skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Toward a predictive theory of correlated materials

Abstract

Correlated electron materials display a rich variety of notable properties ranging from unconventional superconductivity to metal-insulator transitions. These properties are of interest from the point of view of applications but are hard to treat theoretically, as they result from multiple competing energy scales. Although possible in more weakly correlated materials, theoretical design and spectroscopy of strongly correlated electron materials have been a difficult challenge for many years. In this paper, by treating all the relevant energy scales with sufficient accuracy, complementary advances in Green’s functions and quantum Monte Carlo methods open a path to first-principles computational property predictions in this class of materials.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Computational Sciences and Engineering Division. Center for Nanophase Materials Sciences
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.; Rutgers Univ., Piscataway, NJ (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1462849
DOE Contract Number:  
AC05-00OR22725; FG02-99ER45761
Resource Type:
Journal Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 361; Journal Issue: 6400; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Kent, Paul R. C., and Kotliar, Gabriel. Toward a predictive theory of correlated materials. United States: N. p., 2018. Web. doi:10.1126/science.aat5975.
Kent, Paul R. C., & Kotliar, Gabriel. Toward a predictive theory of correlated materials. United States. doi:10.1126/science.aat5975.
Kent, Paul R. C., and Kotliar, Gabriel. Fri . "Toward a predictive theory of correlated materials". United States. doi:10.1126/science.aat5975.
@article{osti_1462849,
title = {Toward a predictive theory of correlated materials},
author = {Kent, Paul R. C. and Kotliar, Gabriel},
abstractNote = {Correlated electron materials display a rich variety of notable properties ranging from unconventional superconductivity to metal-insulator transitions. These properties are of interest from the point of view of applications but are hard to treat theoretically, as they result from multiple competing energy scales. Although possible in more weakly correlated materials, theoretical design and spectroscopy of strongly correlated electron materials have been a difficult challenge for many years. In this paper, by treating all the relevant energy scales with sufficient accuracy, complementary advances in Green’s functions and quantum Monte Carlo methods open a path to first-principles computational property predictions in this class of materials.},
doi = {10.1126/science.aat5975},
journal = {Science},
issn = {0036-8075},
number = 6400,
volume = 361,
place = {United States},
year = {2018},
month = {7}
}

Works referenced in this record:

Multitier self-consistent G W + EDMFT
journal, September 2017


Density-functional calculation of effective Coulomb interactions in metals
journal, April 1991


Quantum Monte Carlo Calculations of Structural Properties of FeO Under Pressure
journal, October 2008


Self-consistent G W determination of the interaction strength: Application to the iron arsenide superconductors
journal, July 2010


Dynamical mean-field theory, density-matrix embedding theory, and rotationally invariant slave bosons: A unified perspective
journal, December 2017


Ab initio calculations of quasiparticle band structure in correlated systems: LDA++ approach
journal, March 1998


Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
journal, November 2004


Dynamical Mean-Field Theory Plus Numerical Renormalization-Group Study of Spin-Orbital Separation in a Three-Band Hund Metal
journal, September 2015


Electronic origin of the volume collapse in cerium
journal, February 2015


Spin-rotation-invariant slave-boson approach to the Hubbard model
journal, October 1989


Quantum cluster theories
journal, October 2005


Ground-state properties of simple elements from GW calculations
journal, July 2009


Electron-phonon coupling and properties of doped BaBiO 3
journal, June 1998


Density Matrix Embedding: A Simple Alternative to Dynamical Mean-Field Theory
journal, November 2012


Spin dynamics and orbital-antiphase pairing symmetry in iron-based superconductors
journal, October 2014

  • Yin, Z. P.; Haule, K.; Kotliar, G.
  • Nature Physics, Vol. 10, Issue 11
  • DOI: 10.1038/nphys3116

Metal-insulator transition and lattice instability of paramagnetic V 2 O 3
journal, May 2015


First-Principles Calculation of Atomic Forces and Structural Distortions in Strongly Correlated Materials
journal, April 2014


Metal-Insulator Transition in VO 2 : A DFT + DMFT Perspective
journal, July 2016


Chemistry on the computer
journal, April 2008

  • Head-Gordon, Martin; Artacho, Emilio
  • Physics Today, Vol. 61, Issue 4
  • DOI: 10.1063/1.2911179

Conservation Laws and Correlation Functions
journal, October 1961


Continuous-time Monte Carlo methods for quantum impurity models
journal, May 2011

