Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule
We calculate harmonic frequencies of the three most abundant carbonic acid conformers. For this, different model chemistries are investigated with respect to their benefits and shortcomings. Based on these results we use perturbation theory to calculate anharmonic corrections at the ωB97XD/aug-cc-pV...
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ftdoajarticles:oai:doaj.org/article:1d317377fc5143e6a28c6e5945b1a815 2023-05-15T15:51:57+02:00 Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule Stefan E. Huber Silvia Dalnodar Wolfgang Kausch Stefan Kimeswenger Michael Probst 2012-09-01T00:00:00Z https://doi.org/10.1063/1.4755786 https://doaj.org/article/1d317377fc5143e6a28c6e5945b1a815 EN eng AIP Publishing LLC http://dx.doi.org/10.1063/1.4755786 https://doaj.org/toc/2158-3226 2158-3226 doi:10.1063/1.4755786 https://doaj.org/article/1d317377fc5143e6a28c6e5945b1a815 AIP Advances, Vol 2, Iss 3, Pp 032180-032180-15 (2012) Physics QC1-999 article 2012 ftdoajarticles https://doi.org/10.1063/1.4755786 2022-12-31T00:43:49Z We calculate harmonic frequencies of the three most abundant carbonic acid conformers. For this, different model chemistries are investigated with respect to their benefits and shortcomings. Based on these results we use perturbation theory to calculate anharmonic corrections at the ωB97XD/aug-cc-pVXZ, X = D, T, Q, level of theory and compare them with recent experimental data and theoretical predictions. A discrete variable representation method is used to predict the large anharmonic contributions to the frequencies of the stretching vibrations in the hydrogen bonds in the carbonic acid dimer. Moreover, we re-investigate the energetics of the formation of the carbonic acid dimer from its constituents water and carbon dioxide using a high-level extrapolation method. We find that the ωB97XD functional performs well in estimating the fundamental frequencies of the carbonic acid conformers. Concerning the reaction energetics, the accuracy of ωB97XD is even comparable to the high-level extrapolation method. We discuss possibilities to detect carbonic acid in various natural environments such as Earth's and Martian atmospheres. Article in Journal/Newspaper Carbonic acid Directory of Open Access Journals: DOAJ Articles AIP Advances 2 3 032180 |
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Open Polar |
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Directory of Open Access Journals: DOAJ Articles |
op_collection_id |
ftdoajarticles |
language |
English |
topic |
Physics QC1-999 |
spellingShingle |
Physics QC1-999 Stefan E. Huber Silvia Dalnodar Wolfgang Kausch Stefan Kimeswenger Michael Probst Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
topic_facet |
Physics QC1-999 |
description |
We calculate harmonic frequencies of the three most abundant carbonic acid conformers. For this, different model chemistries are investigated with respect to their benefits and shortcomings. Based on these results we use perturbation theory to calculate anharmonic corrections at the ωB97XD/aug-cc-pVXZ, X = D, T, Q, level of theory and compare them with recent experimental data and theoretical predictions. A discrete variable representation method is used to predict the large anharmonic contributions to the frequencies of the stretching vibrations in the hydrogen bonds in the carbonic acid dimer. Moreover, we re-investigate the energetics of the formation of the carbonic acid dimer from its constituents water and carbon dioxide using a high-level extrapolation method. We find that the ωB97XD functional performs well in estimating the fundamental frequencies of the carbonic acid conformers. Concerning the reaction energetics, the accuracy of ωB97XD is even comparable to the high-level extrapolation method. We discuss possibilities to detect carbonic acid in various natural environments such as Earth's and Martian atmospheres. |
format |
Article in Journal/Newspaper |
author |
Stefan E. Huber Silvia Dalnodar Wolfgang Kausch Stefan Kimeswenger Michael Probst |
author_facet |
Stefan E. Huber Silvia Dalnodar Wolfgang Kausch Stefan Kimeswenger Michael Probst |
author_sort |
Stefan E. Huber |
title |
Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
title_short |
Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
title_full |
Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
title_fullStr |
Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
title_full_unstemmed |
Carbonic acid revisited: Vibrational spectra, energetics and the possibility of detecting an elusive molecule |
title_sort |
carbonic acid revisited: vibrational spectra, energetics and the possibility of detecting an elusive molecule |
publisher |
AIP Publishing LLC |
publishDate |
2012 |
url |
https://doi.org/10.1063/1.4755786 https://doaj.org/article/1d317377fc5143e6a28c6e5945b1a815 |
genre |
Carbonic acid |
genre_facet |
Carbonic acid |
op_source |
AIP Advances, Vol 2, Iss 3, Pp 032180-032180-15 (2012) |
op_relation |
http://dx.doi.org/10.1063/1.4755786 https://doaj.org/toc/2158-3226 2158-3226 doi:10.1063/1.4755786 https://doaj.org/article/1d317377fc5143e6a28c6e5945b1a815 |
op_doi |
https://doi.org/10.1063/1.4755786 |
container_title |
AIP Advances |
container_volume |
2 |
container_issue |
3 |
container_start_page |
032180 |
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1766387310524366848 |