Chemical Physics at Interfaces within a Refrigerant-Lubricated Contact: From Electronic Structure to Large-Scale Molecular Dynamics Simulations

Tromp, Stéphane; Joly, Laurent; Cobián, Manuel; Fillot, Nicolas

doi:10.1021/acs.jpcc.7b11267

Cited by 8 publications

(19 citation statements)

References 53 publications

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“…Thus, only non-bonded interfacial interactions between atoms in the amide molecules with the iron oxide surface atoms are directly parameterized. [41][42][43] In most FFs, such interactions are described using the 12-6 LJ 31 and Coulombic pair potentials: 30,32…”

Section: Interface Force-field Parameterizationmentioning

confidence: 99%

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Simulating Surfactant–Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

et al. 2019

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Understanding the behaviour of surfactant molecules on iron oxide surfaces is important for many industrial applications. Molecular dynamics (MD) simulations of such systems have been limited by the absence of a force-field (FF) which accurately describes the molecule-surface interactions. In this study, interaction energies from density functional theory (DFT) + U calculations with a van der Waals functional are used to parameterize a classical FF for MD simulations of amide surfactants on iron oxide surfaces. The Original FF, which was derived using mixing rules and surface Lennard-Jones (LJ) parameters developed for nonpolar molecules, were shown to significantly underestimate the adsorption energy and overestimate the equilibrium adsorption distance compared to DFT. Conversely, the Optimized FF showed excellent agreement with the interaction energies obtained from DFT calculations for a wide range of surface coverages and molecular conformations near to and adsorbed on α-Fe 2 O 3 (0001).

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Section: Interface Force-field Parameterizationmentioning

confidence: 99%

“…Thus, the performance of the Optimized FF compares favorably with interface FFs developed for other molecule-surface combinations where direct comparisons between E int from the FF and DFT were conducted. 43,62,64 Large-scale NEMD simulations…”

Section: Interface Force-field Parameterizationmentioning

confidence: 99%

Simulating Surfactant–Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

et al. 2019

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“…FFs developed for other molecule-surface combinations where direct comparisons between E int from the FF and DFT were conducted. 43,62,64 Large-scale NEMD simulations…”

Section: Resultsmentioning

confidence: 99%

“…This has been shown by numerous theoretical and experimental studies to be the most stable termination of α-Fe 2 O 3 at room temperature. 54 The α-Fe 2 O 3 (0001) surface 42 as well as the α-Fe 2 O 3 (0012) surface 43 have been used in recent FF parameterization studies. In tribology experiments, it is possible that the outer layer of α-Fe 2 O 3 (0001) will become hydroxylated 55 due to water contamination of the lubricant.…”

Section: Methodsmentioning

confidence: 99%

“…where E sys is the total energy of the adsorbed system, E surf is the total energy of the α- Interface force-field parameterization Thus, only non-bonded interfacial interactions between atoms in the amide molecules with the iron oxide surface atoms are directly parameterized. [41][42][43] In most FFs, such interactions are described using the 12-6 LJ 31 and Coulombic pair potentials: 30,32…”

Section: Interaction Energymentioning

confidence: 99%

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Simulating Surfactant-Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

Latorre¹,

Ewen

Gattinoni³

et al. 2019

Preprint

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<div>Understanding the behaviour of surfactant molecules on iron oxide surfaces is important for many industrial applications. Molecular dynamics (MD) simulations of such systems have been limited by the absence of a force-feild (FF) which accurately describes the molecule-surface interactions. In this study, interaction energies from density functional theory (DFT) + U calculations with a van der Waals functional are used to parameterize a classical FF for MD simulations of amide surfactants on iron oxide surfaces. The Original FF, which was derived using mixing rules and surface Lennard-Jones (LJ) parameters developed for nonpolar molecules, were shown to signi cantly underestimate the adsorption energy and overestimate the equilibrium adsorption distance compared to DFT. Conversely, the Optimized FF showed excellent agreement with the interaction energies obtained from DFT calculations for a wide range of surface coverages and molecular conformations near to and adsorbed on a-Fe2O3(0001). This was facilitated through the use of a Morse potential for strong chemisorption interactions, modi fied LJ parameters for weaker physisorption interactions, and adjusted partial charges for the electrostatic interactions. The Original FF and Optimized FF were compared in classical nonequilibrium molecular dynamics (NEMD) simulations of amide molecules con fined between iron oxide surfaces. When the Optimized FF was employed, the amide molecules were pulled closer to the surface and the orientation of the headgroups was more similar to that observed in the DFT calculations compared to the Original FF. The Optimized FF proposed here facilitates classical MD simulations of amide-iron oxide interfaces in which the interactions are representative of accurate DFT calculations.</div>

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Tribological Performance of the R1233zd Refrigerant in Extreme Confinement at the Nanoasperity Level: A Molecular Dynamics Study Using an ab Initio-Based Force Field

et al. 2019

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Chemical Physics at Interfaces within a Refrigerant-Lubricated Contact: From Electronic Structure to Large-Scale Molecular Dynamics Simulations

Cited by 8 publications

References 53 publications

Simulating Surfactant–Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

Simulating Surfactant–Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

Simulating Surfactant-Iron Oxide Interfaces: From Density Functional Theory to Molecular Dynamics

Tribological Performance of the R1233zd Refrigerant in Extreme Confinement at the Nanoasperity Level: A Molecular Dynamics Study Using an ab Initio-Based Force Field

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