  • Gull, Emanuel; Millis, Andrew J.; Lichtenstein, Alexander I.
  • Reviews of Modern Physics, Vol. 83, Issue 2
  • DOI: 10.1103/RevModPhys.83.349

Density-matrix based determination of low-energy model Hamiltonians from ab initio wavefunctions
journal, August 2015

  • Changlani, Hitesh J.; Zheng, Huihuo; Wagner, Lucas K.
  • The Journal of Chemical Physics, Vol. 143, Issue 10
  • DOI: 10.1063/1.4927664

Deterministic Construction of Nodal Surfaces within Quantum Monte Carlo: The Case of FeS
journal, January 2018

  • Scemama, Anthony; Garniron, Yann; Caffarel, Michel
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 3
  • DOI: 10.1021/acs.jctc.7b01250

Binding and Diffusion of Lithium in Graphite: Quantum Monte Carlo Benchmarks and Validation of van der Waals Density Functional Methods
journal, November 2014

  • Ganesh, P.; Kim, Jeongnim; Park, Changwon
  • Journal of Chemical Theory and Computation, Vol. 10, Issue 12
  • DOI: 10.1021/ct500617z

Electron-phonon interactions and related physical properties of metals from linear-response theory
journal, December 1996


First-principles calculations of the electronic structure and spectra of strongly correlated systems: dynamical mean-field theory
journal, September 1997

  • Anisimov, V. I.; Poteryaev, A. I.; Korotin, M. A.
  • Journal of Physics: Condensed Matter, Vol. 9, Issue 35
  • DOI: 10.1088/0953-8984/9/35/010

Density functional theory is straying from the path toward the exact functional
journal, January 2017

  • Medvedev, Michael G.; Bushmarinov, Ivan S.; Sun, Jianwei
  • Science, Vol. 355, Issue 6320
  • DOI: 10.1126/science.aah5975

Electronic structure calculations with dynamical mean-field theory
journal, August 2006


Effective on-site interaction for dynamical mean-field theory
journal, August 2012


Self-consistent solution of Hedin's equations: Semiconductors and insulators
journal, May 2017


Structural Relaxation due to Electronic Correlations in the Paramagnetic Insulator KCuF 3
journal, August 2008


Pressure-induced metallization of dense (H2S)2H2 with high-Tc superconductivity
journal, November 2014

  • Duan, Defang; Liu, Yunxian; Tian, Fubo
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06968

Mott physics and spin fluctuations: A functional viewpoint
journal, June 2016


Perspective: Explicitly correlated electronic structure theory for complex systems
journal, February 2017

  • Grüneis, Andreas; Hirata, So; Ohnishi, Yu-ya
  • The Journal of Chemical Physics, Vol. 146, Issue 8
  • DOI: 10.1063/1.4976974

Correlated electrons in δ-plutonium within a dynamical mean-field picture
journal, April 2001

  • Savrasov, S. Y.; Kotliar, G.; Abrahams, E.
  • Nature, Vol. 410, Issue 6830
  • DOI: 10.1038/35071035

Gutzwiller density functional theory for correlated electron systems
journal, February 2008


Alleviation of the Fermion-Sign Problem by Optimization of Many-Body Wave Functions
journal, March 2007


Benchmarking exchange-correlation functionals for hydrogen at high pressures using quantum Monte Carlo
journal, May 2014


Strong pressure-dependent electron-phonon coupling in FeSe
journal, June 2014


Electronic structure of Pu and Am metals by self-consistent relativistic G W method
journal, April 2012


First-principles treatment of Mott insulators: linearized QSGW+DMFT approach
journal, July 2016


Continuous-Time Solver for Quantum Impurity Models
journal, August 2006


G W with linearized augmented plane waves extended by high-energy local orbitals
journal, March 2016


Extended dynamical mean-field theory and GW method
journal, August 2002


Dynamical mean-field theory from a quantum chemical perspective
journal, March 2011

  • Zgid, Dominika; Chan, Garnet Kin-Lic
  • The Journal of Chemical Physics, Vol. 134, Issue 9
  • DOI: 10.1063/1.3556707

Importance of Many-Body Effects in the Kernel of Hemoglobin for Ligand Binding
journal, March 2013


Exact Double Counting in Combining the Dynamical Mean Field Theory and the Density Functional Theory
journal, November 2015


