The Scaled Hirshfeld Partitioning: Mathematical Development and Information-Theoretic Foundation

尺度化赫什菲尔德划分:数学发展与信息论基础

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Abstract

Atomic charges play a central role in the analysis of molecular electronic structure and are widely used in the development of computational models. We introduce a simple and computationally efficient extension of Hirshfeld's 1977 stockholder partitioning method, called scaled Hirshfeld, in which neutral proatom densities are scaled to construct a promolecular density better adapted to the molecular electron density. We present a fixed-point iterative algorithm to compute the proatom scaling coefficients and show that this formulation is equivalent to the information-theoretic additive variational Hirshfeld method with a minimal basis. This equivalence establishes a rigorous mathematical foundation for the scaled Hirshfeld method and ensures size consistency as well as the existence of a unique solution. Numerical results demonstrate that the proposed approach yields charges larger than those obtained with the original Hirshfeld method, while retaining computational efficiency and providing an improved description of molecular dipole moments and electrostatic potentials.

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