Automated identification of isofragmented reactions and application in correcting molecular property models

O'Donnell, Aidan; Li, Bowen; Rangarajan, Srinivas; Gounaris, Chrysanthos E.

doi:10.1016/j.ces.2023.119411

Cited by 1 publication

(2 citation statements)

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“…This advancement enables the development and integration of high-throughput IDR calculations into open-source statistical mechanics and thermochemistry software. 34,37,39,43 One problem we have often encountered in practice is that the choice of reference species (a.k.a. the training set) used in the above-mentioned thermo-correction approaches can vary from study to study.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The recent work of Buerger et al , has shown that these reactions can be systematically and automatically identified, rather than relying on the traditional approach of manual design. This advancement enables the development and integration of high-throughput IDR calculations into open-source statistical mechanics and thermochemistry software. ,,, …”

Section: Introductionmentioning

confidence: 99%

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Toward Accurate Quantum Mechanical Thermochemistry: (1) Extensible Implementation and Comparison of Bond Additivity Corrections and Isodesmic Reactions

Wu,

Payne,

Pang

et al. 2024

J. Phys. Chem. A

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Obtaining accurate enthalpies of formation of chemical species, ΔH f , often requires empirical corrections that connect the results of quantum mechanical (QM) calculations with the experimental enthalpies of elements in their standard state. One approach is to use atomization energy corrections followed by bond additivity corrections (BACs), such as those defined by Petersson et al. or Anantharaman and Melius. Another approach is to utilize isodesmic reactions (IDRs) as shown by Buerger et al. We implement both approaches in Arkane, an open-source software that can calculate species thermochemistry using results from various QM software packages. In this work, we collect 421 reference species from the literature to derive ΔH f corrections and fit atomization energy corrections and BACs for 15 commonly used model chemistries. We find that both types of BACs yield similar accuracy, although Anantharaman-and Melius-type BACs appear to generalize better. Furthermore, BACs tend to achieve better accuracy than IDRs for commonly used model chemistries, and IDRs can be less robust because of the sensitivity to the chosen reference species and reactions. Overall, Anantharaman-and Melius-type BACs are our recommended approach for achieving accurate QM corrections for enthalpies.

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Section: ■ Introductionmentioning

confidence: 99%