Global optimization of atomic clusters via physically constrained tensor train decomposition

Physical Review B: Condensed Matter and Materials Physics. 2026. Vol. 113. No. 22. Article 224111.

Sozykin K., Rybin N., Chertkov A., Phan A., Oseledets I., Shapeev A., Novikov I., Ryzhakov G.

The global optimization of atomic clusters represents a fundamental challenge in computational chemistry and materials science due to the exponential growth of local minima with system size (i.e., the curse of dimensionality). We introduce a framework that overcomes this limitation by exploiting the low-rank structure of potential energy surfaces through tensor train (TT) decomposition. Our approach combines two complementary TT-based strategies: the algebraic TTOpt method, which utilizes maximum volume sampling, and the probabilistic PROTES method, which employs generative sampling. A key innovation is the development of physically constrained encoding schemes that incorporate molecular constraints directly into the discretization process. We demonstrate the efficacy of our method by identifying global minima of Lennard-Jones clusters containing up to 45 atoms. Furthermore, we establish its practical applicability to real-world systems by optimizing 20-atom carbon clusters using a machine-learned moment tensor potential, achieving geometries consistent with quantum-accurate simulations. This work establishes TT decomposition as a powerful tool for molecular structure prediction and provides a general framework adaptable to a wide range of high-dimensional optimization problems in computational material science.

Keywords: global optimization, Tensor Train decomposition, magnetic machine-learning interatomic potentials