Anomalous dynamical light scattering in soft glassy gels

We compute the dynamical structure factor S(q,τ) of an elastic medium where force dipoles appear at random in space and in time, due to “micro-collapses” of the structure. Various regimes are found, depending on the wave vector q and the collapse time θ. In an early-time regime, the logarithm of the structure factor behaves as (qτ)^3/2, as predicted in L. Cipelletti, S. Manley, R.C. Ball, D.A. Weitz, Phys. Rev. Lett. 84, 2275 (2000) using heuristic arguments. However, in an intermediate-time regime we rather obtain a (qτ)^5/4 behaviour. Finally, the asymptotic long-time regime is found to behave as q ^3/2τ. We also give a plausible scenario for aging, in terms of a strain-dependent energy barrier for micro-collapses. The relaxation time is found to grow with the age t _w, quasi-exponentially at first, and then as t _w ^4/5 with logarithmic corrections. Received 23 July 2001     

Proton NMR relaxation in albumin solutions doped with Mn(II)

The aim of this study is to obtain further information about the source of proton relaxation in the Mn(II)-human serum albumin complex. For this purpose, proton relaxation rates in albumin solutions 1/T ₁ and 1/T ₂ were measured versus increasing amounts of manganese [Mn_t]. The fractions of manganese bound to albumin [Mn_b] and free manganese [Mn_f] were then determined from proton relaxation rate enhancement data. Paramagnetic contributions of bound manganese to the observed relaxation rates (1/T _1p^*)_b and (1/T _2p^*)_b were also determined. Finally, the (1/T _2p^*)_b/(1/T _1p^*)_b ratio was used in a derived equation to estimate an effective correlation time τ. Mean τ value of the complex was found to be in the order of 3 ns, while the hydration number of bound manganese q was estimated to be about 4. The 1/τ was found to be the sum of the inverse values of rotational correlation time 1/τ _r, mean residence time of water in hydration spheres of the complex 1/τ _m, and longitudinal electronic relaxation time of manganese 1/τ _s in the complex. In conclusion, the relaxation mechanism in albumin solutions containing Mn(II) can be interpreted through dipolar and scalar interactions modulated by τ _r, τ _m and τ _s. This analysis enables one to get reasonable figures for the τ _r and q of Mn(II) in albumin solution.     

Non-linear scission/recombination kinetics of living polymerization

Living polymers are formed by reversible association of primary units (unimers). Generally the chain statistical weight involves a factor σ < 1 suppressing short chains in comparison with free unimers. Living polymerization is a sharp thermodynamic transition for σ ≪ 1 which is typically the case. We show that this sharpness has an important effect on the kinetics of living polymerization (one-dimensional association). The kinetic model involves i) the unimer activation step (a transition to an assembly-competent state); ii) the scission/recombination processes providing growth of polymer chains and relaxation of their length distribution. Analyzing the polymerization with no chains but unimers at t = 0 , with initial concentration of unimers M ≳ M ^* (M^* is the critical polymerization concentration), we determine the time evolution of the chain length distribution and find that: 1) for M ^* ≪ M ≪ M ^*/σ the kinetics is characterized by 5 distinct time stages demarcated by 4 characteristic times t₁, t₂, t₃ and t^*; 2) there are transient regimes (t ₁ ≲ t ≲ t ₃) when the molecular-weight distribution is strongly non-exponential; 3) the chain scissions are negligible at times shorter than t₂. The chain growth is auto-accelerated for t ₁ ≲ t ≲ t ₂ : the cut-off chain length (= polymerization degree 〈n〉_w N ₁ ∝ t ² in this regime. 4) For t ₂ < t < t ₃ the length distribution is characterized by essentially 2 non-linear modes; the shorter cut-off length N₁ is decreasing with time in this regime, while the length scale N₂ of the second mode is increasing. (5) The terminal relaxation time of the polymer length distribution, t^*, shows a sharp maximum in the vicinity of M^*; the effective exponent is as high as ∼ σ^-1/3 just above M^*.     

