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Rolf Schilling

Publications and source records attributed to Rolf Schilling.

35 records · Page 2Linked to original sources
arXiv2010

Glass transition of hard spheres in high dimensions

We have investigated analytically and numerically the liquid-glass transition of hard spheres for dimensions $d\to \infty $ in the framework of mode-coupling theory. The numerical results for the critical collective and self nonergodicity parameters $f_{c}(k;d) $ and $f_{c}^{(s)}(k;d) $ exhibit non-Gaussian $k$ -dependence even up to $d=800$. $f_{c}^{(s)}(k;d) $ and $f_{c}(k;d) $ differ for $k\sim d^{1/2}$, but become identical on a scale $k\sim d$, which is proven analytically. The critical packing fraction $ϕ_{c}(d) \sim d^{2}2^{-d}$ is above the corresponding Kauzmann packing fraction $ϕ_{K}(d)$ derived by a small cage expansion. Its quadratic pre-exponential factor is different from the linear one found earlier. The numerical values for the exponent parameter and therefore the critical exponents $a$ and $b$ depend on $d$, even for the largest values of $d$.

cond-mat.soft↗
arXiv2007

Event-Driven Simulation of the Dynamics of Hard Ellipsoids

We introduce a novel algorithm to perform event-driven simulations of hard rigid bodies of arbitrary shape, that relies on the evaluation of the geometric distance. In the case of a monodisperse system of uniaxial hard ellipsoids,we perform molecular dynamics simulations varying the aspect-ratio X0 and the packing fraction phi. We evaluate the translational Dtrans and the rotational Drot diffusion coefficient and the associated isodiffusivity lines in the phi-X0 plane. We observe a decoupling of the translational and rotational dynamics which generates an almost perpendicular crossing of the Dtrans and Drot isodiffusivity lines. While the self intermediate scattering function exhibits stretched relaxation, i.e. glassy dynamics, only for large phi and X0 about equals to 1, the second order orientational correlator C2(t) shows stretching only for large and small X0 values. We discuss these findings in the context of a possible pre-nematic order driven glass transition.

cond-mat.soft↗
arXiv2006

Energy landscape properties studied by symbolic sequences

We investigate a classical lattice system with $N$ particles. The potential energy $V$ of the scalar displacements is chosen as a $ϕ^4$ on-site potential plus interactions. Its stationary points are solutions of a coupled set of nonlinear equations. Starting with Aubry's anti-continuum limit it is easy to establish a one-to-one correspondence between the stationary points of $V$ and symbolic sequences $\bmσ = (σ_1,...,σ_N)$ with $σ_n=+,0,-$. We prove that this correspondence remains valid for interactions with a coupling constant $ε$ below a critical value $ε_c$ and that it allows the use of a ''thermodynamic'' formalism to calculate statistical properties of the so-called ``energy landscape'' of $V$. This offers an explanation why topological quantities of $V$ may become singular, like in phase transitions. Particularly, we find the saddle index distribution is maximum at a saddle index $n_s^{max}=1/3$ for all $ε< ε_c$. Furthermore there exists an interval ($v^*,v_{max}$) in which the saddle index $n_s$ as function of average energy $\bar{v}$ is analytical in $\bar{v}$ and it vanishes at $v^*$, above the ground state energy $v_{gs}$, whereas the average saddle index $\bar{n}_s$ as function of energy $v$ is highly nontrivial. It can exhibit a singularity at a critical energy $v_c$ and it vanishes at $v_{gs}$, only. Close to $v_{gs}, \bar{n}_s(v)$ exhibits power law behavior which even holds for noninteracting particles.

cond-mat.dis-nn↗
arXiv2005

Molecular Correlation Functions for Uniaxial Ellipsoids in the Isotropic State

We perform event-driven molecular dynamics simulations of a system composed by uniaxial hard ellipsoids for different values of the aspect-ratio and packing fraction . We compare the molecular orientational-dependent structure factors previously calculated within the Percus-Yevick approximation with the numerical results. The agreement between theoretical and numerical results is rather satisfactory. We also show that, for specific orientational quantities, the molecular structure factors are sensitive to the particle shape and can be used to distinguish prolate from oblate ellipsoids. A first-order theoretical expansion around the spherical shape and a geometrical analysis of the configurations confirms and explains such an observation.

