4.7 Article

Density Matrix Embedding Using Multiconfiguration Pair-Density Functional Theory

Related references

Note: Only part of the references are listed.
Article Chemistry, Physical

Local Excitations of a Charged Nitrogen Vacancy in Diamond with Multireference Density Matrix Embedding Theory

Soumi Haldar et al.

Summary: In this study, we investigated the negatively charged nitrogen-vacancy center in diamond using periodic density matrix embedding theory (pDMET). To accurately describe the strongly correlated excited states of the system, we utilized the complete active space self-consistent field (CASSCF) method followed by n-electron valence state second-order perturbation theory (NEVPT2) as the impurity solver. By extrapolating the excitation energies to the nonembedding limit using linear regression, we obtained the first triplet-triplet excitation energy of 2.31 eV and the singlet-singlet transition energy of 1.02 eV, both in agreement with experimental observations. This is the first application of pDMET to a charged periodic system and the first investigation of the NV- defect using NEVPT2 for periodic supercell models.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2023)

Article Physics, Multidisciplinary

Systematic Improvability in Quantum Embedding for Real Materials

Max Nusspickel et al.

Summary: In this study, a new quantum embedding theory is proposed, which combines density-matrix embedding theory with local correlation approaches from quantum chemistry. This theory allows for systematic convergence of properties of real materials and can provide accurate results without the need for empirical parameters.

PHYSICAL REVIEW X (2022)

Article Chemistry, Physical

Periodic Density Matrix Embedding for CO Adsorption on the MgO(001) Surface

Abhishek Mitra et al.

Summary: In this study, density matrix embedding theory (DMET) was used to calculate the adsorption energy of CO on the MgO(001) surface, demonstrating the potential of quantum embedding methods in understanding gas molecule adsorption on metal oxide surfaces.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2022)

Article Chemistry, Physical

Large-Scale Benchmarking of Multireference Vertical-Excitation Calculations via Automated Active-Space Selection

Daniel S. King et al.

Summary: In this study, we calculated the excitation energies using four methods and applied the APC selection scheme. We found that the performance of NEVPT2 is affected by the basis set size, while HMC-PDFT performs well in certain cases. Additionally, this is the largest benchmarking of MC-PDFT and HMC-PDFT to date, providing useful validation for these methods and the APC selection scheme.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2022)

Article Multidisciplinary Sciences

Systematic electronic structure in the cuprate parent state from quantum many-body simulations

Zhi-Hao Cui et al.

Summary: We demonstrate a numerical strategy to simulate correlated materials at the fully ab initio level and gain a detailed microscopic understanding of cuprate superconducting materials. Our work uncovers microscopic trends in electron correlations and reveals the link between material composition and magnetic energy scales.

SCIENCE (2022)

Article Computer Science, Interdisciplinary Applications

Quantum embedding theories to simulate condensed systems on quantum computers

Christian Vorwerk et al.

Summary: This article discusses computational frameworks for carrying out electronic structure calculations of solids on noisy intermediate-scale quantum computers using embedding theories, focusing on a specific class of materials - solid materials hosting spin defects. These materials are promising for future quantum technologies, such as quantum computers, quantum sensors, and quantum communication devices. Although quantum simulations on quantum architectures are still in their early stages, promising results have been achieved for realistic systems.

NATURE COMPUTATIONAL SCIENCE (2022)

Article Materials Science, Multidisciplinary

Quantum embedding methods for correlated excited states of point defects: Case studies and challenges

Lukas Muechler et al.

Summary: Quantitatively describing excited electronic states of point defects and impurities is crucial for understanding material properties and applications in quantum technologies. Recently, embedding methods that use many-body approaches for defect states and density functional theory for the bulk host material have been implemented. Through systematic characterization of different systems, we identified important factors such as convergence, functional selection, and correction treatment.

PHYSICAL REVIEW B (2022)

Article Chemistry, Multidisciplinary

Electronic structure of strongly correlated systems: recent developments in multiconfiguration pair-density functional theory and multiconfiguration nonclassical-energy functional theory

Chen Zhou et al.

Summary: This article provides an introduction to strongly correlated systems and multiconfiguration pair-density functional theory (MC-PDFT) which is used to quantitatively treat near-degeneracy correlation and dynamic correlation in these systems. The article also discusses recent developments and applications of MC-PDFT and related methods.

CHEMICAL SCIENCE (2022)

Article Chemistry, Physical

Regional Embedding Enables High-Level Quantum Chemistry for Surface Science

Bryan T. G. Lau et al.

Summary: This paper introduces a regional embedding approach that allows for correlated wave function treatments of target fragments through small, fragment-localized orbital spaces. Applications show that regional embedding combined with focal-point corrections can provide converged CCSD(T) adsorption energies with very small fragment sizes.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

Article Chemistry, Physical

Excited States of Crystalline Point Defects with Multireference Density Matrix Embedding Theory

Abhishek Mitra et al.

Summary: The study explores the application of embedding-based methods in electronic excitations of solid-state defects, showing that the DMET method can achieve high accuracy. The practicality of the method is extended and validated in oxygen vacancies on the MgO(100) surface and neutral silicon vacancies in diamond.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

Review Chemistry, Physical

Multiconfiguration Pair-Density Functional Theory

Prachi Sharma et al.

Summary: Kohn-Sham density functional theory is less accurate for strongly correlated systems compared to weakly correlated systems. The available functionals for spin densities do not accurately predict energies for strongly correlated systems when using multiconfigurational wave functions with spin symmetry. Multiconfiguration pair-density functional theory overcomes these limitations by using a functional of the total density and on-top pair density, allowing efficient calculation of energy for strongly correlated systems.

ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 72 (2021)

Article Chemistry, Physical

Quantum Embedding Theory for Strongly Correlated States in Materials

He Ma et al.

Summary: Quantum embedding theories provide a promising approach to investigate strongly correlated electronic states by considering screened Coulomb interactions and effective Hamiltonians, avoiding the need for the random phase approximation or evaluating virtual electronic orbitals. This allows for a detailed derivation of the theory and generalization to active spaces composed of non-eigenstate orbitals, as demonstrated in the study of spin defects in semiconductors.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2021)

Review Chemistry, Physical

Role of oxygen vacancy in metal oxide based photoelectrochemical water splitting

Zhiliang Wang et al.

Summary: Oxygen vacancies play a crucial role in the optimization of photoelectrodes for PEC water splitting, affecting light absorption, charge separation, and surface reaction kinetics. Although the presence of oxygen vacancies may increase recombination, recent research has shown their beneficial impact on PEC performance, contrary to previous understanding. A comprehensive analysis of oxygen vacancies in metal oxide photoelectrodes is essential for achieving high efficiency in PEC.

ECOMAT (2021)

Article Physics, Condensed Matter

Wannier90 as a community code: new features and applications

Giovanni Pizzi et al.

JOURNAL OF PHYSICS-CONDENSED MATTER (2020)

Article Chemistry, Physical

Periodic Electronic Structure Calculations with the Density Matrix Embedding Theory

Hung Q. Pham et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2020)

Article Chemistry, Physical

Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Density Matrix Embedding Theory

Zhi-Hao Cui et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2020)

Article Chemistry, Physical

Recent developments in the PySCF program package

Qiming Sun et al.

JOURNAL OF CHEMICAL PHYSICS (2020)

Article Chemistry, Physical

A New Mixing of Nonlocal Exchange and Nonlocal Correlation with Multiconfiguration Pair-Density Functional Theory

Riddhish Pandharkar et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2020)

Article Chemistry, Physical

Density-Matrix Embedding Theory Study of the One-Dimensional Hubbard-Holstein Model

Teresa E. Reinhard et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2019)

Article Chemistry, Physical

Using SCF metadynamics to extend density matrix embedding theory to excited states

Henry K. Tran et al.

JOURNAL OF CHEMICAL PHYSICS (2019)

Article Chemistry, Multidisciplinary

PYSCF: the Python-based simulations of chemistry framework

Qiming Sun et al.

WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE (2018)

Article Chemistry, Physical

Projection-Based Correlated Wave Function in Density Functional Theory Embedding for Periodic Systems

Dhabih V. Chulhai et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2018)

Review Chemistry, Multidisciplinary

Multiconfiguration Pair-Density Functional Theory: A New Way To Treat Strongly Correlated Systems

Laura Gagliardi et al.

ACCOUNTS OF CHEMICAL RESEARCH (2017)

Review Chemistry, Multidisciplinary

Quantum Embedding Theories

Qinaing Sun et al.

ACCOUNTS OF CHEMICAL RESEARCH (2016)

Article Chemistry, Physical

Bootstrap embedding: An internally consistent fragment-based method

Matthew Welborn et al.

JOURNAL OF CHEMICAL PHYSICS (2016)

Article Chemistry, Physical

A Practical Guide to Density Matrix Embedding Theory in Quantum Chemistry

Sebastian Wouters et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2016)

Article Materials Science, Multidisciplinary

Ground-state phase diagram of the square lattice Hubbard model from density matrix embedding theory

Bo-Xiao Zheng et al.

PHYSICAL REVIEW B (2016)

Article Chemistry, Physical

Multiconfiguration Pair-Density Functional Theory

Giovanni Li Manni et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2014)

Review Chemistry, Multidisciplinary

Theoretical Approaches to Excited-State-Related Phenomena in Oxide Surfaces

Carmen Sousa et al.

CHEMICAL REVIEWS (2013)

Article Chemistry, Physical

Density Matrix Embedding: A Strong-Coupling Quantum Embedding Theory

Gerald Knizia et al.

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2013)

Article Physics, Multidisciplinary

Concentration of Vacancies at Metal-Oxide Surfaces: Case Study of MgO(100)

Norina A. Richter et al.

PHYSICAL REVIEW LETTERS (2013)

Article Physics, Multidisciplinary

First-Principles Optical Spectra for F Centers in MgO

Patrick Rinke et al.

PHYSICAL REVIEW LETTERS (2012)

Article Physics, Multidisciplinary

Maximally localized Wannier functions: Theory and applications

Nicola Marzari et al.

REVIEWS OF MODERN PHYSICS (2012)

Review Physics, Multidisciplinary

Reduced density matrices and entanglement entropy in free lattice models

Ingo Peschel et al.

JOURNAL OF PHYSICS A-MATHEMATICAL AND THEORETICAL (2009)

Article Physics, Multidisciplinary

Restoring the density-gradient expansion for exchange in solids and surfaces

John P. Perdew et al.

PHYSICAL REVIEW LETTERS (2008)

Article Chemistry, Multidisciplinary

The role of F-centers in catalysis by Au supported on MgO

Z Yan et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2005)

Article Materials Science, Multidisciplinary

Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and surface of MgO -: art. no. 054101

D Domínguez-Ariza et al.

PHYSICAL REVIEW B (2003)

Article Chemistry, Physical

Mechanism and kinetics of color center formation on epitaxial thin films of MgO

J Kramer et al.

SURFACE SCIENCE (2002)

Article Chemistry, Physical

Introduction of n-electron valence states for multireference perturbation theory

C Angeli et al.

JOURNAL OF CHEMICAL PHYSICS (2001)