Application of the Wolf method for the evaluation of Coulombic interactions to complex condensed matter systems: Aluminosilicates and water

Demontis, Pierfranco; Spanu, Silvano; Suffritti, Giuseppe Baldovino

doi:10.1063/1.1364638

Cited by 91 publications

(106 citation statements)

References 9 publications

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“…In the QM/MM-DSF simulations, we used a damping parameter of α = 0.2/Å for the DSF potential. This value was shown to yield good convergence and numerical accuracy for Madelung energy on NaCl crystals in our previous study 39 and is also in close agreement with the optimal value of 2/R c (with an R c of 10-12 Å) suggested by Demontis et al 54 for Wolf summation.…”

Section: Simulation Detailssupporting

confidence: 72%

Treating electrostatics with Wolf summation in combined quantum mechanical and molecular mechanical simulations

Ojeda-May

2015

The Journal of Chemical Physics

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The Wolf summation approach [D. Wolf et al., J. Chem. Phys. 110, 8254 (1999)], in the damped shifted force (DSF) formalism [C. J. Fennell and J. D. Gezelter, J. Chem. Phys. 124, 234104 (2006)], is extended for treating electrostatics in combined quantum mechanical and molecular mechanical (QM/MM) molecular dynamics simulations. In this development, we split the QM/MM electrostatic potential energy function into the conventional Coulomb r −1 term and a term that contains the DSF contribution. The former is handled by the standard machinery of cutoff-based QM/MM simulations whereas the latter is incorporated into the QM/MM interaction Hamiltonian as a Fock matrix correction. We tested the resulting QM/MM-DSF method for two solution-phase reactions, i.e., the association of ammonium and chloride ions and a symmetric SN 2 reaction in which a methyl group is exchanged between two chloride ions. The performance of the QM/MM-DSF method was assessed by comparing the potential of mean force (PMF) profiles with those from the QM/MM-Ewald and QM/MM-isotropic periodic sum (IPS) methods, both of which include long-range electrostatics explicitly. For ion association, the QM/MM-DSF method successfully eliminates the artificial free energy drift observed in the QM/MM-Cutoff simulations, in a remarkable agreement with the two long-range-containing methods. For the SN 2 reaction, the free energy of activation obtained by the QM/MM-DSF method agrees well with both the QM/MM-Ewald and QM/MM-IPS results. The latter, however, requires a greater cutoff distance than QM/MM-DSF for a proper convergence of the PMF. Avoiding time-consuming lattice summation, the QM/MM-DSF method yields a 55% reduction in computational cost compared with the QM/MM-Ewald method. These results suggest that, in addition to QM/MM-IPS, the QM/MM-DSF method may serve as another efficient and accurate alternative to QM/MM-Ewald for treating electrostatics in condensed-phase simulations of chemical reactions. C 2015 AIP Publishing LLC. [http://dx

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Section: Simulation Detailssupporting

confidence: 72%

Treating electrostatics with Wolf summation in combined quantum mechanical and molecular mechanical simulations

Ojeda-May

2015

The Journal of Chemical Physics

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“…There is a close connection between the Wolf method and the Ewald method, but the Wolf method allows the long-ranged Coulomb interactions to be turned into relatively shortranged effective potentials by neutralizing the net charge of the system within the volume bounded by the cut-off radius. It was shown [29] that, in most systems of interest, the best reproduction of the results obtained by the Ewald method can be achieved with r c = L min /2 The adsorption properties were computed using the grand canonical Monte Carlo (MC) method in the zeolite NaA system with a fixed cubic box length of 2.4555 nm (therefore, r c and α were set to 1.22775 nm and 1.6290 nm, respectively). The length of the simulations was typically in the order of 10 8 MC moves in addition to an equilibration period of at least 8×10 7 MC moves.…”

Section: Introductionmentioning

confidence: 99%

Prediction of adsorption equilibria of water–methanol mixtures in zeolite NaA by molecular simulation

Kristóf

Csányi

Rutkai

et al. 2006

Molecular Simulation

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“…First, the self energy should be given by taking the appropriate limit for r ij ! 0; as shown in equation (4). Thus Second, the error term is now different from equation (5 …”

Section: Empirical Overlap Integralmentioning

confidence: 99%

“…The computational cost is thus reduced. For a detailed comparison of the computational efficiency of these two methods, see the paper by Demontis et al [4].…”

Section: Original Wolf Summentioning

confidence: 99%

“…The standard technique in dealing with this problem is the so called Ewald sum [2], in which the conditionally convergent sum in equation (1) is transformed mathematically into two rapid convergent series in both real and reciprocal spaces, as well as a self correction term. Despite its popularity, the use of the Ewald sum is problematic, especially for disordered systems where the artificially imposed periodicity in the Ewald sum is absent [3,4]. Computationally, this method is also very costly.…”

Section: Introductionmentioning

confidence: 99%

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Modified Wolf electrostatic summation: Incorporating an empirical charge overlap

Ma¹,

Garofalini²

2005

Molecular Simulation

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The original Wolf sum [D. Wolf et al., J. Chem. Phys. 110 (1999) was modified to account for the effect of charge overlap in an empirical manner in order to correct the direct 1/r coulomb interaction in covalent systems. The resulting modified Wolf sum takes a form that is similar to the original one. More importantly, the inclusion of the charge overlap effect does not introduce any additional systematic error. Thus, the error analysis can be evaluated either analytically for 3D periodic systems or estimated numerically for general cases, which is the same as in the original Wolf sum. Application of this modified Wolf sum to covalent or partially covalent systems such as SiC and SiO 2 shows that it gives a more realistic description of the electrostatic interactions in those systems. Although the Wolf method does not conserve energy in principle, in practice the energy is conserved very well. Thus this method is particular suitable in molecular dynamics simulations.

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Application of the Wolf method for the evaluation of Coulombic interactions to complex condensed matter systems: Aluminosilicates and water

Cited by 91 publications

References 9 publications

Treating electrostatics with Wolf summation in combined quantum mechanical and molecular mechanical simulations

Treating electrostatics with Wolf summation in combined quantum mechanical and molecular mechanical simulations

Prediction of adsorption equilibria of water–methanol mixtures in zeolite NaA by molecular simulation

Modified Wolf electrostatic summation: Incorporating an empirical charge overlap

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