<i>Ab initio</i> based force field and molecular dynamics simulations of crystalline TATB

Gee, Richard H.; Roszak, Szczepan; Balasubramanian, K.; Fried, Laurence E.

doi:10.1063/1.1676120

Cited by 95 publications

(92 citation statements)

References 37 publications

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“…4, Dimers a and c, have been discussed using quantum chemical methods [18][19][20]. An all-atom molecular forcefield for TATB was established by Gee et al [18] to simulate its isobaric thermal expansion and isothermal compression under hydrostatic pressures, resulting in good agreement with experiment. In this forcefield, the intermolecular interaction potential is determined by the single-point energies of TATB dimers calculated using the MP2/6-31 G(d, p) method.…”

Section: Methodologiesmentioning

confidence: 99%

Why is the crystal shape of TATB is so similar to its molecular shape? Understanding by only its root molecule

et al. 2011

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We present an understanding of the quasi-regular or regular hexagonal enlargement of 1,3,5-triamino-2,4,6 (TATB) from its root molecule to its bulk crystal, by only its root molecule. That is, the mechanism of regular hexagonal TATB molecules stacking to a quasi-regular or regular hexagonal TATB crystal was discussed using a combined method of a density functional theory BLYP and Dreiding forcefield, and a series of static scanning calculations. As a result, we found that there are two styles of forming the most energetically favored TATB dimers: a hydrogen bonding along the molecular plane and an offset π-stacking vertical to the plane, just leading to the outspread and the thickening of the regular hexagon during the crystal growth, respectively. At the same time, it was found that the rotation of one TATB layer in any parallel stacked double-layer should overcome a very high energy barrier. It suggests that the TATB molecules or layers are arranged on the crystal face always along the special orientation of a regular hexagon and other orientations are strongly thermodynamically forbidden, resulting in a hexagonal crystal bulk.

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Section: Methodologiesmentioning

confidence: 99%

Why is the crystal shape of TATB is so similar to its molecular shape? Understanding by only its root molecule

et al. 2011

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“…25 The MK charges were shown to properly reproduce the electrostatic interactions in the molecular crystal of TATB. 26 The ab initio MK charges thus derived were used in the MD simulations.…”

Section: Theoretical Methodsmentioning

confidence: 99%

New theoretical insight into the interactions and properties of formic acid: Development of a quantum-based pair potential for formic acid

Roszak

Gee

Balasubramanian

et al. 2005

The Journal of Chemical Physics

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We performed ab initio quantum chemical studies for the development of intra and intermolecular interaction potentials for formic acid for use in molecular dynamics simulations of formic acid molecular crystal. The formic acid structures considered in the ab initio studies include both the cis and trans monomers which are the conformers that have been postulated as part of chains constituting liquid and crystal phases under extreme conditions. Although the cis to trans transformation is not energetically favored, the trans isomer was found as a component of stable gas-phase species. Our decomposition scheme for the interaction energy indicates that the hydrogen bonded complexes are dominated by the Hartree-Fock forces while parallel clusters are stabilized by the electron correlation energy. The calculated three-body and higher interactions are found to be negligible, thus rationalizing the development of an atom-atom pair potential for formic acid based on high-level ab initio calculations of small formic acid clusters. Here we present an atom-atom pair potential that includes both intra-and inter-molecular degrees of freedom for formic acid. The newly developed pair potential is used to examine formic acid in the condensed phase via molecular dynamics simulations. The isothermal compression under hydrostatic pressure obtained from molecular dynamics simulations is in good agreement with experiment. Further, the calculated equilibrium melting temperature is found to be in good agreement with experiment.3

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“…In the temperature range of our interest (-54 to 74°C) the libration mechanism is unlikely, as is supported by atomistic simulations using a recently-developed forcefield [24], as well as X-ray observations [18].…”

Section: Mesoscale Interactionsmentioning

confidence: 63%

“…This is accomplished by the Wulff construction procedure [22] as automated in the Morphology module [23] from Accelrys. For the surface energy calculations we employed an accurate inter-atomic potential developed for TATB [24].…”

Section: Model Constructionmentioning

confidence: 99%

Irreversible volume growth in polymer-bonded powder systems: Effects of crystalline anisotropy, particle size distribution, and binder strength

Maiti

Gee

Hoffman

et al. 2008

Journal of Applied Physics

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Pressed-powdered crystallites of intrinsically anisotropic materials have been shown to undergo irreversible volume expansion when subjected to repeated cycles of heating and cooling. In a previous letter publication [R. H. Gee et al., Appl. Phys. Lett. 70, 254105 (2007)], we developed a coarse-grained (micron-scale) interaction Hamiltonian for such a system and quantitatively reproduced experimentally observed irreversible growth through explicit molecular dynamics simulations. In this paper, we report (1) recent experiments with a high-density fluoropolymer binder that significantly lowers irreversible growth, (2) identification of a critical interaction parameter of our model that has a strong correlation with binder properties, (3) sensitivity of irreversible growth to the details of particle size and alignment distribution, and (4) a physical picture of irreversible growth in terms of particle displacements.

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Ab initio based force field and molecular dynamics simulations of crystalline TATB

Cited by 95 publications

References 37 publications

Why is the crystal shape of TATB is so similar to its molecular shape? Understanding by only its root molecule

Why is the crystal shape of TATB is so similar to its molecular shape? Understanding by only its root molecule

New theoretical insight into the interactions and properties of formic acid: Development of a quantum-based pair potential for formic acid

Irreversible volume growth in polymer-bonded powder systems: Effects of crystalline anisotropy, particle size distribution, and binder strength

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