A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter
The calculation of intermolecular interactions in molecular crystals using model energies provides a unified route to understanding the complex interplay of driving forces in crystallization, elastic properties and more. Presented here is a new single-parameter interaction energy model (CE-1p), exte...
| Main Authors: | , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Subjects: | |
| Online Access: | http://purl.org/au-research/grants/arc/FL180100087 http://hdl.handle.net/20.500.11937/94788 |
| _version_ | 1848765923939319808 |
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| author | Spackman, Peter Spackman, M.A. Gale, Julian |
| author_facet | Spackman, Peter Spackman, M.A. Gale, Julian |
| author_sort | Spackman, Peter |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | The calculation of intermolecular interactions in molecular crystals using model energies provides a unified route to understanding the complex interplay of driving forces in crystallization, elastic properties and more. Presented here is a new single-parameter interaction energy model (CE-1p), extending the previous CrystalExplorer energy model and calibrated using density functional theory (DFT) calculations at the !B97M-V/def2-QZVP level over 1157 intermolecular interactions from 147 crystal structures. The new model incorporates an improved treatment of dispersion interactions and polarizabilities using the exchange-hole dipole model (XDM), along with the use of effective core potentials (ECPs), facilitating application to molecules containing elements across the periodic table (from H to Rn). This new model is validated against high-level reference data with outstanding performance, comparable to state-of-the-art DFT methods for molecular crystal lattice energies over the X23 set (mean absolute deviation 3.6 kJ mol–1) and for intermolecular interactions in the S66x8 benchmark set (root mean-square deviation 3.3 kJ mol–1). The performance of this model is further examined compared to the GFN2-xTB tight-binding model, providing recommendations for the evaluation of intermolecular interactions in molecular crystal systems. |
| first_indexed | 2025-11-14T11:42:58Z |
| format | Journal Article |
| id | curtin-20.500.11937-94788 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | eng |
| last_indexed | 2025-11-14T11:42:58Z |
| publishDate | 2023 |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-947882024-05-07T07:23:43Z A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter Spackman, Peter Spackman, M.A. Gale, Julian computational modelling intermolecular interactions lattice energy molecular crystals The calculation of intermolecular interactions in molecular crystals using model energies provides a unified route to understanding the complex interplay of driving forces in crystallization, elastic properties and more. Presented here is a new single-parameter interaction energy model (CE-1p), extending the previous CrystalExplorer energy model and calibrated using density functional theory (DFT) calculations at the !B97M-V/def2-QZVP level over 1157 intermolecular interactions from 147 crystal structures. The new model incorporates an improved treatment of dispersion interactions and polarizabilities using the exchange-hole dipole model (XDM), along with the use of effective core potentials (ECPs), facilitating application to molecules containing elements across the periodic table (from H to Rn). This new model is validated against high-level reference data with outstanding performance, comparable to state-of-the-art DFT methods for molecular crystal lattice energies over the X23 set (mean absolute deviation 3.6 kJ mol–1) and for intermolecular interactions in the S66x8 benchmark set (root mean-square deviation 3.3 kJ mol–1). The performance of this model is further examined compared to the GFN2-xTB tight-binding model, providing recommendations for the evaluation of intermolecular interactions in molecular crystal systems. 2023 Journal Article http://hdl.handle.net/20.500.11937/94788 10.1107/S2052252523008941 eng http://purl.org/au-research/grants/arc/FL180100087 http://creativecommons.org/licenses/by/4.0/ fulltext |
| spellingShingle | computational modelling intermolecular interactions lattice energy molecular crystals Spackman, Peter Spackman, M.A. Gale, Julian A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title | A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title_full | A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title_fullStr | A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title_full_unstemmed | A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title_short | A transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| title_sort | transferable quantum mechanical energy model for intermolecular interactions using a single empirical parameter |
| topic | computational modelling intermolecular interactions lattice energy molecular crystals |
| url | http://purl.org/au-research/grants/arc/FL180100087 http://hdl.handle.net/20.500.11937/94788 |