The Behaviour of Aging Functions in One-Dimensional Bouchaud's Trap Model

Let τ_i be a collection of i.i.d. positive random variables with distribution in the domain of attraction of an α-stable law with α<1. The symmetric Bouchaud's trap model on ℤ is a Markov chain X(t) whose transition rates are given by w_xy=(2τ_x)⁻¹ if x, y are neighbours in ℤ. We study the behaviour of two correlation functions: ℙ[X(t_w+t)=X(t_w)] and It is well known that for any of these correlation functions a time-scale t=f(t_w) such that aging occurs can be found. We study these correlation functions on time-scales different from f(t_w), and we describe more precisely the behaviour of a singular diffusion obtained as the scaling limit of Bouchaud's trap model. Work supported by DFG Research Center Matheon ``Mathematics for key technologies'     

Dynamics of isolated twin boundary in (TMTSF)

Intermittent and irregular motion of isolated twin boundary (kink) in organic crystal (TMTSF)₂PF₆ was studied at room temperature. Both the local velocity and the time of intermission are determined not only by external stress and temperature but also by the time (t w) elapsed after the backward passage and before the following forward one. When the kink moves after longer t w, its velocity becomes smaller and the time of intermission longer. Both tend to saturate for t w longer than 10² s. This result indicates that some disorder is induced in the lattice by the backward motion and it is relaxed during t w. We also found that the effect of the backward motion of one kink on its following motion is equivalent quantitatively to that of the forward motion of the pair-created counterpart. Received: 14 April 1998 / Received in final form and Accepted: 1st September 1998     

Reacting polymers with highly correlated initial conditions

We propose and theoretically study an experiment designed to measure short-time polymer reaction kinetics in melts or dilute solutions. The photolysis of groups centrally located along chain backbones, one group per chain, creates pairs of spatially highly correlated macroradicals. We calculate time-dependent rate coefficients κ(t) governing their first-order recombination kinetics, which are novel on account of the far-from-equilibrium initial conditions. In dilute solutions (good solvents) reaction kinetics are intrinsically weak, despite the highly reactive radical groups involved. This leads to a generalised mean-field kinetics in which the rate of radical density decay - ∼S(t), where S(t) ∼t ^{- (1 + g/3)} is the equilibrium return probability for 2 reactive groups, given initial contact. Here g≈ 0.27 is the correlation hole exponent for self-avoiding chain ends. For times beyond the longest coil relaxation time τ, - ∼S(t) remains true, but center of gravity coil diffusion takes over with rms displacement of reactive groups x(t) ∼t ^1/2 and S(t) ∼ 1/x ³(t). At the shortest times ( t 10^-6s), recombination is inhibited due to spin selection rules and we find ∼tS(t). In melts, kinetics are intrinsically diffusion-controlled, leading to entirely different rate laws. During the regime limited by spin selection rules, the density of radicals decays linearly, n(0) - n(t) ∼t. At longer times the standard result - ∼d ³(t)/d (for randomly distributed ends) is replaced by ∼d2x ³(t)/d ² for these correlated initial conditions. The long-time behavior, t > τ, has the same scaling form in time as for dilute solutions. Received 18 May 2000     

Stretched exponential relaxation in the Coulomb glass

The relaxation of the specific heat and the entropy to their equilibrium values is investigated numerically for the three-dimensional Coulomb glass at very low temperatures. The long time relaxation follows a stretched exponential function, f (t) = f ₀exp - (t/τ)^β , with the exponent β increasing with the temperature. The relaxation time diverges as an Arrhenius law when T→ 0. Received 24 May 2001 and Received in final form 12 September 2001     

On the investigation of magnetic critical phenomena in ferromagnets by μSR and PAC

On the basis of current theoretical views on the critical phenomena in isotropic Heisenberg ferromagnets the power temperature behavior Λ=c(τ)λ₀τ^-w has been derived for the muon spin relaxation rate Λ as π-T _c ⁻¹ (T-T _c ) → 0⁺. It is shown that the crossover from an exchange critical regime to a dipolar one is accompanied not only with the change in the critical exponentw in the above law, but also with the reduction of the coefficientc(π). A comparison with the temperature behaviour of the inverse nuclear relaxation timet _R ⁻¹ measured in the PAC experiment is carried out.     

