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Register a new userEvidence of growing spatial correlations at the glass transition from nonlinear response experiments
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Fran\\c{c}ois Ladieu
Publication date
2010
fields
Physics
and research's language is
English
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The ac nonlinear dielectric response $chi_3(omega,T)$ of glycerol was measured close to its glass transition temperature $T_g$ to investigate the prediction that supercooled liquids respond in an increasingly non-linear way as the dynamics slows down (as spin-glasses do). We find that $chi_3(omega,T)$ indeed displays several non trivial features. It is peaked as a function of the frequency $omega$ and obeys scaling as a function of $omega tau(T)$, with $tau(T)$ the relaxation time of the liquid. The height of the peak, proportional to the number of dynamically correlated molecules $N_{corr}(T)$, increases as the system becomes glassy, and $chi_3$ decays as a power-law of $omega$ over several decades beyond the peak. These findings confirm the collective nature of the glassy dynamics and provide the first direct estimate of the $T$ dependence of $N_{corr}$.
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A theory for the non-local shear stress correlations in supercooled liquids is derived from first principles. It captures the crossover from viscous to elastic dynamics at an idealized liquid to glass transition and explains the emergence of long-ranged stress correlations in glass, as expected from classical continuum elasticity. The long-ranged stress correlations can be traced to the coupling of shear stress to transverse momentum, which is ignored in the classic Maxwell model. To rescue this widely used model, we suggest a generalization in terms of a single relaxation time $tau$ for the fast degrees of freedom only. This generalized Maxwell model implies a divergent correlation length $xiproptotau$ as well as dynamic critical scaling and correctly accounts for the far-field stress correlations. It can be rephrased in terms of generalized hydrodynamic equations, which naturally couple stress and momentum and furthermore allow to connect to fluidity and elasto-plastic models.
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