Computer simulation of zeolite structure and reactivity using embedded cluster methods

Sherwood, Paul; Vries, Alex H. de; Collins, Simon J.; Greatbanks, Stephen P.; Burton, Neil A.; Vincent, Mark A.; Hillier, Ian H.

doi:10.1039/a701790a

Cited by 199 publications

(183 citation statements)

References 38 publications

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“…The conclusion that for a reaction that does not involve much charge transfer, the inclusion of the electrostatic field of the SS will yield small effects in relative energies but large affects in the electronic structure of the PS also gain supports from studies of zeolite-substrate systems [56]. In [56], it has been found that the inclusion of the electrostatic field of the SS slightly alters the barrier (by ca.…”

Section: What Do We Learn From a Qm/mm Calculation?mentioning

confidence: 78%

“…In [56], it has been found that the inclusion of the electrostatic field of the SS slightly alters the barrier (by ca. 2 kcal/mol) of a methyl shift reaction over a zeolite acid site, but has considerably large effects on the charge distribution and vibrational Comparing the results of QM/MM calculations with experimental results is the ultimate test of a QM/MM scheme.…”

Section: What Do We Learn From a Qm/mm Calculation?mentioning

confidence: 99%

“…In this subsection, we more specifically address some question about how to treat periodic systems and other solid-state materials such as metals, metal oxides, and surface-adsorbate systems. Excellent discussions [47,56,74,85,96,97,[101][102][103]108,115,133,140,145] are available for many aspects, and we focus here especially on studies of zeolites.…”

Section: Treating Solid-state Systemsmentioning

confidence: 99%

“…Nevertheless, the question is raised: are charge parameterized for a particular MM context also appropriate for use in a QM Hamiltonian? In an extreme case, for example, a zeolite-substrate system, the formal atomic charges used in aluminosilicate force field are chosen to reproduce the structural rather than electrostatic data; such charges may not be appropriate for the construction of the one-electron terms in the effective QM Hamiltonian [56].…”

Section: Electrostatic Embedding?mentioning

confidence: 99%

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QM/MM: what have we learned, where are we, and where do we go from here?

2006

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This paper briefly reviews the current status of the most popular methods for combined quantum mechanical/molecular mechanical (QM/MM) calculations, including their advantages and disadvantages. There is a special emphasis on very general link-atom methods and various ways to treat the charge near the boundary. Mechanical and electric embedding are contrasted. We consider methods applicable to gas-phase organic chemistry, liquid-phase organic and organometallic chemistry, biochemistry, and solid-state chemistry. Then we review some recent tests of QM/MM methods and summarize what we learn about QM/MM from these studies. We also discuss some available software. Finally, we present a few comments about future directions of research in this exciting area, where we focus on more intimate blends of QM with MM.

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Section: What Do We Learn From a Qm/mm Calculation?mentioning

confidence: 78%

Section: What Do We Learn From a Qm/mm Calculation?mentioning

confidence: 99%

Section: Treating Solid-state Systemsmentioning

confidence: 99%

Section: Electrostatic Embedding?mentioning

confidence: 99%

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QM/MM: what have we learned, where are we, and where do we go from here?

2006

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“…Among these are the QM/MM, [1][2][3][4][5][6] ONIOM, 7,8 fragment molecular orbital (FMO), [9][10][11][12][13][14][15] and wavefunction theory (WFT)-in-density functional theory (DFT) embedding [16][17][18][19][20][21][22][23][24][25][26][27][28][29][30] approaches, which allow for the treatment of systems that would not be practical using conventional WFT approaches. In particular, WFT-in-DFT embedding utilizes the theoretical framework of DFT embedding to enable the WFT description of a given subsystem in the effective potential that is created by the remaining electronic density of the system.…”

Section: Introductionmentioning

confidence: 99%

Accurate basis set truncation for wavefunction embedding

Barnes

Goodpaster

Manby³

et al. 2013

The Journal of Chemical Physics

127

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Density functional theory (DFT) provides a formally exact framework for performing embedded subsystem electronic structure calculations, including DFT-in-DFT and wavefunction theory-in-DFT descriptions. In the interest of efficiency, it is desirable to truncate the atomic orbital basis set in which the subsystem calculation is performed, thus avoiding high-order scaling with respect to the size of the MO virtual space. In this study, we extend a recently introduced projection-based embedding method [F. R. Manby, M. Stella, J. D. Goodpaster, and T. F. Miller III, J. Chem. Theory Comput. 8, 2564 (2012)] to allow for the systematic and accurate truncation of the embedded subsystem basis set. The approach is applied to both covalently and non-covalently bound test cases, including water clusters and polypeptide chains, and it is demonstrated that errors associated with basis set truncation are controllable to well within chemical accuracy. Furthermore, we show that this approach allows for switching between accurate projection-based embedding and DFT embedding with approximate kinetic energy (KE) functionals; in this sense, the approach provides a means of systematically improving upon the use of approximate KE functionals in DFT embedding. © 2013 AIP Publishing LLC. [http://dx

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Solids: Computer Modeling

Catlow

2005

Encyclopedia of Inorganic Chemistry

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We review the role of computer modeling techniques in solid state chemistry. The basic aims and objectives of the field are summarised. We then describe basic aspects of the methodologies both of techniques based on interatomic potentials and electronic structure methods. We consider the range of applicability of each technique. Later sections of the chapter describe recent topical examples including modeling and prediction of crystal structures, simulation of nano‐cluster structures and energies and modeling of reaction mechanisms in heterogeneously catalysed reactions.

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Computer simulation of zeolite structure and reactivity using embedded cluster methods

Cited by 199 publications

References 38 publications

QM/MM: what have we learned, where are we, and where do we go from here?

QM/MM: what have we learned, where are we, and where do we go from here?

Accurate basis set truncation for wavefunction embedding

Solids: Computer Modeling

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