Academic Journal
Enhancing the Accuracy of Ab Initio Molecular Dynamics by Fine Tuning of Effective Two-Body Interactions: Acetonitrile as a Test Case
| العنوان: | Enhancing the Accuracy of Ab Initio Molecular Dynamics by Fine Tuning of Effective Two-Body Interactions: Acetonitrile as a Test Case |
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| المؤلفون: | Barbosa, N, Pagliai, M, Sinha, S, Barone, V, Alfè, D, Brancato, G |
| المصدر: | Journal of Physical Chemistry A , 125 (48) pp. 10475-10484. (2021) |
| سنة النشر: | 2021 |
| المجموعة: | University College London: UCL Discovery |
| الوصف: | Grimme’s dispersion-corrected density functional theory (DFT-D) methods have emerged among the most practical approaches to perform accurate quantum mechanical calculations on molecular systems ranging from small clusters to microscopic and mesoscopic samples, i.e., including hundreds or thousands of molecules. Moreover, DFT-D functionals can be easily integrated into popular ab initio molecular dynamics (MD) software packages to carry out first-principles condensed-phase simulations at an affordable computational cost. Here, starting from the well-established D3 version of the dispersion-correction term, we present a simple protocol to improve the accurate description of the intermolecular interactions of molecular clusters of growing size, considering acetonitrile as a test case. Optimization of the interaction energy was performed with reference to diffusion quantum Monte Carlo calculations, successfully reaching the same inherent accuracy of the latter (statistical error of ∼0.1 kcal/mol per molecule). The refined DFT-D3 model was then used to perform ab initio MD simulations of liquid acetonitrile, again showing significant improvements toward available experimental data with respect to the default correction. |
| نوع الوثيقة: | article in journal/newspaper |
| وصف الملف: | text |
| اللغة: | English |
| Relation: | https://discovery.ucl.ac.uk/id/eprint/10140677/1/Manuscript_final.pdf; https://discovery.ucl.ac.uk/id/eprint/10140677/ |
| الاتاحة: | https://discovery.ucl.ac.uk/id/eprint/10140677/1/Manuscript_final.pdf https://discovery.ucl.ac.uk/id/eprint/10140677/ |
| Rights: | open |
| رقم الانضمام: | edsbas.B5A9BD18 |
| قاعدة البيانات: | BASE |
| الوصف غير متاح. |