An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families
Abstract
An automated computational thermochemistry protocol based on explicitly correlated coupled-cluster theory was determined to produce highly accurate enthalpies of formation and atomization energies for small- to medium-sized molecular species (3–12 atoms). Each possible source of error was carefully examined, and the sizes of contributions to the total atomization enthalpies were used to generate uncertainty estimates. The protocol was first used to generate total atomization enthalpies for a family of four molecular species exhibiting a variety of charges, multiplicities, and electronic ground states. The new protocol was demonstrated to be in good agreement with the Active Thermochemical Tables database for the four species: the methyl peroxy radical, methoxyoxoniumylidene (methyl peroxy cation), methyl peroxy anion, and methyl hydroperoxide. Updating the Active Thermochemical Tables to include those results yielded significantly improved accuracy for the formation enthalpies of those species. The derived protocol was then used to predict formation enthalpies for the larger ethyl peroxy family of species.
- Authors:
-
- Missouri Univ. of Science and Technology, Rolla, MO (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1559535
- Grant/Contract Number:
- AC02-06CH11357; SC0019740
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
- Additional Journal Information:
- Journal Volume: 123; Journal Issue: 26; Journal ID: ISSN 1089-5639
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Active Thermochemical Tables; thermochemistry
Citation Formats
Welch, Bradley K., Dawes, Richard, Bross, David H., and Ruscic, Branko. An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families. United States: N. p., 2019.
Web. doi:10.1021/acs.jpca.9b04381.
Welch, Bradley K., Dawes, Richard, Bross, David H., & Ruscic, Branko. An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families. United States. https://doi.org/10.1021/acs.jpca.9b04381
Welch, Bradley K., Dawes, Richard, Bross, David H., and Ruscic, Branko. Tue .
"An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families". United States. https://doi.org/10.1021/acs.jpca.9b04381. https://www.osti.gov/servlets/purl/1559535.
@article{osti_1559535,
title = {An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families},
author = {Welch, Bradley K. and Dawes, Richard and Bross, David H. and Ruscic, Branko},
abstractNote = {An automated computational thermochemistry protocol based on explicitly correlated coupled-cluster theory was determined to produce highly accurate enthalpies of formation and atomization energies for small- to medium-sized molecular species (3–12 atoms). Each possible source of error was carefully examined, and the sizes of contributions to the total atomization enthalpies were used to generate uncertainty estimates. The protocol was first used to generate total atomization enthalpies for a family of four molecular species exhibiting a variety of charges, multiplicities, and electronic ground states. The new protocol was demonstrated to be in good agreement with the Active Thermochemical Tables database for the four species: the methyl peroxy radical, methoxyoxoniumylidene (methyl peroxy cation), methyl peroxy anion, and methyl hydroperoxide. Updating the Active Thermochemical Tables to include those results yielded significantly improved accuracy for the formation enthalpies of those species. The derived protocol was then used to predict formation enthalpies for the larger ethyl peroxy family of species.},
doi = {10.1021/acs.jpca.9b04381},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 26,
volume = 123,
place = {United States},
year = {Tue Jun 04 00:00:00 EDT 2019},
month = {Tue Jun 04 00:00:00 EDT 2019}
}
Web of Science
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An ab initio based full-dimensional potential energy surface for OH + O 2 ⇄ HO 3 and low-lying vibrational levels of HO 3
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