physics governing these materials.

12 pages, 4 figures

References in corpus (43)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• The density-matrix renormalization group
• Implementation strategies in phonopy and phono3py
• A continuous-time solver for quantum impurity models
• A Universal Graph Deep Learning Interatomic Potential for the Periodic Table
• Hubbard-corrected DFT energy functionals: the LDA+U description of correlated systems
• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Dynamical Mean-Field Theory within the Full-Potential Methods: Electronic structure of Ce-115 materials
• Heavy Fermions and Quantum Phase Transitions
• Correlated Topological Insulators with Mixed Valence
• The Density Matrix Renormalization Group in Chemistry and Molecular Physics: Recent Developments and New Challenges
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• Free energy from stationary implementation of the DFT+DMFT functional
• LDA+Gutzwiller Method for Correlated Electron Systems: Formalism and Its Applications
• Orbital Selectivity in Hund's metals: The Iron Chalcogenides
• The $\gamma$-$\alpha$ iso-structural Transition in Cerium, a Critical Element
• Forces for Structural Optimizations in Correlated Materials within DFT+Embedded DMFT Functional Approach
• Covalency in transition metal oxides within all-electron Dynamical Mean Field Theory
• Applications of DFT+DMFT in Materials Science
• Gutzwiller density functional theory for correlated electron systems
• Equivalence of Gutzwiller and slave-boson mean-field theories for multi-band Hubbard models
• A Self-consistent DFT+DMFT scheme in the Projector Augmented Wave : Applications to Cerium, Ce2O3 and Pu2O3 with the Hubbard I solver and comparison to DFT+U
• Gutzwiller density functional calculations of the electronic structure of FeAs-based superconductors: Evidence for a three-dimensional Fermi surface
• Slave Boson Theory of Orbital Differentiation with Crystal Field Effects: Application to UO${}_2$
• Electronic structure of cerium: A comprehensive first-principles study
• A Novel Approach to Describe Chemical Environments in High Dimensional Neural Network Potentials
• Gutzwiller theory of band magnetism in LaOFeAs
• Spin-charge separation and many-body localization
• Pressure dependence of dynamically screened Coulomb interactions in NiO: Effective Hubbard, Hund, intershell and intersite components
• Tuning the Néel temperature in an antiferromagnet: the case of NixCo1-xO microstructures
• Electron correlation and spin density wave order in iron pnictides
• Many-body renormalisation of forces in f-electron materials
• DFT+DMFT study on soft moment magnetism and covalent bonding in SrRu${}_2$O${}_6$
• Melting curve of elemental zirconium
• Interplay of spin-orbit and entropic effects in Cerium
• Thermodynamics of volume collapse transitions in cerium and related compounds
• Thermodynamics of the $\alpha$-$\gamma$ transition in cerium studied by an LDA + Gutzwiller method
• Intermediate-pressure phases of cerium studied by an LDA + Gutzwiller method
• Topological Phase Transition in an Archetypal f-electron Correlated System: Ce
• Finite-Temperature Gutzwiller Approximation from Time-Dependent Variational Principle
• Phase Transition Pathway Sampling via Swarm Intelligence and Graph Theory
• Ab-initio Gutzwiller method: first application to Plutonium