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Emergence of solid-like Debye scaling in the vibrational density of states of liquids under nanoconfinement

Yuanxi YuSha JinXue Fan ...+3 Liang Hong
Feb 2024
At frequencies higher than the inverse of the structural relaxation time $\tau$, the dynamics of liquids display several solid-like properties, including propagating collective shear waves and emergent elasticity. However, in classical bulk liquids, where $\tau$ is typically of the order of 1 ps or less, this solid-like behavior remains elusive in the low-frequency region of the vibrational density of states (VDOS). Here, we provide compelling evidence for the emergent solid-like nature of liquids at short distances through inelastic neutron scattering measurements of the low-frequency VDOS in liquid water and glycerol confined within graphene oxide membranes. In particular, upon increasing the strength of confinement, we observe a transition from a liquid-like VDOS (linear in the frequency $\omega$) to a solid-like behavior (Debye law, $\sim\omega^2$) in the range of $1$-$4$ meV. Molecular dynamics simulations confirm these findings and reveal additional solid-like features, including propagating collective shear waves and a reduction in the self-diffusion constant. Finally, we show that the onset of solid-like dynamics is pushed towards low frequency along with the slowing-down of the relaxation processes upon confinement, and that the scale at which solidity emerges is qualitatively compatible with k-gap theory and the concept of gapped momentum states. Our results provide convincing experimental evidence of the continuity between liquids and solids, as originally advocated by Frenkel and Maxwell, and a deeper understanding of the dynamics of liquids across a wide range of length scales.
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