cond-mat.soft↗
arXiv2005

Butterfly hysteresis curve is a signature of adiabatic Landau-Zener transition

We stress that the so-called butterfly hysteresis curves observed in dynamical magnetization measurements on systems of low-spin magnetic molecules such as V-15 and V-6 are a signature of adiabatic Landau-Zener transitions rather than that of a phonon bottleneck. We investigate the magnetization dynamics analytically with the help of a simple relaxation theory in the basis of the adabatic energy levels of the spin 1/2, to a qualitative accordance with experimental observations. In particular, reversible behavior is found near zero field, the corresponding susceptibility being bounded by the equilibrium and adiabatic susceptibilities from below and above, respectively.

cond-mat.stat-mech↗
arXiv2005

Microscopic theory of glassy dynamics and glass transition for molecular crystals

We derive a microscopic equation of motion for the dynamical orientational correlators of molecular crystals. Our approach is based upon mode coupling theory. Compared to liquids we find four main differences: (i) the memory kernel contains Umklapp processes, (ii) besides the static two-molecule orientational correlators one also needs the static one-molecule orientational density as an input, where the latter is nontrivial, (iii) the static orientational current density correlator does contribute an anisotropic, inertia-independent part to the memory kernel, (iv) if the molecules are assumed to be fixed on a rigid lattice, the tensorial orientational correlators and the memory kernel have vanishing l,l'=0 components. The resulting mode coupling equations are solved for hard ellipsoids of revolution on a rigid sc-lattice. Using the static orientational correlators from Percus-Yevick theory we find an ideal glass transition generated due to precursors of orientational order which depend on X and p, the aspect ratio and packing fraction of the ellipsoids. The glass formation of oblate ellipsoids is enhanced compared to that for prolate ones. For oblate ellipsoids with X <~ 0.7 and prolate ellipsoids with X >~ 4, the critical diagonal nonergodicity parameters in reciprocal space exhibit more or less sharp maxima at the zone center with very small values elsewhere, while for prolate ellipsoids with 2 <~ X <~ 2.5 we have maxima at the zone edge. The off-diagonal nonergodicity parameters are not restricted to positive values and show similar behavior. For 0.7 <~ X <~ 2, no glass transition is found. In the glass phase, the nonergodicity parameters show a pronounced q-dependence.

cond-mat.soft↗
arXiv2003

Ornstein-Zernike equation and Percus-Yevick theory for molecular crystals

We derive the Ornstein-Zernike equation for molecular crystals of axially symmetric particles and apply the Percus-Yevick approximation to this system. The one-particle orientational distribution function has a nontrivial dependence on the orientation and is needed as an input. Despite some differences, the Ornstein-Zernike equation for molecular crystals has a similar structure as for liquids. We solve both equations for hard ellipsoids on a sc lattice. Compared to molecular liquids, the tensorial orientational correlators exhibit less structure. However, depending on the lengths a and b of the rotation axis and the perpendicular axes of the ellipsoids, different behavior is found. For oblate and prolate ellipsoids with b >= 0.35 (units of the lattice constant), damped oscillations in distinct directions of direct space occur for some correlators. They manifest themselves in some correlators in reciprocal space as a maximum at the Brillouin zone edge, accompanied by maxima at the zone center for other correlators. The oscillations indicate alternating orientational fluctuations, while the maxima at the zone center originate from nematic-like orientational fluctuations. For a <= 2.5 and b <= 0.35, the oscillations are weaker. For a >= 3.0 and b <= 0.35, no oscillations occur any longer. For many of the correlators in reciprocal space, an increase of a at fixed b leads to a divergence at the zone center q = 0, consistent with nematic-like long range fluctuations, and for some oblate and prolate systems with b ~< 1.0 a simultaneous tendency to divergence of few other correlators at the zone edge is observed. Comparison with correlators from MC simulations shows satisfactory agreement. We also obtain a phase boundary for order-disorder transitions.

