Accurate and Efficient Phonon Calculations in Molecular Crystals via Minimal Molecular Displacements.

ABSTRACT: Vibrational dynamics governs the fundamental properties of molecular crystals, shaping their thermodynamics, mechanics, spectroscopy, and transport phenomena. However desirable, the accurate first-principles calculation of solid-state vibrations (i.e. phonons) stands as a major computational challenge in molecular crystals characterized by many atoms in the unit cell and by weak intermolecular interactions. Here, we propose a formulation of harmonic lattice dynamics based on a natural basis of molecular coordinates consisting of rigid-body displacements and intramolecular vibrations. This enables a sensible minimal molecular displacement approximation for the calculation of the dynamical matrix, combining isolated molecule calculations with only a small number of expensive crystal supercel

SUBMITTER: Soprani L 

PROVIDER: S-EPMC12392453 | biostudies-literature | 2025 Aug

REPOSITORIES: biostudies-literature