Efficient multiple time scale molecular dynamics: Using colored noise thermostats to stabilize resonances

Morrone, Joseph A.; Markland, Thomas E.; Ceriotti, Michele; Berne, B. J.

doi:10.1063/1.3518369

Cited by 69 publications

(89 citation statements)

References 39 publications

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“…It has been shown that resonance instabilities can be effectively mitigated using specially designed Langevin thermostats. 41,44 The application of these techniques here is beyond the scope of the Luehr, Markland and Martínez -Page 13 present study, but should increase the outer time step by a further factor of 2-4 fold and thus further improve the computational speedups reported here.…”

Section: Resultsmentioning

confidence: 99%

Multiple time step integrators in ab initio molecular dynamics

Luehr

Markland

Martı́nez

2014

The Journal of Chemical Physics

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Multiple time-scale algorithms exploit the natural separation of time-scales in chemical systems to greatly accelerate the efficiency of molecular dynamics simulations. Although the utility of these methods in systems where the interactions are described by empirical potentials is now well established, their application to ab initio molecular dynamics calculations has been limited by difficulties associated with splitting the ab initio potential into fast and slowly varying components. Here we show that such a timescale separation is possible using two different schemes: one based on fragment decomposition and the other on range separation of the Coulomb operator in the electronic Hamiltonian. We demonstrate for both water clusters and a solvated hydroxide ion that multiple time-scale molecular dynamics allows for outer time steps of 2.5 fs, which are as large as those obtained when such schemes are applied to empirical potentials, while still allowing for bonds to be broken and reformed throughout the dynamics. This permits computational speedups of up to 4.4x, compared to standard Born-Oppenheimer ab initio molecular dynamics with a 0.5 fs time step, while maintaining the same energy conservation and accuracy.

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Section: Resultsmentioning

confidence: 99%

Multiple time step integrators in ab initio molecular dynamics

Luehr

Markland

Martı́nez

2014

The Journal of Chemical Physics

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“…For GLE simulations we have adopted the method of Colored Noise thermostats [22,23,51]. Since this method can only deal with memory kernels given as a superposition of functions…”

Section: Simulation Detailsmentioning

confidence: 99%

Vibrational spectroscopy via the Caldeira-Leggett model with anharmonic system potentials

Gottwald

Ivanov

Kühn

2016

The Journal of Chemical Physics

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Abstract. The Caldeira-Leggett (CL) model, which describes a system bi-linearly coupled to a harmonic bath, has enjoyed popularity in condensed phase spectroscopy owing to its utmost simplicity. However, the applicability of the model to cases with anharmonic system potentials, as it is required for the description of realistic systems in solution, is questionable due to the presence of the invertibility problem [J. Phys. Chem. Lett., 6, 2722Lett., 6, (2015] unless the system itself resembles the CL model form. This might well be the case at surfaces or in the solid regime, which we here confirm for a particular example of an iodine molecule in the atomic argon environment under high pressure. For this purpose we extend the recently proposed Fourier method for parameterizing linear generalized Langevin dynamics [J. Chem. Phys., 142, 244110 (2015)] to the non-linear case based on the CL model and perform an extensive error analysis. In order to judge on the applicability of this model in advance, we give handy empirical criteria and discuss the effect of the potential renormalization term. The obtained results provide evidence that the CL model can be used for describing a potentially broad class of systems.

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“…Solving the GLE for complex heterogeneous and extended systems is still a challenge. A major step towards the solution of this problem for a realistic application has been recently given [43,44,47,48,52]. In particular, an efficient and transferable algorithm has been developed in Ref.…”

Section: Introductionmentioning

confidence: 99%

Nonequilibrium processes from generalized Langevin equations: Realistic nanoscale systems connected to two thermal baths

et al. 2016

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We extend the generalized Langevin equation (GLE) method [L. Stella, C. D. Lorenz, and L. Kantorovich, Phys. Rev. B 89, 134303 (2014)] to model a central classical region connected to two realistic thermal baths at two different temperatures. In such nonequilibrium conditions a heat flow is established, via the central system, in between the two baths. The GLE-2B (GLE two baths) scheme permits us to have a realistic description of both the dissipative central system and its surrounding baths. Following the original GLE approach, the extended Langevin dynamics scheme is modified to take into account two sets of auxiliary degrees of freedom corresponding to the mapping of the vibrational properties of each bath. These auxiliary variables are then used to solve the non-Markovian dissipative dynamics of the central region. The resulting algorithm is used to study a model of a short Al nanowire connected to two baths. The results of the simulations using the GLE-2B approach are compared to the results of other simulations that were carried out using standard thermostatting approaches (based on Markovian Langevin and Nosé-Hoover thermostats). We concentrate on the steady-state regime and study the establishment of a local temperature profile within the system. The conditions for obtaining a flat profile or a temperature gradient are examined in detail, in agreement with earlier studies. The results show that the GLE-2B approach is able to treat, within a single scheme, two widely different thermal transport regimes, i.e., ballistic systems, with no temperature gradient, and diffusive systems with a temperature gradient.

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Efficient multiple time scale molecular dynamics: Using colored noise thermostats to stabilize resonances

Cited by 69 publications

References 39 publications

Multiple time step integrators in ab initio molecular dynamics

Multiple time step integrators in ab initio molecular dynamics

Vibrational spectroscopy via the Caldeira-Leggett model with anharmonic system potentials

Nonequilibrium processes from generalized Langevin equations: Realistic nanoscale systems connected to two thermal baths

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