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We review the works devoted to third and fifth harmonic susceptibilities in glasses, namely $\chi$ (3) 3 and $\chi$ (5) 5. We explain why these nonlinear responses are especially well adapted to test whether or not some amorphous correlations develop upon cooling. We show that the experimental frequency and temperature dependences of $\chi$ (3) 3 and of $\chi$ (5) 5 have anomalous features, since their behavior is qualitatively different to that of an ideal gas, which is the high-temperature limit of a fluid. Most of the works have interpreted this anomalous behavior as reflecting the growth, upon cooling, of amorphously ordered domains, as predicted by the general framework of Bouchaud and Biroli (BB). We explain why most-if not all-of the challenging interpretations can be recast in a way which is consistent with that of Bouchaud and Biroli. Finally, the comparison of the anomalous features of $\chi$ (5) 5 and of $\chi$ (3) 3 shows that the amorphously ordered domains are compact, i.e., the fractal dimension d f is close to the dimension d of space. This suggests that the glass transition of molecular liquids corresponds to a new universality class of critical phenomena.

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.

Glasses are ubiquitous in daily life and technology. However the microscopic mechanisms generating this state of matter remain subject to debate: Glasses are considered either as merely hyper-viscous liquids or as resulting from a genuine thermodynamic phase transition towards a rigid state. We show that third- and fifth-order susceptibilities provide a definite answer to this longstanding controversy. Performing the corresponding high-precision nonlinear dielectric experiments for supercooled glycerol and propylene carbonate, we find strong support for theories based upon thermodynamic amorphous order. Moreover, when lowering temperature, we find that the growing transient domains are compact - that is their fractal dimension d_f = 3. The glass transition may thus represent a class of critical phenomena different from canonical second-order phase transitions for which d_f < 3., Comment: 9 pages, 3 figures

We have measured, as a function of the age $t_a$, the aging of the nonlinear dielectric susceptibility $\chi_3$ of glycerol below the glass transition. Whereas the linear susceptibility can be accurately accounted for in terms of an age dependent relaxation time $\tau_{\alpha}(t_a)$, this scaling breaks down for $\chi_3$, suggesting an increase of the amplitude of $\chi_3$. This is a strong indication that the number $N_{corr}$ of molecules involved in relaxation events increases with $t_a$. For $T=0.96 \times T_g$, we find that $N_{corr}$ increases by $\sim 10%$ when $t_a$ varies from $1\mathrm{ks}$ to $100\mathrm{ks}$. This sheds new light on the relation between length scales and time scales in glasses., Comment: Accepted in Physical Review Letters

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 Physics

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.

We present our first experimental determination of the magnetic noise of a superspinglass made of < 1 pico-liter frozen ferrofluid. The measurements were performed with a local magnetic field sensor based on Hall microprobes operated with the spinning current technique. The results obtained, though preliminary, qualitatively agree with the theoretical predictions of Fluctuation-Dissipation theorem (FDT) violation [1]., Comment: 4pages, 2 figures

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 figures

In this paper we investigate the superspin glass behavior of a concentrated assembly of interacting maghemite nanoparticles and compare it to that of canonical atomic spin glass systems. ac versus temperature and frequency measurements show evidence of a superspin glass transition taking place at low temperature. In order to fully characterize the superspin glass phase, the aging behavior of both the thermo-remanent magnetization (TRM) and ac susceptibility has been investigated. It is shown that the scaling laws obeyed by superspin glasses and atomic spin glasses are essentially the same, after subtraction of a superparamagnetic contribution from the superspin glass response functions. Finally, we discuss a possible origin of this superparamagnetic contribution in terms of dilute spin glass models.

