Evidence of Nonrigidity Effects in the Description of Low-Energy Anisotropic Molecular Collisions of Hydrogen Molecules with Excited Metastable Helium Atoms
Cold collisions serve as a sensitive probe of the interaction potential. In the recent study of Klein et al. (Nature Phys. 2017, 13, 35-38), the one-parameter scaling of the interaction potential was necessary to obtain agreement between theoretical and observed patterns of the orbiting resonances for excited metastable helium atoms colliding with hydrogen molecules. Here, we show that the effect of nonrigidity of the H2 molecule on the resonant structure, absent in the previous study, is critical to predict the correct positions of the resonances in that case. We have complemented the theoretical description of the interaction potential and revised reaction rate coefficients by proper inclusion of the flexibility of the molecule. The calculated reaction rate coefficients are in remarkable agreement with the experimental data without empirical adjustment of the interaction potential. We have shown that even state-of-the-art calculations of the interaction energy cannot ensure agreement with the experiment if such an important physical effect as flexibility of the interacting molecule is neglected. Our findings about the significance of the nonrigidity effects can be especially crucial in cold chemistry, where the quantum nature of molecules is pronounced.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2020 |
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| Erschienen: |
2020 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:16 |
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| Enthalten in: |
Journal of chemical theory and computation - 16(2020), 4 vom: 14. Apr., Seite 2450-2459 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Pawlak, Mariusz [VerfasserIn] |
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| Links: |
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| Anmerkungen: |
Date Revised 01.10.2020 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/acs.jctc.0c00183 |
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| Förderinstitution / Projekttitel: |
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NLM307387372 |
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| 245 | 1 | 0 | |a Evidence of Nonrigidity Effects in the Description of Low-Energy Anisotropic Molecular Collisions of Hydrogen Molecules with Excited Metastable Helium Atoms |
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| 500 | |a Date Revised 01.10.2020 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Cold collisions serve as a sensitive probe of the interaction potential. In the recent study of Klein et al. (Nature Phys. 2017, 13, 35-38), the one-parameter scaling of the interaction potential was necessary to obtain agreement between theoretical and observed patterns of the orbiting resonances for excited metastable helium atoms colliding with hydrogen molecules. Here, we show that the effect of nonrigidity of the H2 molecule on the resonant structure, absent in the previous study, is critical to predict the correct positions of the resonances in that case. We have complemented the theoretical description of the interaction potential and revised reaction rate coefficients by proper inclusion of the flexibility of the molecule. The calculated reaction rate coefficients are in remarkable agreement with the experimental data without empirical adjustment of the interaction potential. We have shown that even state-of-the-art calculations of the interaction energy cannot ensure agreement with the experiment if such an important physical effect as flexibility of the interacting molecule is neglected. Our findings about the significance of the nonrigidity effects can be especially crucial in cold chemistry, where the quantum nature of molecules is pronounced | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Żuchowski, Piotr S |e verfasserin |4 aut | |
| 700 | 1 | |a Moiseyev, Nimrod |e verfasserin |4 aut | |
| 700 | 1 | |a Jankowski, Piotr |e verfasserin |4 aut | |
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