The divide–expand–consolidate coupled cluster scheme

Kjærgaard, Thomas; Baudin, Pablo; Bykov, Dmytro; Kristensen, Kasper; Jørgensen, Poul

doi:10.1002/wcms.1319

Cited by 48 publications

(49 citation statements)

References 120 publications

(298 reference statements)

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“…In these methods, the MP2 or coupled cluster (CC) equations should be solved within the entire system in a single calculation. Another group of the local correlation methods divides the entire system into smaller clusters (a subset of occupied and virtual LMOs) and the correlation energy of the whole system is estimated as the sum of the contributions from various clusters . The MP2 or CC equations are solved within these small clusters.…”

Section: Introductionmentioning

confidence: 99%

“…In 2011 and 2013, Kállay and co‐workers developed efficient CCSD and CCSD(T) methods by combining the CIM approach with the frozen natural orbital techniques . In addition, the divide‐expand‐consolidate scheme developed by Jørgensen and co‐workers is closely related to the CIM approach. In their approach, the whole system is divided into atomic fragments and atomic pair fragments, whose definitions are similar to the clusters in the CIM approach.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Fully optimized implementation of the cluster‐in‐molecule local correlation approach for electron correlation calculations of large systems

2018

J Comput Chem

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A fully optimized implementation of the cluster-in-molecule (CIM) local correlation method for faster and more accurate electron correlation calculations of large systems is reported. The speedup comes from the new procedure of constructing virtual localized molecular orbitals of clusters. In the new procedure, Boughton-Pulay projection method is employed instead of a much more expensive Boys localization procedure. In addition, basis set superposition error correction for binding energy calculations and parallelized electron correlation calculations of clusters are now implemented. Benchmark calculations and illustrative applications at the Møller-Plesset perturbation theory, coupled cluster singles and doubles (CCSD), and CCSD with perturbative triples correction levels show that this newly optimized CIM approach is a reliable theoretical tool for electron correlation calculations of various large chemical systems.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Fully optimized implementation of the cluster‐in‐molecule local correlation approach for electron correlation calculations of large systems

2018

J Comput Chem

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“…Despite the current success in the development of feasible quantum-chemical methods able to accurately describe relatively large-size supramolecular complexes, the molecular size is still critical for routine quantum-chemical calculations on molecular systems of more than 1000 atoms. Notwithstanding, new avenues of research concerning the development of large-scale quantum-chemical techniques allow dealing with very large molecular systems [ 64 , 122 , 123 , 124 ], and point to a bright future for the field of quantum chemistry and molecular modelling applied to supramolecular chemistry problems.…”

Section: Discussionmentioning

confidence: 99%

Quantum-Chemical Insights into the Self-Assembly of Carbon-Based Supramolecular Complexes

et al. 2018

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Understanding how molecular systems self-assemble to form well-organized superstructures governed by noncovalent interactions is essential in the field of supramolecular chemistry. In the nanoscience context, the self-assembly of different carbon-based nanoforms (fullerenes, carbon nanotubes and graphene) with, in general, electron-donor molecular systems, has received increasing attention as a means of generating potential candidates for technological applications. In these carbon-based systems, a deep characterization of the supramolecular organization is crucial to establish an intimate relation between supramolecular structure and functionality. Detailed structural information on the self-assembly of these carbon-based nanoforms is however not always accessible from experimental techniques. In this regard, quantum chemistry has demonstrated to be key to gain a deep insight into the supramolecular organization of molecular systems of high interest. In this review, we intend to highlight the fundamental role that quantum-chemical calculations can play to understand the supramolecular self-assembly of carbon-based nanoforms through a limited selection of supramolecular assemblies involving fullerene, fullerene fragments, nanotubes and graphene with several electron-rich π-conjugated systems.

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“…However, today's programming standards impose parallelism, and if determinant-driven calculations prove to be be er adapted to parallelism, such methods could regain popularity. More conventional approaches have also been very successfully parallelized: CCSD(T), 57,58 DMRG, 59 GW, 60 QMC, [61][62][63] and many others. P was used in numerous applications, in particular to obtain reference ground-state energies [34][35][36][37][38]64 as well as excitation energies 44,54,65 for atomic and molecular systems.…”

Section: Introductionmentioning

confidence: 99%

Quantum Package 2.0: An Open-Source Determinant-Driven Suite of Programs

Garniron¹,

Applencourt²,

Gasperich³

et al. 2019

Preprint

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TOC graphical abstract antum chemistry is a discipline which relies heavily on very expensive numerical computations. e scaling of correlated wave function methods lies, in their standard implementation, between O(N 5 ) and O(e N ), where N is proportional to the system size. erefore, performing accurate calculations on chemically meaningful systems requires i) approximations that can lower the computational scaling, and ii) e cient implementations that take advantage of modern massively parallel architectures. P is an open-source programming environment for quantum chemistry specially designed for wave function methods. Its main goal is the development of determinantdriven selected con guration interaction (sCI) methods and multi-reference second-order perturbation theory (PT2). e determinant-driven framework allows the programmer to include any arbitrary set of determinants in the reference space, hence providing greater methodological freedom. e sCI method implemented in P is based on the CIPSI (Con guration Interaction using a Perturbative Selection made Iteratively) algorithm which complements the variational sCI energy with a PT2 correction. Additional external plugins have been recently added to perform calculations with multireference coupled cluster theory and range-separated density-functional theory. All the programs are developed with the IRPF90 code generator, which simpli es collaborative work and the development of new features. P strives to allow easy implementation and experimentation of new methods, while making parallel computation as simple and e cient as possible on modern supercomputer architectures. Currently, the code enables, routinely, to realize runs on roughly 2 000 CPU cores, with tens of millions of determinants in the reference space. Moreover, we have been able to push up to 12 288 cores in order to test its parallel e ciency. In the present manuscript, we also introduce some key new developments: i) a renormalized second-order perturbative correction for e cient extrapolation to the full CI limit, and ii) a stochastic version of the CIPSI selection performed simultaneously to the PT2 calculation at no extra cost.

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The divide–expand–consolidate coupled cluster scheme

Cited by 48 publications

References 120 publications

Fully optimized implementation of the cluster‐in‐molecule local correlation approach for electron correlation calculations of large systems

Fully optimized implementation of the cluster‐in‐molecule local correlation approach for electron correlation calculations of large systems

Quantum-Chemical Insights into the Self-Assembly of Carbon-Based Supramolecular Complexes

Quantum Package 2.0: An Open-Source Determinant-Driven Suite of Programs

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