Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules
Само за регистроване кориснике
2017
Аутори
Gruden-Pavlović, MajaAnđeklović, Ljubica
Jissy, Akkarapattiakal Kuriappan
Stepanović, Stepan
Zlatar, Matija
Cui, Qiang
Elstner, Marcus
Чланак у часопису (Објављена верзија)
Метаподаци
Приказ свих података о документуАпстракт
Density Functional Tight Binding (DFTB) models are two to three orders of magnitude faster than ab initio and Density Functional Theory (DFT) methods and therefore are particularly attractive in applications to large molecules and condensed phase systems. To establish the applicability of DFTB models to general chemical reactions, we conduct benchmark calculations for barrier heights and reaction energetics of organic molecules using existing databases and several new ones compiled in this study. Structures for the transition states and stable species have been fully optimized at the DFTB level, making it possible to characterize the reliability of DFTB models in a more thorough fashion compared to conducting single point energy calculations as done in previous benchmark studies. The encouraging results for the diverse sets of reactions studied here suggest that DFTB models, especially the most recent third-order version (DFTB3/3OB augmented with dispersion correction), in most cases p...rovide satisfactory description of organic chemical reactions with accuracy almost comparable to popular DFT methods with large basis sets, although larger errors are also seen for certain cases. Therefore, DFTB models can be effective for mechanistic analysis (e.g., transition state search) of large (bio)molecules, especially when coupled with single point energy calculations at higher levels of theory.
Кључне речи:
DFTB / transition state optimization / barrier heights / reaction energiesИзвор:
Journal of Computational Chemistry, 2017, 38, 25, 2171-2185Издавач:
- Wiley, Hoboken
Финансирање / пројекти:
- Рационални дизајн и синтеза биолошки активних и координационих једињења и функционалних материјала, релевантних у (био)нанотехнологији (RS-172035)
- National Institutes of Health (NIH) [R01-GM106443]
- German Academic Exchange Service (DAAD)
- Serbian-German bilateral project [451-03-01038/2015-09/7]
Напомена:
- Supplementary material: http://cherry.chem.bg.ac.rs/handle/123456789/3210
DOI: 10.1002/jcc.24866
ISSN: 0192-8651
PubMed: 28736893
WoS: 000407616400005
Scopus: 2-s2.0-85027395007
Колекције
Институција/група
Hemijski fakultet / Faculty of ChemistryTY - JOUR AU - Gruden-Pavlović, Maja AU - Anđeklović, Ljubica AU - Jissy, Akkarapattiakal Kuriappan AU - Stepanović, Stepan AU - Zlatar, Matija AU - Cui, Qiang AU - Elstner, Marcus PY - 2017 UR - https://cherry.chem.bg.ac.rs/handle/123456789/2504 AB - Density Functional Tight Binding (DFTB) models are two to three orders of magnitude faster than ab initio and Density Functional Theory (DFT) methods and therefore are particularly attractive in applications to large molecules and condensed phase systems. To establish the applicability of DFTB models to general chemical reactions, we conduct benchmark calculations for barrier heights and reaction energetics of organic molecules using existing databases and several new ones compiled in this study. Structures for the transition states and stable species have been fully optimized at the DFTB level, making it possible to characterize the reliability of DFTB models in a more thorough fashion compared to conducting single point energy calculations as done in previous benchmark studies. The encouraging results for the diverse sets of reactions studied here suggest that DFTB models, especially the most recent third-order version (DFTB3/3OB augmented with dispersion correction), in most cases provide satisfactory description of organic chemical reactions with accuracy almost comparable to popular DFT methods with large basis sets, although larger errors are also seen for certain cases. Therefore, DFTB models can be effective for mechanistic analysis (e.g., transition state search) of large (bio)molecules, especially when coupled with single point energy calculations at higher levels of theory. PB - Wiley, Hoboken T2 - Journal of Computational Chemistry T1 - Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules VL - 38 IS - 25 SP - 2171 EP - 2185 DO - 10.1002/jcc.24866 ER -
@article{ author = "Gruden-Pavlović, Maja and Anđeklović, Ljubica and Jissy, Akkarapattiakal Kuriappan and Stepanović, Stepan and Zlatar, Matija and Cui, Qiang and Elstner, Marcus", year = "2017", abstract = "Density Functional Tight Binding (DFTB) models are two to three orders of magnitude faster than ab initio and Density Functional Theory (DFT) methods and therefore are particularly attractive in applications to large molecules and condensed phase systems. To establish the applicability of DFTB models to general chemical reactions, we conduct benchmark calculations for barrier heights and reaction energetics of organic molecules using existing databases and several new ones compiled in this study. Structures for the transition states and stable species have been fully optimized at the DFTB level, making it possible to characterize the reliability of DFTB models in a more thorough fashion compared to conducting single point energy calculations as done in previous benchmark studies. The encouraging results for the diverse sets of reactions studied here suggest that DFTB models, especially the most recent third-order version (DFTB3/3OB augmented with dispersion correction), in most cases provide satisfactory description of organic chemical reactions with accuracy almost comparable to popular DFT methods with large basis sets, although larger errors are also seen for certain cases. Therefore, DFTB models can be effective for mechanistic analysis (e.g., transition state search) of large (bio)molecules, especially when coupled with single point energy calculations at higher levels of theory.", publisher = "Wiley, Hoboken", journal = "Journal of Computational Chemistry", title = "Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules", volume = "38", number = "25", pages = "2171-2185", doi = "10.1002/jcc.24866" }
Gruden-Pavlović, M., Anđeklović, L., Jissy, A. K., Stepanović, S., Zlatar, M., Cui, Q.,& Elstner, M.. (2017). Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules. in Journal of Computational Chemistry Wiley, Hoboken., 38(25), 2171-2185. https://doi.org/10.1002/jcc.24866
Gruden-Pavlović M, Anđeklović L, Jissy AK, Stepanović S, Zlatar M, Cui Q, Elstner M. Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules. in Journal of Computational Chemistry. 2017;38(25):2171-2185. doi:10.1002/jcc.24866 .
Gruden-Pavlović, Maja, Anđeklović, Ljubica, Jissy, Akkarapattiakal Kuriappan, Stepanović, Stepan, Zlatar, Matija, Cui, Qiang, Elstner, Marcus, "Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules" in Journal of Computational Chemistry, 38, no. 25 (2017):2171-2185, https://doi.org/10.1002/jcc.24866 . .