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Advances in QM/MM Molecular Dynamics Simulations of Chemical Processes at Aqueous Interfaces

  • Marilia T. C. Martins-Costa
  • Manuel F. Ruiz-LópezEmail author
Chapter
Part of the Challenges and Advances in Computational Chemistry and Physics book series (COCH, volume 21)

Abstract

We review recent studies carried out in our group on the modeling of aqueous interfaces using Molecular Dynamics simulations with a combined Quantum Mechanics and Molecular Mechanics force-field (QM/MM ). We first present the methodology and we comment on some ongoing developments. Since in the QM/MM approach the adsorbed molecule is described quantum mechanically, this computational scheme has allowed us to get insights on interface solvation effects on molecular properties. In particular, we have shown that polarization phenomena at the air–water interface may produce larger effects than polarization in bulk water. This finding contrasts with the usual assumption that polarity at liquid interfaces is close to the arithmetic average of the polarity of the two bulk phases, and that solvation effects at the air–water interface should be similar to the effects in a low polar solvent such as butyl ether. A summary of previous results is presented with some selected examples that are briefly discussed, and which include systems of atmospheric interest at the air–water interface, as well as systems of biological relevance at a water-organic interface. Then, we report some new results for a series of small volatile organic compounds at the air–water interface, namely methyl chloride, acetonitrile and methanol. These molecules share a similar structure but display quite different behaviors at the interface; the discussion focuses on the orientational dynamics and the solvation effects on reactivity indices. Finally, some conclusions and future directions in this exciting field are presented.

Keywords

Molecular Dynamics Simulation Volatile Organic Compound Water Interface Liquid Interface Radial Distribution Function 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.

Acronyms

B3LYP

Becke’s 3-parameter-Lee-Yang-Parr exchange-correlation functional defined in reference [64]

HF

Hartree-Fock method

HOMO

Highest occupied molecular orbital

LUMO

Lowest unoccupied molecular orbital

MM

Molecular mechanics

MD

Molecular dynamics

NVT

Canonical ensemble (constant number of particles, constant volume, constant temperature)

QM

Quantum mechanics

ROS

Reactive oxygen species

SCF

Self-consistent field method

SFG

Sum frequency generation

VOC

Volatile organic compound

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Copyright information

© Springer International Publishing Switzerland 2015

Authors and Affiliations

  • Marilia T. C. Martins-Costa
    • 1
  • Manuel F. Ruiz-López
    • 1
    Email author
  1. 1.SRSMCUniversity of Lorraine and CNRSVandoeuvre-lès-NancyFrance

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