Collective dynamics and self-motions in the van der Waals liquid tetrahydrofuran from meso- to inter-molecular scales disentangled by neutron spectroscopy with polarization analysis
By using time-of-flight neutron spectroscopy with polarization analysis, we have separated coherent and incoherent contributions to the scattering of deuterated tetrahydrofuran in a wide scattering vector (Q)-range from meso- to inter-molecular length scales. The results are compared with those rece...
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Veröffentlicht in: | The Journal of chemical physics 2023-05, Vol.158 (18) |
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creator | Arbe, Arantxa Nilsen, Gøran J. Devonport, Mark Farago, Bela Alvarez, Fernando Martínez González, José A. Colmenero, Juan |
description | By using time-of-flight neutron spectroscopy with polarization analysis, we have separated coherent and incoherent contributions to the scattering of deuterated tetrahydrofuran in a wide scattering vector (Q)-range from meso- to inter-molecular length scales. The results are compared with those recently reported for water to address the influence of the nature of inter-molecular interactions (van der Waals vs hydrogen bond) on the dynamics. The phenomenology found is qualitatively similar in both systems. Both collective and self-scattering functions are satisfactorily described in terms of a convolution model that considers vibrations, diffusion, and a Q-independent mode. We observe a crossover in the structural relaxation from being dominated by the Q-independent mode at the mesoscale to being dominated by diffusion at inter-molecular length scales. The characteristic time of the Q-independent mode is the same for collective and self-motions and, contrary to water, faster and with a lower activation energy (≈1.4 Kcal/mol) than the structural relaxation time at inter-molecular length scales. This follows the macroscopic viscosity behavior. The collective diffusive time is well described by the de Gennes narrowing relation proposed for simple monoatomic liquids in a wide Q-range entering the intermediate length scales, in contraposition to the case of water. |
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The results are compared with those recently reported for water to address the influence of the nature of inter-molecular interactions (van der Waals vs hydrogen bond) on the dynamics. The phenomenology found is qualitatively similar in both systems. Both collective and self-scattering functions are satisfactorily described in terms of a convolution model that considers vibrations, diffusion, and a Q-independent mode. We observe a crossover in the structural relaxation from being dominated by the Q-independent mode at the mesoscale to being dominated by diffusion at inter-molecular length scales. The characteristic time of the Q-independent mode is the same for collective and self-motions and, contrary to water, faster and with a lower activation energy (≈1.4 Kcal/mol) than the structural relaxation time at inter-molecular length scales. This follows the macroscopic viscosity behavior. The collective diffusive time is well described by the de Gennes narrowing relation proposed for simple monoatomic liquids in a wide Q-range entering the intermediate length scales, in contraposition to the case of water.</description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/5.0147427</identifier><identifier>PMID: 37154281</identifier><identifier>CODEN: JCPSA6</identifier><language>eng</language><publisher>United States: American Institute of Physics</publisher><subject>Coherent scattering ; Deuteration ; Diffusion ; Hydrogen bonds ; Molecular interactions ; Phenomenology ; Physics ; Polarization ; Relaxation time ; Scattering functions ; Spectroscopic analysis ; Spectrum analysis ; Tetrahydrofuran</subject><ispartof>The Journal of chemical physics, 2023-05, Vol.158 (18)</ispartof><rights>Author(s)</rights><rights>2023 Author(s). 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The results are compared with those recently reported for water to address the influence of the nature of inter-molecular interactions (van der Waals vs hydrogen bond) on the dynamics. The phenomenology found is qualitatively similar in both systems. Both collective and self-scattering functions are satisfactorily described in terms of a convolution model that considers vibrations, diffusion, and a Q-independent mode. We observe a crossover in the structural relaxation from being dominated by the Q-independent mode at the mesoscale to being dominated by diffusion at inter-molecular length scales. The characteristic time of the Q-independent mode is the same for collective and self-motions and, contrary to water, faster and with a lower activation energy (≈1.4 Kcal/mol) than the structural relaxation time at inter-molecular length scales. This follows the macroscopic viscosity behavior. 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The results are compared with those recently reported for water to address the influence of the nature of inter-molecular interactions (van der Waals vs hydrogen bond) on the dynamics. The phenomenology found is qualitatively similar in both systems. Both collective and self-scattering functions are satisfactorily described in terms of a convolution model that considers vibrations, diffusion, and a Q-independent mode. We observe a crossover in the structural relaxation from being dominated by the Q-independent mode at the mesoscale to being dominated by diffusion at inter-molecular length scales. The characteristic time of the Q-independent mode is the same for collective and self-motions and, contrary to water, faster and with a lower activation energy (≈1.4 Kcal/mol) than the structural relaxation time at inter-molecular length scales. This follows the macroscopic viscosity behavior. The collective diffusive time is well described by the de Gennes narrowing relation proposed for simple monoatomic liquids in a wide Q-range entering the intermediate length scales, in contraposition to the case of water.</abstract><cop>United States</cop><pub>American Institute of Physics</pub><pmid>37154281</pmid><doi>10.1063/5.0147427</doi><tpages>16</tpages><orcidid>https://orcid.org/0000-0002-4651-0044</orcidid><orcidid>https://orcid.org/0000-0002-2440-4953</orcidid><orcidid>https://orcid.org/0000-0002-0148-0486</orcidid><orcidid>https://orcid.org/0000-0002-5137-4649</orcidid><orcidid>https://orcid.org/0000-0002-7038-0315</orcidid><orcidid>https://orcid.org/0000-0001-5262-6732</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Coherent scattering Deuteration Diffusion Hydrogen bonds Molecular interactions Phenomenology Physics Polarization Relaxation time Scattering functions Spectroscopic analysis Spectrum analysis Tetrahydrofuran |
title | Collective dynamics and self-motions in the van der Waals liquid tetrahydrofuran from meso- to inter-molecular scales disentangled by neutron spectroscopy with polarization analysis |
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