Permutation-adapted complete and independent basis for atomic cluster expansion descriptors

Technical Report · 01 August 2022

DOI:https://doi.org/10.2172/1879613· OSTI ID:1879613

Goff, James M. ^[1]; Sievers, Charles ^[2]; Wood, Mitchell A. ^[1]; Thompson, Aidan P. ^[1]

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1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Boeing Research and Technology (BR&T), Seattle, WA (United States)

In many recent applications, particularly in the field of atom-centered descriptors for interatomic potentials, tensor products of spherical harmonics have been used to characterize complex atomic environments. When coupled with a radial basis, the atomic cluster expansion (ACE) basis is obtained. However, symmetrization with respect to both rotation and permutation results in an overcomplete set of ACE descriptors with linear dependencies occurring within blocks of functions corresponding to particular generalized Wigner symbols. All practical applications of ACE employ semi-numerical constructions to generate a complete, fully independent basis. While computationally tractable, the resultant basis cannot be expressed analytically, is susceptible to numerical instability, and thus has limited reproducibility. Here we present a procedure for generating explicit analytic expressions for a complete and independent set of ACE descriptors. The procedure uses a coupling scheme that is maximally symmetric w.r.t. permutation of the atoms, exposing the permutational symmetries of the generalized Wigner symbols, and yields a permutation-adapted rotationally and permutationally invariant basis (PA-RPI ACE). Theoretical support for the approach is presented, as well as numerical evidence of completeness and independence. A summary of explicit enumeration of PA-RPI functions up to rank 6 and polynomial degree 32 is provided. The PA-RPI blocks corresponding to particular generalized Wigner symbols may be either larger or smaller than the corresponding blocks in the simpler rotationally invariant basis. Finally, we demonstrate that basis functions of high polynomial degree persist under strong regularization, indicating the importance of not restricting the maximum degree of basis functions in ACE models a priori.

• Research Organization: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Fusion Energy Sciences (FES); USDOE National Nuclear Security Administration (NNSA)
• DOE Contract Number: NA0003525
• OSTI ID: 1879613
• Report Number(s): SAND2022-10403R; 708773
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS