TY - JOUR
T1 - Advanced Potential Energy Surfaces for Molecular Simulation
AU - Albaugh, Alex
AU - Boateng, Henry A.
AU - Bradshaw, Richard T.
AU - Demerdash, Omar N.
AU - Dziedzic, Jacek
AU - Mao, Yuezhi
AU - Margul, Daniel T.
AU - Swails, Jason
AU - Zeng, Qiao
AU - Case, David A.
AU - Eastman, Peter
AU - Wang, Lee Ping
AU - Essex, Jonathan W.
AU - Head-Gordon, Martin
AU - Pande, Vijay S.
AU - Ponder, Jay W.
AU - Shao, Yihan
AU - Skylaris, Chris Kriton
AU - Todorov, Ilian T.
AU - Tuckerman, Mark E.
AU - Head-Gordon, Teresa
N1 - Publisher Copyright:
© 2016 American Chemical Society.
PY - 2016/9/22
Y1 - 2016/9/22
N2 - Advanced potential energy surfaces are defined as theoretical models that explicitly include many-body effects that transcend the standard fixed-charge, pairwise-additive paradigm typically used in molecular simulation. However, several factors relating to their software implementation have precluded their widespread use in condensed-phase simulations: the computational cost of the theoretical models, a paucity of approximate models and algorithmic improvements that can ameliorate their cost, underdeveloped interfaces and limited dissemination in computational code bases that are widely used in the computational chemistry community, and software implementations that have not kept pace with modern high-performance computing (HPC) architectures, such as multicore CPUs and modern graphics processing units (GPUs). In this Feature Article we review recent progress made in these areas, including well-defined polarization approximations and new multipole electrostatic formulations, novel methods for solving the mutual polarization equations and increasing the MD time step, combining linear-scaling electronic structure methods with new QM/MM methods that account for mutual polarization between the two regions, and the greatly improved software deployment of these models and methods onto GPU and CPU hardware platforms. We have now approached an era where multipole-based polarizable force fields can be routinely used to obtain computational results comparable to state-of-the-art density functional theory while reaching sampling statistics that are acceptable when compared to that obtained from simpler fixed partial charge force fields.
AB - Advanced potential energy surfaces are defined as theoretical models that explicitly include many-body effects that transcend the standard fixed-charge, pairwise-additive paradigm typically used in molecular simulation. However, several factors relating to their software implementation have precluded their widespread use in condensed-phase simulations: the computational cost of the theoretical models, a paucity of approximate models and algorithmic improvements that can ameliorate their cost, underdeveloped interfaces and limited dissemination in computational code bases that are widely used in the computational chemistry community, and software implementations that have not kept pace with modern high-performance computing (HPC) architectures, such as multicore CPUs and modern graphics processing units (GPUs). In this Feature Article we review recent progress made in these areas, including well-defined polarization approximations and new multipole electrostatic formulations, novel methods for solving the mutual polarization equations and increasing the MD time step, combining linear-scaling electronic structure methods with new QM/MM methods that account for mutual polarization between the two regions, and the greatly improved software deployment of these models and methods onto GPU and CPU hardware platforms. We have now approached an era where multipole-based polarizable force fields can be routinely used to obtain computational results comparable to state-of-the-art density functional theory while reaching sampling statistics that are acceptable when compared to that obtained from simpler fixed partial charge force fields.
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U2 - 10.1021/acs.jpcb.6b06414
DO - 10.1021/acs.jpcb.6b06414
M3 - Article
C2 - 27513316
AN - SCOPUS:84988884685
SN - 1520-6106
VL - 120
SP - 9811
EP - 9832
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 37
ER -