Experimental Confirmation of the Universal Law for the Vibrational Density of States of Liquids
An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due to the difficulty in dealing with the imaginary modes dominant in the low-energy region, as described by the instantaneous normal mode (INM) approach. Nevertheless, Zaccone and...
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Abstract | An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due to the difficulty in dealing with the imaginary modes dominant in the low-energy region, as described by the instantaneous normal mode (INM) approach. Nevertheless, Zaccone and Baggioli have recently developed such a model based on overdamped Langevin liquid dynamics. The model was proposed to be the universal law for the vibrational density of states of liquids. Distinct from the Debye law, g({\omega}) ~ {\omega}2, for solids, the universal law for liquids reveals a linear relationship, g({\omega}) ~ {\omega}, in the low-energy region. The universal law has been successfully verified with computer simulated VDOS for Lennard-Jones liquids. We further confirm this universal law with experimental VDOS measured by inelastic neutron scattering on real liquid systems including water, liquid metal, and polymer liquids. We have applied this model and extracted the effective relaxation rate for the short time dynamics for each liquid. The model has been further evaluated in the predication of the specific heat. The results have been compared with the existing experimental data as well as with values obtained by different approaches. |
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AbstractList | An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due to the difficulty in dealing with the imaginary modes dominant in the low-energy region, as described by the instantaneous normal mode (INM) approach. Nevertheless, Zaccone and Baggioli have recently developed such a model based on overdamped Langevin liquid dynamics. The model was proposed to be the universal law for the vibrational density of states of liquids. Distinct from the Debye law, g({\omega}) ~ {\omega}2, for solids, the universal law for liquids reveals a linear relationship, g({\omega}) ~ {\omega}, in the low-energy region. The universal law has been successfully verified with computer simulated VDOS for Lennard-Jones liquids. We further confirm this universal law with experimental VDOS measured by inelastic neutron scattering on real liquid systems including water, liquid metal, and polymer liquids. We have applied this model and extracted the effective relaxation rate for the short time dynamics for each liquid. The model has been further evaluated in the predication of the specific heat. The results have been compared with the existing experimental data as well as with values obtained by different approaches. J. Phys. Chem. Lett. 2022, 13, 3105 An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due to the difficulty in dealing with the imaginary modes dominant in the low-energy region, as described by the instantaneous normal mode (INM) approach. Nevertheless, Zaccone and Baggioli have recently developed such a model based on overdamped Langevin liquid dynamics. The model was proposed to be the universal law for the vibrational density of states of liquids. Distinct from the Debye law, g({\omega}) ~ {\omega}2, for solids, the universal law for liquids reveals a linear relationship, g({\omega}) ~ {\omega}, in the low-energy region. The universal law has been successfully verified with computer simulated VDOS for Lennard-Jones liquids. We further confirm this universal law with experimental VDOS measured by inelastic neutron scattering on real liquid systems including water, liquid metal, and polymer liquids. We have applied this model and extracted the effective relaxation rate for the short time dynamics for each liquid. The model has been further evaluated in the predication of the specific heat. The results have been compared with the existing experimental data as well as with values obtained by different approaches. |
Author | Zengji Yue Yu, Dehong Wang, Xiaolin Stamper, Caleb Cortie, David |
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BackLink | https://doi.org/10.48550/arXiv.2201.11914$$DView paper in arXiv https://doi.org/10.1021/acs.jpclett.2c00297$$DView published paper (Access to full text may be restricted) |
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Snippet | An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due to the difficulty in dealing with... J. Phys. Chem. Lett. 2022, 13, 3105 An analytical model describing the vibrational phonon density of states (VDOS) of liquids has long been elusive, mainly due... |
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SubjectTerms | Density of states Inelastic scattering Liquid metals Liquids Mathematical models Neutron scattering Physics - Other Condensed Matter Physics - Soft Condensed Matter |
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Title | Experimental Confirmation of the Universal Law for the Vibrational Density of States of Liquids |
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