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Register a new userNonlinear dielectric spectroscopy in a fragile plastic crystal
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In this work we provide a thorough examination of the nonlinear dielectric properties of a succinonitrile-glutaronitrile mixture, representing one of the rare example of a plastic crystal with fragile glassy dynamics. The detected alteration of the complex dielectric permittivity under high fields can be explained considering the heterogeneous nature of glassy dynamics and a field-induced variation of entropy. While the first mechanism was also found in structural glass formers, the latter effect seems to be typical for plastic crystals. Morover, the third harmonic component of the dielectric susceptibility is reported, revealing a spectral shape as predicted for cooperative molecular dynamics. In accord with the fragile nature of the glass transition in this plastic crystal, we deduce a relatively strong temperature dependence of the number of correlated molecules, in contrast to the much weaker temperature dependence in plastic-crystalline cyclo-octanol, whose glass transition is of strong nature.
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The glassy dynamics of plastic-crystalline cyclo-octanol and ortho-carborane, where only the molecular reorientational degrees of freedom freeze without long-range order, is investigated by nonlinear dielectric spectroscopy. Marked differences to canonical glass formers show up: While molecular cooperativity governs the glassy freezing, it leads to a much weaker slowing down of molecular dynamics than in supercooled liquids. Moreover, the observed nonlinear effects cannot be explained with the same heterogeneity scenario recently applied to canonical glass formers. This supports ideas that molecular relaxation in plastic crystals may be intrinsically non-exponential. Finally, no nonlinear effects were detected for the secondary processes in cyclo-octanol.
We summarize current developments in the investigation of glassy matter using nonlinear dielectric spectroscopy. This work also provides a brief introduction into the phenomenology of the linear dielectric response of glass-forming materials and discusses the main mechanisms that can give rise to nonlinear dielectric response in this material class. Here we mainly concentrate on measurements of the conventional dielectric permittivity at high fields and the higher-order susceptibilities characterizing the 3-omega and 5-omega components of the dielectric response as performed in our group. Typical results on canonical glass-forming liquids and orientationally disordered plastic crystals are discussed, also treating the special case of supercooled monohydroxy alcohols.
This work aims at reconsidering several interpretations coexisting in the recent literature concerning non-linear susceptibilities in supercooled liquids. We present experimental results on glycerol and propylene carbonate showing that the three independent cubic susceptibilities have very similar frequency and temperature dependences, both for their amplitudes and phases. This strongly suggests a unique physical mechanism responsible for the growth of these non-linear susceptibilities. We show that the framework proposed by two of us [BB, Phys. Rev. B 72, 064204 (2005)], where the growth of non-linear susceptibilities is intimately related to the growth of glassy domains, accounts for all the salient experimental features. We then review several complementary and/or alternative models, and show that the notion of cooperatively rearranging glassy domains is a key (implicit or explicit) ingredient to all of them. This paves the way for future experiments which should deepen our understanding of glasses.
We study nonlinear response in quantum spin systems {near infinite-randomness critical points}. Nonlinear dynamical probes, such as two-dimensional (2D) coherent spectroscopy, can diagnose the nearly localized character of excitations in such systems. {We present exact results for nonlinear response in the 1D random transverse-field Ising model, from which we extract information about critical behavior that is absent in linear response. Our analysis yields exact scaling forms for the distribution functions of relaxation times that result from realistic channels for dissipation in random magnets}. We argue that our results capture the scaling of relaxation times and nonlinear response in generic random quantum magnets in any spatial dimension.
Many plastic crystals, molecular solids with long-range, center-of-mass crystalline order but dynamic disorder of the molecular orientations, are known to exhibit exceptionally high ionic conductivity. This makes them promising candidates for applications as solid-state electrolytes, e.g., in batteries. Interestingly, it was found that the mixing of two different plastic-crystalline materials can considerably enhance the ionic dc conductivity, an important benchmark quantity for electrochemical applications. An example is the admixture of different nitriles to succinonitrile, the latter being one of the most prominent plastic-crystalline ionic conductors. However, until now only few such mixtures were studied. In the present work, we investigate succinonitrile mixed with malononitrile, adiponitrile, and pimelonitrile, to which 1 mol% of Li ions were added. Using differential scanning calorimetry and dielectric spectroscopy, we examine the phase behavior and the dipolar and ionic dynamics of these systems. We especially address the mixing-induced enhancement of the ionic conductivity and the coupling of the translational ionic mobility to the molecular reorientational dynamics, probably arising via a revolving-door mechanism.
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