How accurate are simulations and experiments for the lattice energies of molecular crystals?
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arXiv
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| Autori principali: | , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| _version_ | 1866913638421364736 |
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| author | Della Pia, Flaviano Zen, Andrea Alfè, Dario Michaelides, Angelos |
| author_facet | Della Pia, Flaviano Zen, Andrea Alfè, Dario Michaelides, Angelos |
| contents | Molecular crystals play a central role in a wide range of scientific fields, including pharmaceuticals and organic semiconductor devices. However, they are challenging systems to model accurately with computational approaches because of a delicate interplay of intermolecular interactions such as hydrogen bonding and van der Waals dispersion forces. Here, by exploiting recent algorithmic developments, we report the first set of diffusion Monte Carlo lattice energies for all 23 molecular crystals in the popular and widely used X23 dataset. Comparisons with previous state-of-the-art lattice energy predictions (on a subset of the dataset) and a careful analysis of experimental sublimation enthalpies reveals that high-accuracy computational methods are now at least as reliable as (computationally derived) experiments for the lattice energies of molecular crystals. Overall, this work demonstrates the feasibility of high-level explicitly correlated electronic structure methods for broad benchmarking studies in complex condensed phase systems, and signposts a route towards closer agreement between experiment and simulation. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2402_13059 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | How accurate are simulations and experiments for the lattice energies of molecular crystals? Della Pia, Flaviano Zen, Andrea Alfè, Dario Michaelides, Angelos Materials Science Chemical Physics Molecular crystals play a central role in a wide range of scientific fields, including pharmaceuticals and organic semiconductor devices. However, they are challenging systems to model accurately with computational approaches because of a delicate interplay of intermolecular interactions such as hydrogen bonding and van der Waals dispersion forces. Here, by exploiting recent algorithmic developments, we report the first set of diffusion Monte Carlo lattice energies for all 23 molecular crystals in the popular and widely used X23 dataset. Comparisons with previous state-of-the-art lattice energy predictions (on a subset of the dataset) and a careful analysis of experimental sublimation enthalpies reveals that high-accuracy computational methods are now at least as reliable as (computationally derived) experiments for the lattice energies of molecular crystals. Overall, this work demonstrates the feasibility of high-level explicitly correlated electronic structure methods for broad benchmarking studies in complex condensed phase systems, and signposts a route towards closer agreement between experiment and simulation. |
| title | How accurate are simulations and experiments for the lattice energies of molecular crystals? |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2402.13059 |