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Experimental tests of the fluctuation- dissipation relation in aging glassy systems some comments on the D. L’Hôte SPEC CE Saclay
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Very beautiful (and difficult) experiments Direct observation of the heterogeneities E. Vidal Russel & N. E. Israeloff Nature 408 (2000) 695 0 2500s 301.5 K 0 700nm Electric Force Microscopy: realizes (almost) the dream to visualize molecular systems as (e.g.) a microscope for colloids, a camera for granular systems, a plotter for simulations... Grigera & Israeloff: First measurement of FDT violation in a structural glass (glycerol) Local measurements
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PVAc Test of FDTviolation in ageing PVAc (bulk) time (s) Initial dT/dt=0.15 K/s “slow quench” aging 300 330 T (K) 0 400 Quench duration not small in comparison with relaxation time at 300K Slow quench Little or no FDR violation relaxation time T (K)
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Test of FDT violation in ageing PVAc (bulk) time (s) “fast quench” initial dT/dt=10 K/s PVAc N.E. Israeloff et al. R.L. Leheny & S.R. Nagel PRB57, 5154 (98). Glycerol dT/dt=0.025 K/s T i =206K PVAc 0 1 2 3 4 5 6 7 Fast quench T (K) 330 320 310 300 Log f t w
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Test of FDT in ageing PVAc (bulk) Large T eff (comp. glycerol) f fixed TiTi TgTg TfTf twtw L. Buisson & S. Ciliberto Physica D204, 1 (04) Polycarbonate Tg=419K Tf=0.93Tg quench: 1 K/s 2 Hz 7 Hz Not gaussian intermittency (spikes) Origin of large T eff ? of different T eff ’s ? of T eff < T f ? Fast quench tw1tw1 t w >1 t w (s) T eff (K) T eff < T f T eff
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Test of FDT in ageing PVAc (bulk) Scaling for spin glasses : Same scaling for response and correlation vs. (t-t w )/t w . If <1, time replaced by effective time (comes from polymers !) same close to 1 ( 0.87 ); but ac ≈ D. Hérisson and M. Ocio, EPJB40, 283 (04) Scaling ? "subaging" (i.e; < 1): due to quench rate ? Parker et al. PRB74, 184432 (06) Rodriguez et al. PRL91, 037203 (03) T eff < T f ?? f twf tw 0.45
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Test of FDT in ageing PVAc What about T during the quench ? Phonon bath DH Phonon bath DH time TiTi TiTi ? TfTf Phonon bath DH TfTf TfTf quench ( t ) t relaxation time of Dynamic Het. i = thermal coupling time to phonon bath R. Richert, S. Weinstein PRL97, 095703 (06) K. Schröter and E. Donth, J. Chem. Phys. 113, 9101 (00) R. V. Chamberlin, PRL82, 2520 (99)...
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Physics of aging e.g.. Domain growth models: T eff ∞ ; (A. Barrat PRE57, 3629 (98)) T eff < T f ? Negative FD ratio for KCModels (heterogeneous dynamics) P. Mayer et al. PRL96, 030602 (06): Also: Barrat & Kob (Nathan) Many T eff ’s ? "Unusual" scaling ? More than two “time sectors“ ? (2 time sectors: FDVratio = 1 or T f /T eff in e.g. mean field models) Test of FDT in ageing PVAc (bulk) The meaning of large T eff, T eff < T f, several T eff ’s ? Possible other origin ? Internal constraints ? release noise Thermal contraction during quench (but the rearrangements to density are also the physics...) Weak T eff in glycerol, large T eff in polymers ? J.L. Barrat & W. Kob, EPL46, 637 (99) Molecular dynamics simulation e.g.: T eff = 2.2 T f (660K !) Additional noise. Nathan’s model
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Local polarization measurements t =0 t =17mn t =48mn 0 100300 200 0 400600nm 500 0 100 300 200 500 400 Spatial fluctuations of the polarization due to DH’s ? P x Assuming each DH has its own polarization. DH size 3nm Probed volume: 20 30 30 nm 3 10 3 DH among which only a few are "active" PVAc DH Convol. resol. P(x) C. Dalle-Ferrier et al. Phys. Rev. E76, 041510 (07) PVAc glass trans.
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What do we see ? "active" DH’s (3 3 nm 3 ) 30 30 20nm 3 ? Or what ? Response/Correlation => spatio-temporal distribution of FDR violation/T eff 0 2500s 0 700nm 301.5 K 305.5 K 0 2500 Issues: Correlations between DH’s: fusions/splitting, fast DH’s close (or not) to slow DH’s ? Spatial structure DH’s Do DH’s move? Correlation (Charac. time) – (DH size) ? Birth, death: comes from what, replaced by what ? etc. Issues: The same with something else than DH’s... Direct observation of the DH’s in a polymer ? H.E. Castillo, C. Chamon, L.F. Cugliandolo, M.P. Kennett, PRL88, 237201 (2002)
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Test of FDR in ageing PVAc (local) Q=C eff V P C eff = 7.2x10 -18 F R(t) =A-Q(t)/V C(t)= T (K)-1/k B slope 305.5262 ± 15 303.5258 ± 30 302.5253 ± 40 305.5 K 303.5 K 302.5 K If Q=(corr.) Q, T eff (corr.) T eff Corrections: Geometry of dipoles acting on the tip Effective field Q = f(p i,r i ) C = f(p i, r i ). f(p j,r j ) correlations between DH’s
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Heisenberg spin glass L. Berthier & A.P. Young PRB69, 184423 (04) twtw Ageing : growing of a correlation length ? E. Vidal Russel & N. E. Israeloff Nature 408 (2000) 695 2 (C) time position K.S. Sinnathamby, H. Oukris & N. E. Israeloff PRL 95 (05) 067205 N HD 1/2 Simple model: Independent DH’s superposition of Lorentzians But: - Correlations size – char. time - Correlations between DH’s - etc. Calculation ?
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Open issues Violation of Fluctuation-dissipation theorem: Very attractive experiments But: T eff < T f No unique T eff (> T f ) for t w 1 Unusual scaling of T eff Additional noise ? Nathan’s model Extrinsic noise ? « DHs temperature" vs. phonon temperature Electric force microscopy: a fantastic tool for local FDT violations, and many other things (spatio-temporal correlations...) What are the observed structures ? Calculations/simulations of the experimental situation ?
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Simple dynamic heterogeneity Correlated dynamic herogeneities
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