High frequency sound and the boson peak in amorphous silica

We present the results of extensive molecular dynamics computer simulations in which the high frequency dynamics of silica, i.e. for frequencies ν > 0.5 THz, is investigated in the viscous liquid state as well as in the glass state. We characterize the properties of high frequency sound modes by analyzing J _l(q,ν) and J _t(q,ν), the longitudinal and transverse current correlation function, respectively. For wave-vectors q > 0.4 ?^-1 the spectra are sitting on top of a flat background. The dynamic structure factor S(q,ν) exhibits for q > 0.23 ?^-1 a boson peak which is located nearly independent of q around 1.7 THz and for which the intensity scales approximately linearly with temperature. We show that the low frequency part of the boson peak is mainly due to the elastic scattering of transverse acoustic modes with frequencies around 1 THz. The strength of this scattering depends on q and is largest around q = 1.7 ?^-1, the location of the first sharp diffraction peak in the static structure factor. By studying S(q,ν) for different system sizes we show that strong finite size effects are present in the low frequency part of the boson peak in that for small systems part of its intensity is missing. We discuss the consequences of these finite size effects for the structural relaxation. Received 27 June 2000 and Received in final form 9 January 2001     

Field-theoretical Renormalization-Group approach to critical dynamics of crosslinked polymer blends

We consider a crosslinked polymer blend that may undergo a microphase separation. When the temperature is changed from an initial value towards a final one very close to the spinodal point, the mixture is out equilibrium. The aim is the study of dynamics at a given time t, before the system reaches its final equilibrium state. The dynamics is investigated through the structure factor, S(q, t), which is a function of the wave vector q, temperature T, time t, and reticulation dose D. To determine the phase behavior of this dynamic structure factor, we start from a generalized Langevin equation (model C) solved by the time composition fluctuation. Beside the standard de Gennes Hamiltonian, this equation incorporates a Gaussian local noise, ζ. First, by averaging over ζ, we get an effective Hamiltonian. Second, we renormalize this dynamic field theory and write a Renormalization-Group equation for the dynamic structure factor. Third, solving this equation yields the behavior of S(q, t), in space of relevant parameters. As result, S(q, t) depends on three kinds of lengths, which are the wavelength q ⁻¹, a time length scale R(t) ∼ t ^1/z , and the mesh size ξ ^*. The scale R(t) is interpreted as the size of growing microdomains at time t. When R(t) becomes of the order of ξ ^*, the dynamics is stopped. The final time, t ^*, then scales as t ^* ∼ ξ ^{* z}, with the dynamic exponent z = 6−η. Here, η is the usual Ising critical exponent. Since the final size of microdomains ξ ^* is very small (few nanometers), the dynamics is of short time. Finally, all these results we obtained from renormalization theory are compared to those we stated in some recent work using a scaling argument.     

Universality of a dynamical percolative approach to 1/f γ noise

A dynamical percolative model explaining the universality of 1/ f ^γ noise is reported. Exponents γ ranging from 0 to 2 are obtained under the hypothesis that noise originates from random switching events between two ON-OFF states in elemental parts (switchers) of a physical system. The usual noise behaviour with γ very close to 1 in an arbitrarily wide frequency range is obtained assuming a statistical distribution of switcher relaxation time τ proportional to τ ^-1 , as in McWhorter's model. The impact of these results with respect to recent self-organised criticality models is discussed. Received 6 November 2000 and Received in final form 22 May 2001     

On the Distribution of Free Path Lengths for the Periodic Lorentz Gas III

 For r(0,1), let Z _r ={xR ² |dist(x,Z ²)>r/2} and define τ _r (x,v)=inf{t>0|x+tv∂Z _r }. Let Φ _r (t) be the probability that τ _r (x,v)≥t for x and v uniformly distributed in Z _r and §¹ respectively. We prove in this paper that

Fluctuations of Power Injection in Randomly Driven Granular Gases

We investigate the large deviation function π_∞(w) for the fluctuations of the power W(t) = wt, integrated over a time t, injected by a homogeneous random driving into a granular gas, in the infinite time limit. Our analytical study starts from a generalized Liouville equation and exploits a Molecular Chaos-like assumption. We obtain an equation for the generating function of the cumulants μ(λ) which appears as a generalization of the inelastic Boltzmann equation and has a clear physical interpretation. Reasonable assumptions are used to obtain μ(λ) in a closed analytical form. A Legendre transform is sufficient to get the large deviation function π_∞(w). Our main result, apart from an estimate of all the cumulants of W(t) at large times t, is that π_∞ has no negative branch. This immediately results in the inapplicability of the Gallavotti-Cohen Fluctuation Relation (GCFR), that in previous studies had been suggested to be valid for injected power in driven granular gases. We also present numerical results, in order to discuss the finite time behavior of the fluctuations of W (t) . We discover that their probability density function converges extremely slowly to its asymptotic scaling form: the third cumulant saturates after a characteristic time τ larger than ∼50 mean free times and the higher order cumulants evolve even slower. The asymptotic value is in good agreement with our theory. Remarkably, a numerical check of the GCFR is feasible only at small times (at most τ/10), since negative events disappear at larger times. At such small times this check leads to the misleading conclusion that GCFR is satisfied for π_∞(w). We offer an explanation for this remarkable apparent verification. In the inelastic Maxwell model, where a better statistics can be achieved, we are able to numerically observe the “failure” of GCFR.     

