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Voltage equilibration for reactive atomistic simulations of electrochemical processes
3.M. Karplus, “Development of multiscale models for complex chemical systems: From H+H2 to biomolecules (Nobel lecture),” Angew. Chem., Int. Ed. Engl. 53(38), 9992 (2014).
7.A. Strachan, G. Klimeck, and M. Lundstrom, “Cyber-enabled simulations in nanoscale science and engineering introduction,” Comput. Sci. Eng. 12(2), 12–17 (2010).
8.S. P. Brophy, A. J. Magana, and A. Strachan, “Lectures and simulation laboratories to improve learners conceptual understanding,” Adv. Eng. Educ. 3(3), 1–27 (2013).
10.M. Sprik, J. Hutter, and M. Parrinello, “Ab initio molecular dynamics simulation of liquid water: Comparison three gradient-corrected density functionals,” J. Chem. Phys. 105(3), 1142–1152 (1996).
12.M. S. Daw and M. I. Baskes, “Embedded-atom method—Derivation and application to impurities, surfaces, and other defects in metals,” Phys. Rev. B 29(12), 6443–6453 (1984).
18.S. L. Mayo, B. D. Olafson, and W. A. Goddard, “Dreiding—A generic force-field for molecular simulations,” J. Phys. Chem. 94(26), 8897–8909 (1990).
19.W. D. Cornell, P. Cieplak, C. I. Bayly, I. R. Gould, K. M. Merz, D. M. Ferguson, D. C. Spellmeyer, T. Fox, J. W. Caldwell, and P. A. Kollman, “A second generation force field for the simulation of proteins, nucleic acids, and organic molecules (Vol. 117,p. 5179, 1995),” J. Am. Chem. Soc. 118(9), 2309 (1996).
20.B. R. Brooks, C. L. Brooks III, A. D. Mackerell, Jr., L. Nilsson, R. J. Petrella, B. Roux, Y. Won, G. Archontis, C. Bartels, S. Boresch, A. Caflisch, L. Caves, Q. Cui, A. R. Dinner, M. Feig, S. Fischer, J. Gao, M. Hodoscek, W. Im, K. Kuczera, T. Lazaridis, J. Ma, V. Ovchinnikov, E. Paci, R. W. Pastor, C. B. Post, J. Z. Pu, M. Schaefer, B. Tidor, R. M. Venable, H. L. Woodcock, X. Wu, W. Yang, D. M. York, and M. Karplus, “CHARMM: The biomolecular simulation program,” J. Comput. Chem. 30(10, SI), 1545–1614 (2009).
21.A. C. T. van Duin, S. Dasgupta, F. Lorant, and W. A. Goddard, “ReaxFF: A reactive force field for hydrocarbons,” J. Phys. Chem. A 105(41), 9396–9409 (2001).
22.H. S. Johnston and C. Parr, “Activation energies from bond energies. 1. Hydrogen transfer reactions,” J. Am. Chem. Soc. 85(17), 2544–2551 (1963).
23.S. W. Rick, S. J. Stuart, and B. J. Berne, “Dynamical fluctuating charge force-fields - application to liquid water,” J. Chem. Phys. 101(7), 6141–6156 (1994).
24.A. Strachan, A. C. T. van Duin, D. Chakraborty, S. Dasgupta, and W. A. Goddard, “Shock waves in high-energy materials: The initial chemical events in nitramine RDX,” Phys. Rev. Lett. 91(9), 098301 (2003).
25.J. C. Fogarty, H. M. Aktulga, A. Y. Grama, A. C. T. van Duin, and S. A. Pandit, “A reactive molecular dynamics simulation of the silica-water interface,” J. Chem. Phys. 132(17), 174704 (2010).
26.A. C. T. van Duin, V. S. Bryantsev, M. S. Diallo, W. A. Goddard, O. Rahaman, D. J. Doren, D. Raymand, and K. Hermansson, “Development and validation of a ReaxFF reactive force field for Cu cation/water interactions and copper metal/metal oxide/metal hydroxide condensed phases,” J. Phys. Chem. A 114(35), 9507–9514 (2010).
27.K. D. Nielson, A. C. T. van Duin, J. Oxgaard, W. Q. Deng, and W. A. Goddard, “Development of the ReaxFF reactive force field for describing transition metal catalyzed reactions, with application to the initial stages of the catalytic formation of carbon nanotubes,” J. Phys. Chem. A 109(3), 493–499 (2005).
31.W. B. Dapp and M. H. Mueser, “Redox reactions with empirical potentials: Atomistic battery discharge simulations,” J. Chem. Phys. 139(6), 064106 (2013).
32.C. Merlet, B. Rotenberg, P. A. Madden, P.-L. Taberna, P. Simon, Y. Gogotsi, and M. Salanne, “On the molecular origin of supercapacitance in nanoporous carbon electrodes,” Nat. Mater. 11(4), 306–310 (2012).
