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Disentangling α and β relaxation in orientationally disordered crystals with theory and experiments.

Accepted version
Peer-reviewed

Type

Article

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Authors

Gebbia, Jonathan F 
Tamarit, Josep-Lluis 
Zaccone, Alessio 

Abstract

We use a microscopically motivated generalized Langevin equation (GLE) approach to link the vibrational density of states (VDOS) to the dielectric response of orientational glasses (OGs). The dielectric function calculated based on the GLE is compared with experimental data for the paradigmatic case of two OGs: freon-112 and freon-113, around and just above T_{g}. The memory function is related to the integral of the VDOS times a spectral coupling function γ(ω_{p}), which tells the degree of dynamical coupling between molecular degrees of freedom at different eigenfrequencies. The comparative analysis of the two freons reveals that the appearance of a secondary β relaxation in freon-112 is due to cooperative dynamical coupling in the regime of mesoscopic motions caused by stronger anharmonicity (absent in freon-113) and is associated with the comparatively lower boson peak in the VDOS. The proposed framework brings together all the key aspects of glassy physics (VDOS with the boson peak, dynamical heterogeneity, dissipation, and anharmonicity) into a single model.

Description

Keywords

cond-mat.soft, cond-mat.soft, cond-mat.dis-nn, cond-mat.mtrl-sci

Journal Title

Phys Rev E

Conference Name

Journal ISSN

2470-0045
2470-0053

Volume Title

97

Publisher

American Physical Society (APS)