Study of the heating effect contribution to the nonlinear dielectric response of a supercooled liquid

We present a detailed study of the heating effects in dielectric measurements carried out on a liquid. Such effects come from the dissipation of the electric power in the liquid and give a contribution to the nonlinear third harmonics susceptibility chi_3 which depends on the frequency and temperature. This study is used to evaluate a possible `spurious' contribution to the recently measured nonlinear susceptibility of an archetypical glassforming liquid (Glycerol). Those measurements have been shown to give a direct evaluation of the number of dynamically correlated molecules temperature dependence close to the glass transition temperature T_g~190K (Crauste-Thibierge et al., Phys. Rev. Lett 104,165703(2010)). We show that the heating contribution is totally negligible (i) below 204K at any frequency; (ii) for any temperature at the frequency where the third harmonics response chi_3 is maximum. Besides, this heating contribution does not scale as a function of f/f_{\alpha}, with f_{\alpha}(T) the relaxation frequency of the liquid. In the high frequency range, when f/f_{\alpha} >= 1, we find that the heating contribution is damped because the dipoles cannot follow instantaneously the temperature modulation due to the heating phenomenon. An estimate of the magnitude of this damping is given.Comment: 25 pages, 10 figures, Accepted for publication in Journal of Chemical Physic

A method for measuring the nonlinear response in dielectric spectroscopy through third harmonics detection

We present a high sensitivity method allowing the measurement of the non linear dielectric susceptibility of an insulating material at finite frequency. It has been developped for the study of dynamic heterogeneities in supercooled liquids using dielectric spectroscopy at frequencies 0.05 Hz < f < 30000 Hz . It relies on the measurement of the third harmonics component of the current flowing out of a capacitor. We first show that standard laboratory electronics (amplifiers and voltage sources) nonlinearities lead to limits on the third harmonics measurements that preclude reaching the level needed by our physical goal, a ratio of the third harmonics to the fundamental signal about 7 orders of magnitude lower than 1. We show that reaching such a sensitivity needs a method able to get rid of the nonlinear contributions both of the measuring device (lock-in amplifier) and of the excitation voltage source. A bridge using two sources fulfills only the first of these two requirements, but allows to measure the nonlinearities of the sources. Our final method is based on a bridge with two plane capacitors characterized by different dielectric layer thicknesses. It gets rid of the source and amplifier nonlinearities because in spite of a strong frequency dependence of the capacitors impedance, it is equilibrated at any frequency. We present the first measurements of the physical nonlinear response using our method. Two extensions of the method are suggested.Comment: 25 pages, 8 figure

Real time decoherence of Landau and Levitov quasi-particles in quantum Hall edge channels

Quantum Hall edge channels at integer filling factor provide a unique test-bench to understand decoherence and relaxation of single electronic excitations in a ballistic quantum conductor. In this Letter, we obtain a full visualization of the decoherence scenario of energy (Landau) and time (Levitov) resolved single electron excitations at filling factor $\nu=2$. We show that the Landau excitation exhibits a fast relaxation followed by spin-charge separation whereas the Levitov excitation only experiences spin-charge separation. We finally suggest to use Hong-Ou-Mandel type experiments to probe specific signatures of these different scenarios.Comment: 14 pages, 8 figure

Evidence of growing spatial correlations at the glass transition from nonlinear response experiments

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 $N_{corr}$.Comment: 22 pages, 6 figures. With respect to v1, a few new sentences were added in the introduction and conclusion, references were updated, some typos corrected

Observation of superspin glass state in magnetically textured ferrofluid (gamma-Fe2O3)

Magnetic properties in a magnetically textured ferrofluid made out of interacting maghemite (gamma-Fe2O3) nanoparticles suspended in glycerin have been investigated. Despite the loss of uniform distribution of anisotropy axes, a superspin glass state exists at low temperature in a concentrated, textured ferrofluid as in the case of its non-textured counterpart. The onset of superspin glass state was verified from the sample's AC susceptibility. The influence of the anisotropy axis orientation on the aging behavior in the glassy states is also discussed

Experimental search for dynamic heterogeneities in molecular glass formers

We have measured the linear dielectric susceptibility of two molecular glass formers close to Tg in order to estimate the size of the dynamically correlated clusters of molecules which are expected to govern the physics of glass formation. This size has been shown to be related to the dynamic dielectric susceptibility dEps(w)/dT (Eps : dielectric susceptibility, T : temperature, w&#61472;: frequency). To allow for an accurate determination of the T derivative, we scanned the interval 192 < T < 232 K every 1 K for glycerol and 159 < T < 179 K every 0.5 K for propylene carbonate. The resolution on T variations was about 1 mK. The result for glycerol is that the number of correlated molecules increases by a factor 3 when T goes from 226 to 195 K. It has been shown that the non-linear susceptibility provides a direct measurement of dynamic correlations. To measure it, we used a standard Lockin technique yielding the third harmonic of the current flowing out of a capacitor. We obtained only an upper limit on the ratio of the third to the first harmonic, due to the non-linear response of standard electronics.Comment: 7 page

Superspin glass aging behavior in textured and nontextured frozen ferrofluid

The effect of magnetic anisotropy-axis alignment of individual nanoparticles on the collective aging behavior in the superspin glass state of a frozen ferrofluid has been investigated. The ferrofluid studied here consists of maghemite nanoparticles (\gamma-Fe2O3, mean diameter = 8.6 nm) dispersed in glycerin at a volume fraction of ~15%. The low temperature aging behavior has been explored through 'zero-field cooled magnetization' (ZFCM) relaxation measurements using SQUID magnetometry. The ZFCM response functions were found to scale with effective age of the system in both textured and non-textured superspin glass states, but with markedly different scaling exponents, \mu. The value of {\mu} was found to shift from ~0.9 in non-textured case to ~ 0.6 in the textured case, despite the identical cooling protocol used in both experiments

Anisotropy-axis orientation effect on the magnetization of {\gamma}-Fe2O3 frozen ferrofluid

The effect of magnetic anisotropy-axis alignment on the superparamagnetic (SPM) and superspin glass (SSG) states in a frozen ferrofluid has been investigated. The ferrofluid studied here consists of maghemite nanoparticles (\gamma-Fe2O3, mean diameter = 8.6 nm) dispersed in glycerine at a volume fraction of ~15%. In the high temperature SPM state, the magnetization of aligned ferrofluid increased by a factor varying between 2 and 4 with respect to that in the randomly oriented state. The negative interaction energy obtained from the Curie-Weiss fit to the high temperature susceptibility in the SPM states as well as the SSG phase onset temperature determined from the linear magnetization curves were found to be rather insensitive to the anisotropy axis alignment. The low temperature aging behaviour, explored via "zero-field cooled magnetization" (ZFCM) relaxation measurements, however, show distinct difference in the aging dynamics in the anisotropy-axis aligned and randomly oriented SSG states.Comment: to appear in Journal of Physics D: Applied Physic