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Register a new userUncertainty estimation for molecular dynamics and sampling
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Machine learning models have emerged as a very effective strategy to sidestep time-consuming electronic-structure calculations, enabling accurate simulations of greater size, time scale and complexity. Given the interpolative nature of these models, the reliability of predictions depends on the position in phase space, and it is crucial to obtain an estimate of the error that derives from the finite number of reference structures included during the training of the model. When using a machine-learning potential to sample a finite-temperature ensemble, the uncertainty on individual configurations translates into an error on thermodynamic averages, and provides an indication for the loss of accuracy when the simulation enters a previously unexplored region. Here we discuss how uncertainty quantification can be used, together with a baseline energy model, or a more robust although less accurate interatomic potential, to obtain more resilient simulations and to support active-learning strategies. Furthermore, we introduce an on-the-fly reweighing scheme that makes it possible to estimate the uncertainty in the thermodynamic averages extracted from long trajectories. We present examples covering different types of structural and thermodynamic properties, and systems as diverse as water and liquid gallium.
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We investigate the continuum limit that the number of beads goes to infinity in the ring polymer representation of thermal averages. Studying the continuum limit of the trajectory sampling equation sheds light on possible preconditioning techniques for sampling ring polymer configurations with large number of beads. We propose two preconditioned Langevin sampling dynamics, which are shown to have improved stability and sampling accuracy. We present a careful mode analysis of the preconditioned dynamics and show their connections to the normal mode, the staging coordinate and the Matsubara mode representation for ring polymers. In the case where the potential is quadratic, we show that the continuum limit of the preconditioned mass modified Langevin dynamics converges to its equilibrium exponentially fast, which suggests that the finite-dimensional counterpart has a dimension-independent convergence rate. In addition, the preconditioning techniques can be naturally applied to the multi-level quantum systems in the nonadiabatic regime, which are compatible with various numerical approaches.
When the cooling rate $v$ is smaller than a certain material-dependent threshold, the glass transition temperature $T_g$ becomes to a certain degree the material parameter being nearly independent on the cooling rate. The common method to determine $T_g$ is to extrapolate viscosity $ u$ of the liquid state at temperatures not far above the freezing conditions to lower temperatures where liquid freezes and viscosity is hardly measurable. It is generally accepted that the glass transition occurs when viscosity drops by $13leq nleq17$ orders of magnitude. The accuracy of $T_g$ depends on the extrapolation quality. We propose here an algorithm for a unique determining of $T_g$. The idea is to unambiguously extrapolate $ u(T)$ to low temperatures without relying upon a specific model. It can be done using the numerical analytical continuation of $ u(T)$-function from above $T_g$ where it is measurable, to $Tgtrsim T_g$. For numerical analytical continuation, we use the Pade approximant method.
We introduce Density sketches (DS): a succinct online summary of the data distribution. DS can accurately estimate point wise probability density. Interestingly, DS also provides a capability to sample unseen novel data from the underlying data distribution. Thus, analogous to popular generative models, DS allows us to succinctly replace the real-data in almost all machine learning pipelines with synthetic examples drawn from the same distribution as the original data. However, unlike generative models, which do not have any statistical guarantees, DS leads to theoretically sound asymptotically converging consistent estimators of the underlying density function. Density sketches also have many appealing properties making them ideal for large-scale distributed applications. DS construction is an online algorithm. The sketches are additive, i.e., the sum of two sketches is the sketch of the combined data. These properties allow data to be collected from distributed sources, compressed into a density sketch, efficiently transmitted in the sketch form to a central server, merged, and re-sampled into a synthetic database for modeling applications. Thus, density sketches can potentially revolutionize how we store, communicate, and distribute data.
We present a scheme to obtain an inexpensive and reliable estimate of the uncertainty associated with the predictions of a machine-learning model of atomic and molecular properties. The scheme is based on resampling, with multiple models being generated based on sub-sampling of the same training data. The accuracy of the uncertainty prediction can be benchmarked by maximum likelihood estimation, which can also be used to correct for correlations between resampled models, and to improve the performance of the uncertainty estimation by a cross-validation procedure. In the case of sparse Gaussian Process Regression models, this resampled estimator can be evaluated at negligible cost. We demonstrate the reliability of these estimates for the prediction of molecular energetics, and for the estimation of nuclear chemical shieldings in molecular crystals. Extension to estimate the uncertainty in energy differences, forces, or other correlated predictions is straightforward. This method can be easily applied to other machine learning schemes, and will be beneficial to make data-driven predictions more reliable, and to facilitate training-set optimization and active-learning strategies.
Many processes in chemistry and physics take place on timescales that cannot be explored using standard molecular dynamics simulations. This renders the use of enhanced sampling mandatory. Here we introduce an enhanced sampling method that is based on constructing a model probability density from which a bias potential is derived. The model relies on the fact that in a physical system most of the configurations visited can be grouped into isolated metastable islands. To each island we associate a distribution that is fitted to a Gaussian mixture. The different distributions are linearly combined together with coefficients that are computed self consistently. Remarkably, from this biased dynamics, rates of transition between different metastable states can be straightforwardly computed.
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