Periodic and fragment models based on the local correlation approach

Usvyat, Denis; Maschio, Lorenzo; Schütz, Martin

doi:10.1002/wcms.1357

Cited by 41 publications

(43 citation statements)

References 205 publications

(414 reference statements)

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“…For an excellent review of the local wave function correlation methodsf or the condensed-phase systems, see Ref. [13].…”

Section: Local Correlation Methodsmentioning

confidence: 99%

Sampling Potential Energy Surfaces in the Condensed Phase with Many‐Body Electronic Structure Methods

Rybkin

2019

Chemistry A European J

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Sampling potential energy surfaces (PES) is pivotal for understanding chemical structure, energetics and reactivity and is of special importance for complex condensed‐phase systems. Until recently such simulations based on electronic structure theory have been performed only by density functional theory and semiempirical methods. Many‐body electronic structure methods, almost routinely used for molecules, have been practically unavailable for sampling PES in the condensed‐phase. This has changed during the last few years, as efficient algorithms and software implementations for the evaluation of electronic energies and forces on atoms have been developed, allowing for geometry optimization, molecular dynamics and Monte‐Carlo simulations, which was previously unthinkable. Herein, we introduce the theory and software developments and overview the applications in the field, the most encouraging results being obtained for aqueous chemistry. Requiring state‐of‐the‐art computer resources PES sampling with many‐body electronic structure methods in the condensed phase provides high‐quality benchmarks and will gradually become more available due to fast progress in reduced scaling algorithms and computational technologies.

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“…For an excellent review of the local wave function correlation methodsf or the condensed-phase systems, see Ref. [13].…”

Section: Local Correlation Methodsmentioning

confidence: 99%

Sampling Potential Energy Surfaces in the Condensed Phase with Many‐Body Electronic Structure Methods

Rybkin

2019

Chemistry A European J

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“…Furthermore, Booth, Grüneis, Kresse, and Alavi have demonstrated that the standard hierarchy of quantum chemical methods and in particular the CC ansatz is also valid for solids . For a review on the uses of CC methods in material science, see the review of Zhang and Grüneis, for a discussion on local correlation approaches for solids, see the work of Usvyat, Maschio, and Schütz …”

Section: Algorithmic Approximationsmentioning

confidence: 99%

Single‐reference coupled cluster methods for computing excitation energies in large molecules: The efficiency and accuracy of approximations

Izsák

2019

WIREs Comput Mol Sci

110

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While methodological developments in the last decade made it possible to compute coupled cluster (CC) energies including excitations up to a perturbative triples correction for molecules containing several hundred atoms, a similar breakthrough has not yet been reported for excited state computations. Accurate CC methods for excited states are still expensive, although some promising candidates for an efficient and accurate excited state CC method have emerged recently. This review examines the various approximation schemes with particular emphasis on their performance for excitation energies and summarizes the best state-of-the-art results which may pave the way for a robust excited state method applicable to molecules of hundreds of atoms.Among these, special attention will be given to exploiting the techniques of similarity transformation, perturbative approximations as well as integral decomposition, local and embedding techniques within the equation of motion CC framework. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Structure and Mechanism > Molecular Structures K E Y W O R D S accuracy, coupled cluster, efficiency, excited states, single reference | INTRODUCTIONIn their lucid review written a few years ago, 1 Sneskov and Christiansen discussed the various coupled cluster (CC) methods available for excited states. Using the systematic machinery of response theory, they described a hierarchy of methods, established a link between response theory and equation of motion (EOM) methods, and finished by discussing a number of approaches that might be used to reduce the computational cost. The present review aims at providing an overview of efficient methods available primarily for large molecules, and hence the emphasis will be laid more upon recent methodological advances which reduce the cost and on the extent this affects the accuracy of these methods. For ground state calculations, choosing a reference method for benchmarks is quite easy, since the CC singles doubles and perturbative triples, or CCSD(T), ansatz 2 is not only widely regarded as the gold standard of quantum chemistry, but it has also recently become possible to compute CCSD(T) energies for molecules containing several hundred atoms. 3 For excited states, progress has been

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“…In contrast to multireference methods, single reference coupled cluster theory is in general not suited to treat strong correlation problems. However, coupled cluster theories have successfully been applied to calculate a wide range of materials properties including (i) cohesive energies of (molecular) solids (Rościszewski et al, 1999;Nolan et al, 2009;Schwerdtfeger et al, 2010;Grüneis et al, 2011;Stoll and Doll, 2012;Booth et al, 2013;Yang et al, 2014;, (ii) pressure-temperature phase diagrams (iii) exfoliation energies of layered materials (Hummel et al, 2016;Sansone et al, 2016;Usvyat et al, 2018) (iv) defect formation energies (Grüneis, 2015b), and (v) adsorption and reaction energies of atoms and molecules on surfaces (Voloshina et al, 2011;Usvyat et al, 2012;Boese and Sauer, 2016;Kubas et al, 2016;Tsatsoulis et al, 2017Tsatsoulis et al, , 2018. Furthermore, the equation of motion coupled cluster theories has been implemented to calculate the excited state and single-electron related properties including electronaddition and removal energies in solids (McClain et al, 2017).…”

Section: Introductionmentioning

confidence: 99%

Coupled Cluster Theory in Materials Science

2019

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The workhorse method of computational materials science is undeniably the density functional theory (DFT) in the Kohn-Sham framework of approximate exchange and correlation energy functionals. However, the need for highly accurate electronic structure theory calculations in materials science motivates the further development and exploration of alternative as well as complementary techniques. Among these alternative approaches, quantum chemical wavefunction based theories and in particular coupled cluster theory hold promise in filling the gap in the toolbox of computational materials scientists. Coupled cluster (CC) theory provides a compelling framework of approximate infinite-order perturbation theory, in the form of an exponential of cluster operators describing the true quantum many-body effects of the electronic wave function at a computational cost that, despite being significantly more expensive than DFT, scales polynomially with system size. The hierarchy of size-extensive approximate methods established in the framework of CC theory, achieves systematic improvability for many materials properties. This is in contrast to currently available density functionals that often suffer from uncontrolled approximations that limit the accuracy in the prediction of materials properties. In this tutorial-style review we will introduce basic concepts of coupled cluster theory and recent developments that increase its computational efficiency for calculations of molecules, solids and materials in general. We will touch upon the connection between coupled cluster theory and the random-phase approximation that is widely used in the field of solid-state physics. We will discuss various approaches to improve the computational performance without compromising on accuracy. These approaches include large-scale parallel design as well as techniques that reduce the pre-factor of the computational complexity. A central part of this article discusses the convergence of calculated properties to the thermodynamic limit, which is of significant importance for reliable predictions of materials properties and constitutes an additional challenge compared to calculations of large molecules. We mention technical aspects of computer code implementations of periodic coupled cluster theories in different numerical frameworks of the one-electron orbital basis; the projector-augmented-wave formalism using a plane wave basis set and the numeric atom-centered-orbital (NAO) with resolution-of-identity. We will discuss results and the possible scope of these implementations and how they can help advance the current state of the art in electronic structure theory calculations of materials.

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Periodic and fragment models based on the local correlation approach

Cited by 41 publications

References 205 publications

Sampling Potential Energy Surfaces in the Condensed Phase with Many‐Body Electronic Structure Methods

Sampling Potential Energy Surfaces in the Condensed Phase with Many‐Body Electronic Structure Methods

Single‐reference coupled cluster methods for computing excitation energies in large molecules: The efficiency and accuracy of approximations

Coupled Cluster Theory in Materials Science

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