B 1 -to- B 8 structural phase transition in MnO under pressure: Comparison of all-electron and pseudopotential approaches
journal, June 2007


Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium
journal, March 2007


Selective Mott Physics as a Key to Iron Superconductors
journal, April 2014


Fermion Monte Carlo without fixed nodes: A game of life, death, and annihilation in Slater determinant space
journal, January 2009

  • Booth, George H.; Thom, Alex J. W.; Alavi, Ali
  • The Journal of Chemical Physics, Vol. 131, Issue 5
  • DOI: 10.1063/1.3193710

Dynamical mean-field theory for molecular electronics: Electronic structure and transport properties
journal, November 2010


Quantum Monte Carlo Method using Phase-Free Random Walks with Slater Determinants
journal, April 2003


Ground state of doped cuprates from first-principles quantum Monte Carlo calculations
journal, October 2015


Competing collinear magnetic structures in superconducting FeSe by first-principles quantum Monte Carlo calculations
journal, July 2016


Analytic Interatomic Forces in the Random Phase Approximation
journal, March 2017


Local Self-Energy Approach for Electronic Structure Calculations
journal, June 2006


Local density approximation combined with Gutzwiller method for correlated electron systems: Formalism and applications
journal, February 2009


Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser
journal, July 2017


The valence-fluctuating ground state of plutonium
journal, July 2015

  • Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan
  • Science Advances, Vol. 1, Issue 6
  • DOI: 10.1126/sciadv.1500188

Quasiparticle Self-Consistent G W Theory
journal, June 2006


Diagrammatic routes to nonlocal correlations beyond dynamical mean field theory
journal, May 2018


The Nature of the Interlayer Interaction in Bulk and Few-Layer Phosphorus
journal, November 2015


Discovering correlated fermions using quantum Monte Carlo
journal, August 2016


Free Energy from Stationary Implementation of the DFT + DMFT Functional
journal, December 2015


Correlated Lattice Fermions in d = Dimensions
journal, January 1989


Effective interactions in multiband systems from constrained summations
journal, May 2012


Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions
journal, January 1996

  • Georges, Antoine; Kotliar, Gabriel; Krauth, Werner
  • Reviews of Modern Physics, Vol. 68, Issue 1
  • DOI: 10.1103/RevModPhys.68.13

Rotationally invariant slave-boson formalism and momentum dependence of the quasiparticle weight
journal, October 2007


Electronic Coherence in δ -Pu: A Dynamical Mean-Field Theory Study
journal, August 2008


Dynamical Mean-Field Theory for Quantum Chemistry
journal, March 2011


Computation of the Correlated Metal-Insulator Transition in Vanadium Dioxide from First Principles
journal, April 2015


Conventional superconductivity at 203 kelvin at high pressures in the sulfur hydride system
journal, August 2015

  • Drozdov, A. P.; Eremets, M. I.; Troyan, I. A.
  • Nature, Vol. 525, Issue 7567
  • DOI: 10.1038/nature14964

Towards an exact description of electronic wavefunctions in real solids
journal, December 2012

  • Booth, George H.; Grüneis, Andreas; Kresse, Georg
  • Nature, Vol. 493, Issue 7432
  • DOI: 10.1038/nature11770

QMCPACK : an open source ab initio quantum Monte Carlo package for the electronic structure of atoms, molecules and solids
journal, April 2018

  • Kim, Jeongnim; Baczewski, Andrew D.; Beaudet, Todd D.
  • Journal of Physics: Condensed Matter, Vol. 30, Issue 19
  • DOI: 10.1088/1361-648X/aab9c3

Coherent band excitations in CePd 3 : A comparison of neutron scattering and ab initio theory
journal, January 2018


Ab initio dynamical vertex approximation
journal, March 2017


Electronic structure of α- and δ-Pu from photoelectron spectroscopy
journal, July 2000


Ground-State Energy of a Many-Fermion System. II
journal, June 1960


Cluster dynamical mean-field theories: Causality and classical limit
journal, May 2004


Multideterminant Wave Functions in Quantum Monte Carlo
journal, June 2012

  • Morales, Miguel A.; McMinis, Jeremy; Clark, Bryan K.
  • Journal of Chemical Theory and Computation, Vol. 8, Issue 7
  • DOI: 10.1021/ct3003404

Accuracy of ab initio electron correlation and electron densities in vanadium dioxide
journal, November 2017