33.N. Onofrio, D. Guzman, and A. Strachan, “Atomic origin of ultrafast resistance switching in nanoscale electrometallization cells,” Nat. Mater. 14, 440–446 (2015).
35.S. J. Stuart, A. B. Tutein, and J. A. Harrison, “A reactive potential for hydrocarbons with intermolecular interactions,” J. Chem. Phys. 112(14), 6472–6486 (2000).
36.D. W. Brenner, O. A. Shenderova, J. A. Harrison, S. J. Stuart, B. Ni, and S. B. Sinnott, “A second-generation reactive empirical bond order (REBO) potential energy expression for hydrocarbons,” J. Phys.: Condens. Matter 14(4), 783–802 (2002).
37.W. J. Mortier, S. K. Ghosh, and S. Shankar, “Electronegativity equalization method for the calculation of atomic charges in molecules,” J. Am. Chem. Soc. 108(15), 4315–4320 (1986).
38.R. A. Nistor, J. G. Polihronov, M. H. Muser, and N. J. Mosey, “A generalization of the charge equilibration method for nonmetallic materials,” J. Chem. Phys. 125(9), 094108 (2006).
39.T. Verstraelen, P. W. Ayers, V. Van Speybroeck, and M. Waroquier, “ACKS2: Atom-condensed Kohn-Sham DFT approximated to second order,” J. Chem. Phys. 138(7), 074108 (2013).
40.J. Chen and T. J. Martinez, “Charge conservation in electronegativity equalization and its implications for the electrostatic properties of fluctuating-charge models,” J. Chem. Phys. 131(4), 044114 (2009).
41.O. Assowe, O. Politano, V. Vignal, P. Arnoux, B. Diawara, O. Verners, and A. C. T. van Duin, “Reactive molecular dynamics of the initial oxidation stages of Ni(111) in pure water: Effect of an applied electric field,” J. Phys. Chem. A 116(48), 11796–11805 (2012).
43.K.-H. Lin, B. L. Holian, T. C. Germann, and A. Strachan, “Mesodynamics with implicit degrees of freedom,” J. Chem. Phys. 141(6), 064107 (2014).
45.J. D. Jackson, Classical Electrodynamics, 3rd ed. (John Wiley & Sons, Inc., New Jersey, USA, 1991).
49.H. M. Aktulga, J. C. Fogarty, S. A. Pandit, and A. Y. Grama, “Parallel reactive molecular dynamics: Numerical methods and algorithmic techniques,” Parallel Comput. 38(4-5), 245–259 (2012).
50.R. Waser, R. Dittmann, G. Staikov, and K. Szot, “Redox-based resistive switching memories–nanoionic mechanisms, prospects, and challenges,” Adv. Mater. 21(25-26), 2632 (2009).
51.N. L. Anderson, R. P. Vedula, P. A. Schultz, R. M. Van Ginhoven, and A. Strachan, “First-principles investigation of low energy E′ center precursors in amorphous silica,” Phys. Rev. Lett. 106(20), 206402 (2011).
52.T. Tsuruoka, K. Terabe, T. Hasegawa, I. Valov, R. Waser, and M. Aono, “Effects of moisture on the switching characteristics of oxide-based, gapless-type atomic switches,” Adv. Funct. Mater. 22(1), 70–77 (2012).
53.I. Valov, I. Sapezanskaia, A. Nayak, T. Tsuruoka, T. Bredow, T. Hasegawa, G. Staikov, M. Aono, and R. Waser, “Atomically controlled electrochemical nucleation at superionic solid electrolyte surfaces,” Nat. Mater. 11(6), 530–535 (2012).
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We introduce electrochemical
dynamics with implicit degrees of freedom (EChemDID), a model to describe electrochemical driving force in reactive molecular dynamics simulations. The method describes the equilibration of external electrochemical potentials (voltage) within metallic structures and their effect on the self-consistent partial atomic charges used in reactive molecular dynamics. An additional variable assigned to each atom denotes the local potential in its vicinity and we use fictitious, but computationally convenient, dynamics to describe its equilibration within connected metallic structures on-the-fly during the molecular dynamics simulation. This local electrostatic potential is used to dynamically modify the atomic electronegativities used to compute partial atomic changes via charge equilibration. Validation tests show that the method provides an accurate description of the electric fields generated by the applied voltage and the driving force for electrochemical
reactions. We demonstrate EChemDID via simulations of the operation of electrochemical metallization cells. The simulations predict the switching of the device between a high-resistance to a low-resistance state as a conductive metallic bridge is formed and resistive currents that can be compared with experimental measurements. In addition to applications in nanoelectronics, EChemDID could be useful to model electrochemical energy conversion devices.
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