Transfer learning for chemically accurate interatomic neural network potentials.

Developing machine learning-based interatomic potentials from ab initio electronic structure methods remains a challenging task for computational chemistry and materials science. This work studies the capability of transfer learning, in particular discriminative fine-tuning, for efficiently generating chemically accurate interatomic neural network potentials on organic molecules from the MD17 and ANI data sets. We show that pre-training the network parameters on data obtained from density functional calculations considerably improves the sample efficiency of models trained on more accurate ab initio data. Additionally, we show that fine-tuning with energy labels alone can suffice to obtain accurate atomic forces and run large-scale atomistic simulations, provided a well-designed fine-tuning data set. We also investigate possible limitations of transfer learning, especially regarding the design and size of the pre-training and fine-tuning data sets. Finally, we provide GM-NN potentials pre-trained and fine-tuned on the ANI-1x and ANI-1ccx data sets, which can easily be fine-tuned on and applied to organic molecules.

Predicting properties of periodic systems from cluster data: A case study of liquid water.

The accuracy of the training data limits the accuracy of bulk properties from machine-learned potentials. For example, hybrid functionals or wave-function-based quantum chemical methods are readily available for cluster data but effectively out of scope for periodic structures. We show that local, atom-centered descriptors for machine-learned potentials enable the prediction of bulk properties from cluster model training data, agreeing reasonably well with predictions from bulk training data. We demonstrate such transferability by studying structural and dynamical properties of bulk liquid water with density functional theory and have found an excellent agreement with experimental and theoretical counterparts.

Fast and Sample-Efficient Interatomic Neural Network Potentials for Molecules and Materials Based on Gaussian Moments.

Artificial neural networks (NNs) are one of the most frequently used machine learning approaches to construct interatomic potentials and enable efficient large-scale atomistic simulations with almost ab initio accuracy. However, the simultaneous training of NNs on energies and forces, which are a prerequisite for, e.g., molecular dynamics simulations, can be demanding. In this work, we present an improved NN architecture based on the previous GM-NN model [Zaverkin V.; Kästner, J. J. Chem. Theory Comput. 2020, 16, 5410-5421], which shows an improved prediction accuracy and considerably reduced training times. Moreover, we extend the applicability of Gaussian moment-based interatomic potentials to periodic systems and demonstrate the overall excellent transferability and robustness of the respective models. The fast training by the improved methodology is a prerequisite for training-heavy workflows such as active learning or learning-on-the-fly.

Muscles Reduce Neuronal Information Load: Quantification of Control Effort in Biological vs. Robotic Pointing and Walking.

It is hypothesized that the nonlinear muscle characteristic of biomechanical systems simplify control in the sense that the information the nervous system has to process is reduced through off-loading computation to the morphological structure. It has been proposed to quantify the required information with an information-entropy based approach, which evaluates the minimally required information to control a desired movement, i.e., control effort. The key idea is to compare the same movement but generated by different actuators, e.g., muscles and torque actuators, and determine which of the two morphologies requires less information to generate the same movement. In this work, for the first time, we apply this measure to numerical simulations of more complex human movements: point-to-point arm movements and walking. These models consider up to 24 control signals rendering the brute force approach of the previous implementation to search for the minimally required information futile. We therefore propose a novel algorithm based on the pattern search approach specifically designed to solve this constraint optimization problem. We apply this algorithm to numerical models, which include Hill-type muscle-tendon actuation as well as ideal torque sources acting directly on the joints. The controller for the point-to-point movements was obtained by deep reinforcement learning for muscle and torque actuators. Walking was controlled by proprioceptive neural feedback in the muscular system and a PD controller in the torque model. Results show that the neuromuscular models consistently require less information to successfully generate the movement than the torque-driven counterparts. These findings were consistent for all investigated controllers in our experiments, implying that this is a system property, not a controller property. The proposed algorithm to determine the control effort is more efficient than other standard optimization techniques and provided as open source.