The dc-magnetization of the unique S=1/2 kagome antiferromagnet Herbertsmithite has been measured down to 0.1K. No sign of spin freezing is observed in agreement with former muSR and ac-susceptibility results. The low temperature magnetic response is dominated by a defect contribution which exhibits a new energy scale $\simeq 1$ K, likely reflecting the coupling of the defects. The defect component is saturated at low temperature by H>8T applied magnetic fields which enables us to estimate an upper bound for the non saturated intrinsic kagome susceptibility at T=1.7K., Comment: to appear in PRB

We report low-temperature magnetisation measurements on a large number of purified ropes of single wall carbon nanotubes. In spite of a large superparamagnetic contribution due to the small ferromagnetic catalytical particles still present in the sample, at low temperature ($T < 0.5K$) and low magnetic field ($H < 80 Oe$), a diamagnetic signal is detectable. This low temperature diamagnetism can be interpreted as the Meissner effect in ropes of carbon nanotubes which have previously been shown to exhibit superconductivity from transport measurements., Comment: 10 pages 3 figures

Volborthite compound is one of the very few realizations of S=1/2 quantum spins on a highly frustrated kagome-like lattice. Low-T SQUID measurements reveal a broad magnetic transition below 2K which is further confirmed by a peak in the 51V nuclear spin relaxation rate (1/T1) at 1.4K$\pm$0.2K. Through 51V NMR, the ground state (GS) appears to be a mixture of different spin configurations, among which 20% correspond to a well defined short range order, possibly of the $\sqrt{3} \times \sqrt{3}$ type. While the freezing involve all the Cu$^{2+}$ spins, only 40% of the copper moment is actually frozen which suggests that quantum fluctuations strongly renormalize the GS., Comment: 4 pages, 4 figures, to appear in PRL

In this paper, we review several important features of the out-of-equilibrium dynamics of spin glasses. Starting with the simplest experiments, we discuss the scaling laws used to describe the isothermal aging observed in spin glasses after a quench down to the low temperature phase. We report in particular new results on the sub-aging behaviour of spin glasses. We then discuss the rejuvenation and memory effects observed when a spin glass is submitted to temperature variations during aging, from the point of view of both energy landscape pictures and of real space pictures. We highlight the fact that both approaches point out the necessity of hierarchical processes involved in aging. Finally, we report an investigation of the effect of small temperature variations on aging in spin glass samples with various anisotropies which indicates that this hierarchy depends on the spin anisotropy., Comment: submitted for the Proceedings of Stat Phys 22, Bangalore (India)

The magnetisation relaxations of three different types of geometrically frustrated magnetic systems have been studied with the same experimental procedures as previously used in spin glasses. The materials investigated are Y$_2$Mo$_2$O$_7$ (pyrochlore system), SrCr$_{8.6}$Ga$_{3.4}$O$_{19}$ (piled pairs of Kagom\'e layers) and (H$_3$O)Fe$_3$(SO$_4$)$_2$(OH)$_6$ (jarosite compound). Despite a very small amount of disorder, all the samples exhibit many characteristic features of spin glass dynamics below a freezing temperature $T_g$, much smaller than their Curie-Weiss temperature $\theta$. The ageing properties of their thermoremanent magnetization can be well accounted for by the same scaling law as in spin glasses, and the values of the scaling exponents are very close. The effects of temperature variations during ageing have been specifically investigated. In the pyrochlore and the bi-Kagom\'e compounds, a decrease of temperature after some waiting period at a certain temperature $T_p$ re-initializes ageing and the evolution at the new temperature is the same as if the system were just quenched from above $T_g$. However, as the temperature is raised back to $T_p$, the sample recovers the state it had previously reached at that temperature. These features are known in spin glasses as rejuvenation and memory effects. They are clear signatures of the spin glass dynamics. In the Kagom\'e compound, there is also some rejuvenation and memory, but much larger temperature changes are needed to observe the effects. In that sense, the behaviour of this compound is quantitatively different from that of spin glasses., Comment: latex VersionCorrigee4.tex, 4 files, 3 figures, 5 pages (Proceedings of the International Conference on Highly Frustrated Magnetism (HFM2003), August 26-30, 2003, Institut Laue Langevin (ILL), Grenoble, France)

The 1kHz real part $\chi'$ of the dielectric constant of a structural glass was measured at low temperature $T$ down to 14 mK. Reducing the sample thickness $h$ to 10 nm suppresses the usual minimum of $\chi'$ for measuring fields $E<.5 $ MV/m. This contradicts the Two Level System (TLS) model but is well accounted for by including TLS-TLS interactions where excitations delocalize between TLS's through a $E$-induced mechanism recently designed: for small $h$'s this interaction is reduced, which explains the two-dimensional behavior of $\chi'(T)$. Hence, interactions play a key role in standard thick samples., Comment: latex finesse3.tex, 5 files, 4 figures, 4 pages [SPEC-S02/050], submitted to Phys. Rev. Lett