cond-mat.stat-mech↗
arXiv2002

Glass transition in systems without static correlations: a microscopic theory

We present a first step toward a microscopic theory for the glass transition in systems with trivial static correlations. As an example we have chosen N infinitely thin hard rods with length L, fixed with their centers on a periodic lattice with lattice constant a. Starting from the N-rod Smoluchowski equation we derive a coupled set of equations for fluctuations of reduced k-rod densities. We approximate the influence of the surrounding rods onto the dynamics of a pair of rods by introduction of an effective rotational diffusion tensor D and in this way we obtain a self-consistent equation for D. This equation exhibits a feedback mechanism leading to a slowing down of the relaxation. It involves as an input the Laplace transform v_0(l/r) at z=0, l=L/a, of a torque-torque correlator of an isolated pair of rods with distance R=ar. Our equation predicts the existence of a continuous ergodicity-breaking transition at a critical length l_c=L_c/a. To estimate the critical length we perform an approximate analytical calculation of v_0(l/r) based on a variational approach and obtain l_c^{var}=5.68, 4.84 and 3.96 for an sc, bcc and fcc lattice. We also evaluate v_0(l/r) numerically exactly from a two-rod simulation. The latter calculation leads to l_c^{num}=3.45, 2.78 and 2.20 for the corresponding lattices. Close to l_c the rotational diffusion constant decreases as D(l) ~ (l_c - l)^γwith γ=1 and a diverging time scale t_ε~ |l_c - l|^{-δ}, δ=2, appears. On this time scale the t- and l-dependence of the 1-rod density is determined by a master function depending only on t/t_ε. In contrast to present microscopic theories our approach predicts a glass transition despite the absence of any static correlations.

cond-mat.soft↗
arXiv2002

Microscopic theory for the glass transition in a system without static correlations

We study the orientational dynamics of infinitely thin hard rods of length L, with the centers-of-mass fixed on a simple cubic lattice with lattice constant a.We approximate the influence of the surrounding rods onto dynamics of a pair of rods by introducing an effective rotational diffusion constant D(l),l=L/a. We get D(l) ~ [1-v(l)], where v(l) is given through an integral of a time-dependent torque-torque correlator of an isolated pair of rods. A glass transition occurs at l_c, if v(l_c)=1. We present a variational and a numerically exact evaluation of v(l).Close to l_c the diffusion constant decreases as D(l) ~ (l_c-l)^γ, with γ=1. Our approach predicts a glass transition in the absence of any static correlations, in contrast to present form of mode coupling theory.

cond-mat.soft↗
arXiv1999

Neutron scattering and molecular correlations in a supercooled liquid

We show that the intermediate scattering function $S_n(q,t)$ for neutron scattering (ns) can be expanded naturely with respect to a set of molecular correlation functions that give a complete description of the translational and orientational two-point correlations in the liquid. The general properties of this expansion are discussed with special focus on the $q$-dependence and hints for a (partial) determination of the molecular correlation functions from neutron scattering results are given. The resulting representation of the static structure factor $S_n(q)$ is studied in detail for a model system using data from a molecular dynamics simulation of a supercooled liquid of rigid diatomic molecules. The comparison between the exact result for $S_n(q)$ and different approximations that result from a truncation of the series representation demonstrates its good convergence for the given model system. On the other hand it shows explicitly that the coupling between translational (TDOF) and orientational degrees of freedom (ODOF) of each molecule and rotational motion of different molecules can not be neglected in the supercooled regime.Further we report the existence of a prepeak in the ns-static structure factor of the examined fragile glassformer, demonstrating that prepeaks can occur even in the most simple molecular liquids. Besides examining the dependence of the prepeak on the scattering length and the temperature we use the expansion of $S_n(q)$ into molecular correlation functions to point out intermediate range orientational order as its principle origin.

cond-mat.stat-mech↗
arXiv1998

Neutron scattering in molecular liquids: Influence of orientational degrees of freedom and the prepeak in a fragile glass former

The intermediate scattering function S(q,t) for neutron scattering is expanded with respect to a complete set of correlation functions which describe the dynamical correlations in a molecular liquid. For the static ns-structure factor S(q) of a system of diatomic molecules the results of the expansion are compared with the exact results from a MD-imulation and it is shown that the Sears-expansion, which is commonly used to interpret such data, fails in the supercooled regime. The representation for S(q) is used to draw conclusions about the q-dependence and especially the origin of the prepeak.

cond-mat.soft↗
arXiv1998

Nonergodicity parameters for a molecular liquid: A comparison between mode coupling theory and simulation

We apply the mode coupling theory (MCT) which was recently worked out for molecular liquids to a liquid of diatomic, rigid molecules. Using the static correlators from a molecular dynamics simulation, we have solved the MCT-equations for the nonergodicity parameters within two approcimation schemes. We find that the critical temperature from our calculation underestimates the simulation result. The q-dependence of the critical nonergodicity parameter is well reproduced.

