Accurate Computation of Gas Uptake in Microporous Organic Molecular Crystals

Li, Wenliang; Krieg, Helge; Möllmann, Jonas; Zhang, Jingping

doi:10.1021/jp2112632

Cited by 43 publications

(65 citation statements)

References 75 publications

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“…These simulations produce isotherms that can be compared to experimental results, but can also highlight favourable adsorption sites. 12,[83][84][85] However, as previously mentioned, PMMs exhibit significant structural flexibility and as a result the accuracy of conventional Monte Carlo simulations may be compromised. 86 GCMC typically treats the porous material as a rigid structure, accordingly, any dynamic porosity or structural responses (such as swelling) in response to guest molecules is ignored.…”

Section: Gas Adsorptionmentioning

confidence: 99%

“…9, however, there was significant overestimation at elevated temperatures and for N 2 , CH 4 and Xe gases. 84 There are a number of computational routes to simulate gas sorption for soft materials that undergo phase transitions, 87 though we note these approaches have only been applied to a limited number of materials. 88,89 In spite of the challenges outlined here, these simulations have still been useful in predicting and understanding gas adsorption Please do not adjust margins…”

Section: Gas Adsorptionmentioning

confidence: 99%

“…This can be simply for characterising the interaction energy between the material and the gas 82 or to generate tailored model potentials for GCMC simulations. 84 A unique approach was recently applied by Barbour and coworkers. 90 Three states, were modeled using DFT simulations; an empty metallocycle, a metallocycle with one guest and a metallocycle with two guests (the maximum occupancy).…”

Section: Gas Adsorptionmentioning

confidence: 99%

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Application of computational methods to the design and characterisation of porous molecular materials

et al. 2017

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Composed from discete units, porous molecular materials (PMMs) possess unique properties not observed for conventional, extended, solids, such as solution processibility and permanent porosity in the liquid phase. However, identifying the origin of porosity is not a trivial process, especially for amorphous or liquid phases. Furthermore, the assembly of molecular components is typically governed by a subtle balance of weak intermolecular forces that makes structure prediction challenging. Accordingly, in this review we canvass the crucial role of molecular simulations in the characterisation and design of PMMs. We will outline strategies for modelling porosity in crystalline, amorphous and liquid phases and also describe the state-of-the-art methods used for high-throughput screening of large datasets to identify materials that exhibit novel performance characteristics.

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Section: Gas Adsorptionmentioning

confidence: 99%

Section: Gas Adsorptionmentioning

confidence: 99%

Section: Gas Adsorptionmentioning

confidence: 99%

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Application of computational methods to the design and characterisation of porous molecular materials

et al. 2017

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“…Other recent applications, the (necessarily limited and biased) following selection tries only to show the wide and rich range of systems being currently afforded, include the modelling of ionic liquids [175], gas adsorption in metalorganic frameworks [176,177], isomerism in monosaccharides [178], conformational analysis [179,180], nonlinear optical responses [181], magnetic couplings in organometallics [182], enzymatic catalysis [183,184], electron paramagnetic resonance hyperfine coupling tensors [185], inclusion complexes and nanoencapsulation [186], electronic circular dichroism [187], organometallic complexes of graphene [188], interfacial chemistry [189], photosynthetic water oxidation [190], hyperpolarizability of pushpull systems [191], lightharvesting complexes [192], adsorbate-zeolite interactions [193], or harmonic and anharmonic vibrational frequency calculations [194], among others. • Figure 1.…”

Section: Self-interaction Errormentioning

confidence: 99%

Double-hybrid density functionals: merging wavefunction and density approaches to get the best of both worlds

Sancho‐García

Adamo

2013

Phys. Chem. Chem. Phys.

109

108

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We review in this Perspective why and how double-hybrid density functionals have become new leading actors in the field of computational chemistry, thanks to the combination of an unprecedented accuracy together with large robustness and reliability. Similarly to their predecessors, the widely employed hybrid density functionals, they are rooted on the Adiabatic Connection Method from which they emerge in a natural way. We present recent achievements concerning applications to chemical systems of the most interest, and current extensions to deal with challenging issues such as non-covalent interactions and excitation energies. These promising methods, despite a slightly higher computational cost than other typical density-based models, are called to play a key role in the near future and can thus pave the way towards new discoveries or advances.2

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“…20,21 These simultaneous optimizations of different force field terms can take advantage of extensive training sets that can be easily generated using electronic structure calculations and may include data on the intermolecular interaction energies. [22][23][24][25][26] Moreover, in this approach the fitted interaction energy would implicitly include the polarization effects, even staying within the fixed point-charge force field framework. 9,27,28 However, such simultaneous force field fitting represents a technically challenging multiobjective optimization of the parameters of different physical nature.…”

Section: Introductionmentioning

confidence: 99%

Genetic Algorithm Optimization of Point Charges in Force Field Development: Challenges and Insights

2015

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Evolutionary methods, such as genetic algorithms (GAs), provide powerful tools for optimization of the force field parameters, especially in the case of simultaneous fitting of the force field terms against extensive reference data. However, GA fitting of the nonbonded interaction parameters that includes point charges has not been explored in the literature, likely due to numerous difficulties with even a simpler problem of the least-squares fitting of the atomic point charges against a reference molecular electrostatic potential (MEP), which often demonstrates an unusually high variation of the fitted charges on buried atoms. Here, we examine the performance of the GA approach for the least-squares MEP point charge fitting, and show that the GA optimizations suffer from a magnified version of the classical buried atom effect, producing highly scattered yet correlated solutions. This effect can be understood in terms of the linearly independent, natural coordinates of the MEP fitting problem defined by the eigenvectors of the least-squares sum Hessian matrix, which are also equivalent to the eigenvectors of the covariance matrix evaluated for the scattered GA solutions. GAs quickly converge with respect to the high-curvature coordinates defined by the eigenvectors related to the leading terms of the multipole expansion, but have difficulty converging with respect to the low-curvature coordinates that mostly depend on the buried atom charges. The performance of the evolutionary techniques dramatically improves when the point charge optimization is performed using the Hessian or covariance matrix eigenvectors, an approach with a significant potential for the evolutionary optimization of the fixed-charge biomolecular force fields.

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Accurate Computation of Gas Uptake in Microporous Organic Molecular Crystals

Cited by 43 publications

References 75 publications

Application of computational methods to the design and characterisation of porous molecular materials

Application of computational methods to the design and characterisation of porous molecular materials

Double-hybrid density functionals: merging wavefunction and density approaches to get the best of both worlds

Genetic Algorithm Optimization of Point Charges in Force Field Development: Challenges and Insights

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