AMELI: Angular Matrix Elements of Lanthanide Ions

TL;DR

The paper introduces AMELI, a Python package for direct, precise calculation of angular matrix elements of lanthanide ions, facilitating spectral analysis in various host materials with a comprehensive, universally applicable approach.

Contribution

It presents a novel, direct computational method for angular matrix elements using a Slater determinant basis, implemented in an open-access Python package, improving accuracy and usability over traditional indirect methods.

Findings

Provides exact matrix elements for all lanthanide ions

Enables universal application across different configurations

Reduces computational barriers for experimental analysis

Abstract

Matrix elements of spherical tensor operators are fundamental to the analysis of lanthanide spectra in both amorphous and crystalline host materials. In the intermediate coupling scheme, the eigenvectors of the Hamiltonian define the electronic structure, while the eigenvalues determine the energy levels of the $f^N$ configuration. By utilizing these eigenvectors to evaluate electric and magnetic dipole operators, one can identify the radiative line strengths for all transitions in both absorption and emission. This work presents a comprehensive framework for the direct calculation of angular matrix elements using a Slater determinant basis and their subsequent transformation to the traditional $LS$-coupling scheme. Unlike conventional indirect methods, this approach is more universally applicable, though it is computationally more intensive. A concise set of general rules is prepared to enable the calculation of angular matrix elements for virtually any spherical tensor operator within an $f^N$ configuration. The computational overhead of this direct approach is well within the capabilities of modern desktop computing. Furthermore, since these configuration-specific angular matrices are mathematical constants independent of the host environment, they need only be calculated once. The Python package AMELI is introduced, which employs exact arithmetic to generate the matrix elements with absolute mathematical precision. Both the underlying algorithms and the calculated matrices for all lanthanide ions are provided in open-access repositories. This removes a significant barrier for experimentalists, providing the necessary operator matrices without requiring them to navigate the intricate theory and algorithmic implementation.