CrystaLattE

CrystaLattE automates computation of lattice energies in molecular crystals using a many-body cluster expansion that evaluates interactions among dimers, trimers, and higher-order clusters.

Key Features:

• Many-Body Cluster Expansion: CrystaLattE employs a many-body cluster expansion to systematically account for interactions among dimers, trimers, and higher-order N-mers in molecular crystals.
• Parallel Computation: Independent computations on different N-mers enable inherent parallelism for scalable evaluation of cluster contributions.
• Redundancy Avoidance: Identical N-mers are detected and redundant calculations avoided using Coulomb-matrix descriptors that exploit three-dimensional periodic symmetry.
• Quantum Chemistry Integration: The software interfaces with the quantum chemistry package Psi4 via the Quantum Chemistry Common Driver and Databases library for electronic structure computations.
• Dispersion-Corrected HF-3c and Three-Body Dispersion: Lattice energies are computed with the dispersion-corrected HF-3c method and supplemented by an Axilrod-Teller-Muto estimate of three-body dispersion interactions.
• Accuracy and Convergence: In a benchmark on crystalline benzene including all symmetry-unique dimers and trimers within a 15 Å cutoff, CrystaLattE produced an error of -1.0 kJ mol^-1 relative to the estimated experimental lattice energy.

Scientific Applications:

• Lattice Energy Prediction: Predict lattice energies of molecular crystals for studies in computational chemistry and materials science.
• Crystal Stability and Phase Behavior: Analyze crystal stability, phase behavior, and material properties using computed lattice energies.
• Many-Body Interaction Analysis: Investigate many-body interactions in crystalline systems by including dimers, trimers, and higher-order clusters.

Methodology:

CrystaLattE uses a many-body cluster expansion with independent computations on dimers, trimers, and higher-order clusters, detects identical N-mers via Coulomb-matrix descriptors, interfaces with Psi4 through the Quantum Chemistry Common Driver and Databases library, employs the dispersion-corrected HF-3c method with an Axilrod-Teller-Muto three-body dispersion estimate, and in a demonstrated case included all symmetry-unique dimers and trimers within a 15 Å cutoff; inputs include a crystallographic information file (CIF) and an execution-parameter input file.