Development of a 3-body:many-body integrated fragmentation method for weakly bound clusters and application to water clusters (H2O)<i>n</i>= 3 − 10, 16, 17

Bates, Desiree M.; Smith, Joshua R.; Janowski, Tomasz; Tschumper, Gregory S.

doi:10.1063/1.3609922

Cited by 71 publications

(87 citation statements)

References 127 publications

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“…229 Relatively large water clusters have also been examined with the N-body:many-body QM:QM technique. 235 The 3-body:Many-body CCSD(T):MP2 approach provided binding energies nearly identical to the canonical CCSD(T) values for more than 40 low-lying isomers of (H 2 O) n=3−10 with the haTZ basis set. The maximum deviation was only 0.07 kcal mol −1 for this test set.…”

Section: Strategies For Extending High-accuracy Methods To Larger Clumentioning

confidence: 87%

Wavefunction methods for the accurate characterization of water clusters

Howard

Tschumper

2013

WIREs Comput Mol Sci

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Although the first ab initio Hartree-Fock computations of the water dimer were reported more than four decades ago, the detailed characterization of water clusters with sophisticated electronic structure techniques remains an important and vibrant area of research. The field of computational quantum chemistry has made significant advances since those pioneering studies. Geometry optimizations of the water dimer can now be carried out at the CCSDTQ level, and CCSD(T) energies can be computed with the aug-cc-pVTZ basis for clusters as large as (H 2 O) 17 . Some of these high-level studies are starting to reveal that the electronic structure is harder to describe for some hydrogen bonds than others. For example, discrepancies between MP2 and CCSD(T) energetics tend to increase when there are qualitative differences in the hydrogen-bonding networks of the water clusters being studied. This review highlights the recent and exciting work in this area and provides an overview of popular strategies for generating reliable properties and benchmark quality energetics for water clusters with correlated wavefunction methods. C 2013 John Wiley & Sons, Ltd.

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Section: Strategies For Extending High-accuracy Methods To Larger Clumentioning

confidence: 87%

Wavefunction methods for the accurate characterization of water clusters

Howard

Tschumper

2013

WIREs Comput Mol Sci

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“…Six-body terms can always be safely neglected. We have also analyzed the possibility of computing high-K contributions applying a hybrid canonical and many-body approach as recently implemented by Bates et al, 67 but it turns out that it cannot be adopted at accuracy levels that we aim at.…”

Section: Discussionmentioning

confidence: 99%

“…69, later reproduced in Ref. 67. At the CCSD(T) level, the lowest isomer is 4444-a in all calculations.…”

Section: Large Water Clustersmentioning

confidence: 96%

“…Bates et al 67 have recently applied a variant of "hybrid fragmentation" approaches to water clusters by computing total cluster interaction energies at a low level of theory and basis set and combining these results with high-level calculations of two-and three-body effects…”

Section: Applications Of Effective Many-body Strategiesmentioning

confidence: 99%

“…The calculation of the post-three-body effects took 6.3 CPU days in Ref. 67 whereas our calculation of four-body effects took 16 CPU days.…”

Section: Large Water Clustersmentioning

confidence: 99%

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Interaction energies of large clusters from many-body expansion

Góra

Podeszwa

Cencek

et al. 2011

The Journal of Chemical Physics

161

144

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In the canonical supermolecular approach, calculations of interaction energies for molecular clusters involve a calculation of the whole cluster, which becomes expensive as the cluster size increases. We propose a novel approach to this task by demonstrating that interaction energies of such clusters can be constructed from those of small subclusters with a much lower computational cost by applying progressively lower-level methods for subsequent terms in the many-body expansion. The efficiency of such "stratified approximation" many-body approach (SAMBA) is due to the rapid convergence of the many-body expansion for typical molecular clusters. The method has been applied to water clusters (H(2)O)(n), n = 6, 16, 24. For the hexamer, the best results that can be obtained with current computational resources in the canonical supermolecular method were reproduced to within about one tenth of the uncertainty of the canonical approach while using 24 times less computer time in the many-body expansion calculations. For (H(2)O)(24), SAMBA is particularly beneficial and we report interaction energies with accuracy that is currently impossible to obtain with the canonical supermolecular approach. Moreover, our results were computed using two orders of magnitude smaller computer resources than used in the previous best calculations for this system. We also show that the basis-set superposition errors should be removed in calculations for large clusters.

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XO: An extended ONIOM method for accurate and efficient modeling of large systems

Guo

Zhang

et al. 2012

J Comput Chem

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Calculation of large complex systems remains to be a great challenge, where there is always a trade-off between accuracy and efficiency. Recently, we proposed the extended our own n-layered integrated molecular orbital (ONIOM) method (XO) (Guo, Wu, Xu, Chem. Phys. Lett. 2010, 498, 203) which surmounts some inherited limitations of the popular ONIOM method by introducing the inclusion-exclusion principle used in the fragmentation methods. The present work sets up general guidelines for the construction of a good XO scheme. In particular, force-error test is proposed to quantitatively validate the usefulness of an XO scheme, taking accuracy, efficiency and scalability all into account. Representative studies on zeolites, polypeptides and cyclodextrins have been carried out to demonstrate how to strive for high accuracy without sacrificing efficiency. As a natural extension, XO is applied to calculate the total energy, fully optimized geometry and vibrational spectra of the whole system, where ONIOM becomes inapplicable.

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Development of a 3-body:many-body integrated fragmentation method for weakly bound clusters and application to water clusters (H2O)n= 3 − 10, 16, 17

Cited by 71 publications

References 127 publications

Wavefunction methods for the accurate characterization of water clusters

Wavefunction methods for the accurate characterization of water clusters

Interaction energies of large clusters from many-body expansion

XO: An extended ONIOM method for accurate and efficient modeling of large systems

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