We have calculated the real part $\chi'$ of the nonlinear dielectric susceptibility of amorphous insulators in the kHz range, by using the two-level system model and a nonperturbative numerical quantum approach. At low temperature $T$, it is first shown that the standard two-level model should lead to a \textit{decrease} of $\chi'$ when the measuring field $E$ is raised, since raising $E$ increases the population of the upper level and induces Rabi oscillations canceling the ones induced from the ground level. This predicted $E$-induced decrease of $\chi'$ is at \textit{odds} with experiments. However, a \textit{good agreement} with low-frequency experimental nonlinear data is achieved if, in our fully quantum simulations, interactions between defects are taken into account by a new relaxation rate whose efficiency increases as $\sqrt{E}$, as was proposed recently by Burin \textit{et al.} (Phys. Rev. Lett. {\bf 86}, 5616 (2001)). In this approach, the behavior of $\chi'$ at low $T$ is mainly explained by the efficiency of this new relaxation channel. This new relaxation rate could be further tested since it is shown that it should lead: \textit{i)} to a completely new nonlinear behavior for samples whose thickness is $\simeq 10$ nm; \textit{ii)} to a decrease of nonequilibrium effects when $E$ is increased., Comment: latex Sept02.tex, 5 files, 4 figures, 17 pages, submitted to Eur. Phys. J. B. Text changes

The magnetic field dependence of the low frequency dielectric constant $e_r$(H) of a structural glass a - SiO2 + xCyHz was studied from 400 mK to 50 mK and for H up to 3T. Measurement of both the real and the imaginary parts of $e_r$ is used to eliminate the difficult question of keeping constant the temperature of the sample while increasing H: a non-zero $e_r$(H) dependence is reported in the same range as that one very recently reported on multicomponent glasses. In addition to the recently proposed explanation based on interactions, the reported $e_r$(H) is interpreted quantitatively as a consequence of the disorder lying within the nanometric barriers of the elementary tunneling systems of the glass., Comment: latex Bcorrige1.tex, 5 files, 4 figures, 7 pages [SPEC-S02/009]

Variable range hopping transport has been investigated in amorphous YSi from 30 mK to 2 K as a function of the temperature T and electric field F. For F=0, where conduction is along sinuous paths (isotropic percolation), the conductance G depends on T according to an Efros-Shklovskii law. The nonlinear I-V's were studied up to very high fields for which G no longer depends on T (directed percolation : current paths along F). We show that heating effects are negligible. Then, we show that for low F values, ln(G(F,T))=ln(G(0,T))-eFL/kT. The order of magnitude (5-10 nm) and the T dependence of L agree with theoretical predictions. From L, we extract the dielectric constant. The very high electric field data do not agree with the theoretical predictions, which could be due to tunneling across the mobility edge. For intermediate electric fields our data evidence the influence of the straightening of the paths (transition from isotropic to directed percolation). The statistical properties of the segments of the paths where the current flows against the electrical force are extracted for the first time., Comment: latex, 11 files, 16 pages, submitted to Phys. Rev. B

We have observed reproducible conductance fluctuations at low temperature in a small GaAs:Si wire driven across the Anderson transition by the application of a gate voltage. We analyse quantitatively the log-normal conductance statistics in terms of truncated quantum fluctuations. Quantum fluctuations due to small changes of the electron energy (controlled by the gate voltage) cannot develop fully due to identified geometrical fluctuations of the resistor network describing the hopping through the sample. The evolution of the fluctuations versus electron energy and magnetic field shows that the fluctuations are non-ergodic, except in the critical insulating region of the Anderson transition, where the localization length is larger than the distance between Si impurities. The mean magnetoconductance is in good accordance with simulations based on the Forward-Directed-Paths analysis, i.e. it saturates to $ {\rm ln} (\sigma (H>1)/\sigma (0))\simeq 1, $ as $ \sigma (0) $ decreases over orders of magnitude in the strongly localized regime., Comment: Email contact: sanquer@amoco.saclay.cea.fr