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• W2783241771 abstract "The structure and vibrational density of states (VDOS) of polymer glasses are investigated using numerical simulations based on the classical Kremer-Grest bead-spring model. We focus on the roles of chain length and bending stiffness, the latter being set by imposing three-body angular potentials along chain backbones. Upon increasing the chain length and bending stiffness, structural reorganisation leads to volumetric expansion of the material and build-up of internal stresses. The VDOS has two dominant bands: a low frequency one corresponding to inter- and intra-chain non-bonding interactions and a high frequency one corresponding principally to vibrations of bonded beads that constitute skeletal chain backbones. Upon increasing the steepness of the angular potential, vibrational modes associated with chain bending gradually move from the low-frequency to the high-frequency band. This redistribution of modes is reflected in a reduction of the so-called Boson peak upon increasing chain stiffness. Remarkably, the finer structure and the peaks of the high-frequency band, and their variations with stiffness, can, for short chains, be explained using an analytical solution derived for a model triatomic molecule. For longer chains, the qualitative evolution of the VDOS with chain stiffness is similar, although the distinct peaks observed for short chains become increasingly smoothed-out. Our findings can be used to guide a systematic approach to interpretation of Brillouin and Raman scattering spectra of glassy polymers in future work, with applications in polymer processing diagnostics." @default.
• W2783241771 created "2018-01-26" @default.
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• W2783241771 date "2018-02-13" @default.
• W2783241771 modified "2023-09-27" @default.
• W2783241771 title "Interpretation of the Vibrational Spectra of Glassy Polymers Using Coarse-Grained Simulations" @default.
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• W2783241771 doi "https://doi.org/10.1021/acs.macromol.7b02352" @default.
• W2783241771 hasPublicationYear "2018" @default.
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