Λ(1405) as a multiquark state

In the QCD sum rule approach we predict the Λ (1405) mass by choosing the π⁰Σ⁰ multiquark interpolating field. It is found that the mass is about 1.419 GeV from Π₁ (q ²) sum rule which is more reliable than Π_q (q ²) sum rule, where Π_q (q ²) and Π₁ (q ²) are two invariant functions of the correlator Π (q ²). We also present the sum rules for the K ⁺ p and the π⁺Σ⁺ multiquark states, and compare to those for the π⁰Σ⁰ multiquark state. The mass of the Λ (1600) can be also reproduced in our approach. Received: 11 November 1997 / Revised version: 28 April 1998     

On the Large Time Asymptotics¶of Decaying Burgers Turbulence

The decay of Burgers turbulence with compactly supported Gaussian “white noise” initial conditions is studied in the limit of vanishing viscosity and large time. Probability distribution functions and moments for both velocities and velocity differences are computed exactly, together with the “time-like” structure functions T _n (t,τ)≡< (u(t+τ) -u(t)) ⁿ >. The analysis of the answers reveals both well known features of Burgers turbulence, such as the presence of dissipative anomaly, the extreme anomalous scaling of the velocity structure functions and self similarity of the statistics of the velocity field, and new features such as the extreme anomalous scaling of the “time-like” structure functions and the non-existence of a global inertial scale due to multiscaling of the Burgers velocity field. We also observe that all the results can be recovered using the one point probability distribution function of the shock strength and discuss the implications of this fact for Burgers turbulence in general. Received: 4 October 1999 / Accepted: 4 February 2000     

Relaxation of post-illumination electric fields in strongly biased high-resistance structures with a single deep impurity level

This paper examines how an electric field relaxes when a discontinuous large carrier-depleting voltage applied to high-resistance symmetric metal-semiconductor-metal (MSM) and metal-insulator-semiconductor-insulator-metal (MISIM) structures having a single impurity level, and how its energy level ɛ _t=E _c−E _t and the tunneling transparency T _n,p of the metal-semiconductor or metal-insulator boundary affect the relaxation. It is shown that the relaxation of the field and the form of its steady-state distribution depend on the ratio of the time constant t _p in the majority-carrier (hole) region to the ionization time τ _t ⁻¹ =α _n (n _*+n ₁)+α _p (p _*+p ₁) of a deep trap in the bulk. This ratio determines the relative contributions of free ρ _p,n and bound charge dnsities ρ _t (where α _n,p is the coefficient for capture by an impurity, and p _*, n _*, p ₁, n ₁ are equilibrium concentrations and Shockley-Read constants in the bulk). For τ _t ≈(τ _t )_max≫t _p ,ρ _t ≫ it is found that ρ _p,n and ρ _t ≫ρ _p,n , which corresponds to a trap energy close to , independent of the value of T _n,p , decaying oscillations arise in the concentration distribution, bulk charge, and field appear in the bulk. The amplitude of these oscillations reaches a maximum at time t≈0.4τ _t. Decreasing the ratio α _p/α_n causes τ _t to deviate from (τ _t)_max. When this happens, the field no longer oscillates; instead, it increases with positive curvature in the cathode portion of the bulk. The quantity T _n,p determines the behavior of the field in the neighborhood of the anode. The value of (dE/dx)₀ is positive for MSM structures (T _n,p ≈1), and negative for MISIM structures (T _n,p ≈0). For transparencies close to a critical value T _n,p ⁰ , the field in the structure remains almost uniform over an impurity ionization time. Fiz. Tverd. Tela (St. Petersburg) 39, 1775–1782 (October 1997)     

