Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations
Abstract
We recently proposed Domain Separated Density Functional Theory (DS-DFT), a framework that allows for the combination of different levels of theory for the computation of the electronic structure of molecules. Here, this work discusses the application of DS-DFT to the computation of transition-state energy barriers and optical absorption spectra. We considered several hydrogen abstraction reactions and optical spectra of molecule/metal cluster systems, including the absorption of individual species such as carbon monoxide, methane, and molecular hydrogen to a Li6 cluster. We present and discuss two domain-separated methods: i), the screened-density approximation (SDA), and, ii), linearly weighted exchange (LWE). We find that SDA, which is applied as a hybridization based on atomic domains, could be useful to computing energy barriers, whereas LWE is suited for the analysis of electronic properties such as ground-state gaps, excitation energies, and oscillator strengths.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Princeton Univ., NJ (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1798256
- Grant/Contract Number:
- SC0004752; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 28; Journal ID: ISSN 1089-5639
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical reactions; Embedding; Energy; Chemical calculations; Approximation
Citation Formats
Mosquera, Martín A., Jones, Leighton O., Borca, Carlos H., Ratner, Mark A., and Schatz, George C. Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations. United States: N. p., 2020.
Web. doi:10.1021/acs.jpca.0c03596.
Mosquera, Martín A., Jones, Leighton O., Borca, Carlos H., Ratner, Mark A., & Schatz, George C. Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations. United States. https://doi.org/10.1021/acs.jpca.0c03596
Mosquera, Martín A., Jones, Leighton O., Borca, Carlos H., Ratner, Mark A., and Schatz, George C. Tue .
"Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations". United States. https://doi.org/10.1021/acs.jpca.0c03596. https://www.osti.gov/servlets/purl/1798256.
@article{osti_1798256,
title = {Domain Separated Density Functional Theory for Reaction Energy Barriers and Optical Excitations},
author = {Mosquera, Martín A. and Jones, Leighton O. and Borca, Carlos H. and Ratner, Mark A. and Schatz, George C.},
abstractNote = {We recently proposed Domain Separated Density Functional Theory (DS-DFT), a framework that allows for the combination of different levels of theory for the computation of the electronic structure of molecules. Here, this work discusses the application of DS-DFT to the computation of transition-state energy barriers and optical absorption spectra. We considered several hydrogen abstraction reactions and optical spectra of molecule/metal cluster systems, including the absorption of individual species such as carbon monoxide, methane, and molecular hydrogen to a Li6 cluster. We present and discuss two domain-separated methods: i), the screened-density approximation (SDA), and, ii), linearly weighted exchange (LWE). We find that SDA, which is applied as a hybridization based on atomic domains, could be useful to computing energy barriers, whereas LWE is suited for the analysis of electronic properties such as ground-state gaps, excitation energies, and oscillator strengths.},
doi = {10.1021/acs.jpca.0c03596},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 28,
volume = 124,
place = {United States},
year = {Tue Jun 16 00:00:00 EDT 2020},
month = {Tue Jun 16 00:00:00 EDT 2020}
}
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