Anisotropic impurity scattering in palladium silver alloys

Measurements have been made of the Hall coefficientR of some alloys of silver in palladium over the temperature range 1°K to 120°K. The alloys contain between ∼1 and ∼10 at.-% silver. Values ofR were also obtained at room temperature and these were in good agreement with earlier published work. The values ofR are negative in all the alloys, and |R| increases both on reducing the temperature and increasing the silver concentration,c. Below ∼10°K, |R| becomes independent of temperature but shows a linear dependence onc, increasing by a factor of 2.5 over the concentration range measured. This increase is too great to be accounted for in terms of band structure changes alone, so we have examined the effects of anisotropic impurity scattering. To a first approximation it can be shown thatR is proportional to an anisotropy parameterA, defined asA=〈τ ²(k)〉/〈τ(k)〉², whereτ(k) represents the relaxation time of an electron in a statek, and 〈〉 is an average over the Fermi surface. In palladium we assume that the majority of the current is carried by the s-electrons. In the presence of silver impurities these electrons can be scattered into s-states or d-states with relaxation times given byτ _ss α1/c(1−c) andτ _sd α1/c ²(1−c) respectively. FollowingPlate we have assumed thatτ _ss is isotropic and thatτ _sd is anisotropic, leading to an overall anisotropic relaxation time for impurity scattering. We then find the parameterA increases approximately linearly with silver content, in accordance with our experimental results.     

Annihilation of nematic point defects: Pre-collision and post-collision evolution

The annihilation of the nematic hedgehog and anti-hedgehog within an infinite cylinder of radius R is studied. The semi-microscopic lattice-type model and Brownian molecular dynamics are used. We distinguish among the i) early pre-collision, ii) late pre-collision, iii) early post-collision, and iv) late post-collision stages. In the pre-collision stage our results agree qualitatively with the existing experimental observations and also continuum-type simulations. The core of each defect exhibits a ring-like structure, where the ring axis is set perpendicular to the cylinder symmetry axis. For ξ⁽⁰⁾_d/(2R) > 1 the interaction between defects is negligible, where ξ⁽⁰⁾_d describes the initial separation of defects. Consequently, the defects annihilate within the simulation time window for ξ⁽⁰⁾_d/(2R) < 1. For close enough defects their separation scales as ξ_d (t_c - t)^0.4±0.1, where t_c stands for the collision time. In elastically anisotropic medium the hedgehog is faster than the anti-hedgehog. In the early pre-collision stage the defects can be treated as point-like particles, possessing inherent core structure, that interact via the nematic director field. In the late pre-collision stage the cores reflect the interaction between defects. After the collision a charge-less ring structure is first formed. In the early post-collision stage the ring adopts an essentially untwisted circular structure of the radius ξ_r. In the late post-collision stage we observe two qualitatively different scenarios. For μ = ξ_r/R < μ_c ∼ 0.25 the ring collapses leading to the escaped radial equilibrium structure. For μ > μ_c the chargeless ring triggers the nucleation growth into the planar polar structure with line defects.     

Interaction force between incompatible star-polymers in dilute solution

We consider a low-density assembly of spherical colloids, such that each is clothed by L end-grafted chemically incompatible polymer chains either of types A or B. These are assumed to be dissolved in a good common solvent. We assume that colloids are of small size to be considered as star-polymers. Two adjacent star-polymers A and B interact through a force F originating from both excluded-volume effects and chemical mismatch between unlike monomers. Using a method developed by Witten and Pincus (Macromolecules 19, 2509 (1986)) in the context of star-polymers of the same chemical nature, we determine exactly the force F as a function of the center-to-center distance h. We find that this force is the sum of two contributions F _e and F _s. The former, that results from the excluded volume, decays as F _e∼A _L h ^-1, with the L -dependent universal amplitude A _L∼L ^3/2. While the second, which comes from the chemical mismatch, decays more slowly as F _s∼χB _L h ^{-1 - τ}, where τ is a critical exponent whose value is found to be τ 0.40, and χ is the standard Flory interaction parameter. We find that the corresponding L-dependent universal amplitude is B _L∼L ^{3 + τ /2}. Theses forces are comparable near the cores of two adjacent star-polymers, i.e. for h∼h _c∼a (a is the monomer size). Finally, for two star-polymers of the same chemical nature (A or B), the force F that simply results from excluded-volume effects coincides exactly with F _e, and then the known result is recovered. Received 2 October 2000 and Received in final form 24 January 2001