cond-mat.dis-nn↗
arXiv1998

Test of the semischematic model for a liquid of linear molecules

We apply to a liquid of linear molecules the semischematic mode-coupling model, previously introduced to describe the center of mass (COM) slow dynamics of a network-forming molecular liquid. We compare the theoretical predictions and numerical results from a molecular dynamics simulation, both for the time and the wave-vector dependence of the COM density-density correlation function. We discuss the relationship between the presented analysis and the results from an approximate solution of the equations from molecular mode-coupling theory [R. Schilling and T. Scheidsteger, Phys. Rev. E 56 2932 (1997)].

cond-mat.soft↗
arXiv1997

Test of mode coupling theory for a supercooled liquid of diatomic molecules.I. Translational degrees of freedom

A molecular dynamics simulation is performed for a supercooled liquid of rigid diatomic molecules. The time-dependent self and collective density correlators of the molecular centers of mass are determined and compared with the predictions of the ideal mode coupling theory (MCT) for simple liquids. This is done in real as well as in momentum space. One of the main results is the existence of a unique transition temperature T_c, where the dynamics crosses over from an ergodic to a quasi-nonergodic behavior. The value for T_c agrees with that found earlier for the orientational dynamics within the error bars. In the beta- regime of MCT the factorization of space- and time dependence is satisfactorily fulfilled for both types of correlations. The first scaling law of ideal MCT holds in the von Schweidler regime, only, since the validity of the critical law can not be confirmed, due to a strong interference with the microscopic dynamics. In this first scaling regime a consistent description within ideal MCT emerges only, if the next order correction to the asymptotic law is taken into account. This correction is almost negligible for q=q_max, the position of the main peak in the static structure factor S(q), but becomes important for q=q_min, the position of its first minimum. The second scaling law, i.e. the time-temperature superposition principle, holds reasonably well for the self and collective density correlators and different values for q. The alpha-relaxation times tau_q^(s) and tau_q follow a power law in T-T_c over 2 -- 3 decades. The corresponding exponent gamma is weakly q-dependent and is around 2.55. This value is in agreement with the one predicted by MCT from the value of the von Schweidler exponent but at variance with the corresponding exponent gamma

cond-mat.stat-mech↗
arXiv1997

Test of mode coupling theory for a supercooled liquid of diatomic molecules. II. q-dependent orientational correlators

Using molecular dynamics computer simulations we study the dynamics of a molecular liquid by means of a general class of time-dependent correlators S_{ll'}^m(q,t) which explicitly involve translational (TDOF) and orientational degrees of freedom (ODOF). The system is composed of rigid, linear molecules with Lennard- Jones interactions. The q-dependence of the static correlators S_{ll'}^m(q) strongly depend on l, l' and m. The time dependent correlators are calculated for l=l'. A thorough test of the predictions of mode coupling theory (MCT) is performed for S_{ll}^m(q,t) and its self part S_{ll}^{(s)m}(q,t), for l=1,..,6. We find a clear signature for the existence of a single temperature T_c, at which the dynamics changes significantly. The first scaling law of MCT, which involves the critical correlator G(t), holds for l>=2, but no critical law is observed. Since this is true for the same exponent parameter lambda as obtained for the TDOF, we obtain a consistent description of both, the TDOF and ODOF, with the exception of l=1. This different behavior for l \ne 1 and l=1 can also be seen from the corresponding susceptibilities (chi'')_{ll}^m(q,omega) which exhibit a minimum at about the same frequency omega_{min} for all q and all l \ne 1, in contrast to (chi'')_{11}^m(q,omega) for which omega'_{min} approx 10 omega_{min} . The asymptotic regime, for which the first scaling law holds, shrinks with increasing l. The second scaling law of MCT (time-temperature superposition principle) is reasonably fulfilled for l \ne 1 but not for l=1. Furthermore we show that the q- and (l,m)-dependence of the self part approximately factorizes, i.e. S_{ll}^{(s)m}(q,t) \cong C_l^{(s)}(t) F_s(q,t) for all m.

cond-mat.stat-mech↗
arXiv1997

Dynamics of the rotational degrees of freedom in a supercooled liquid of diatomic molecules

Using molecular dynamics computer simulations, we investigate the dynamics of the rotational degrees of freedom in a supercooled system composed of rigid, diatomic molecules. The interaction between the molecules is given by the sum of interaction-site potentials of the Lennard-Jones type. In agreement with mode-coupling theory (MCT), we find that the relaxation times of the orientational time correlation functions C_1^(s), C_2^(s) and C_1 show at low temperatures a power-law with the same critical temperature T_c, and which is also identical to the critical temperature for the translational degrees of freedom. In contrast to MCT we find, however, that for these correlators the time-temperature superposition principle does not hold well and that also the critical exponent gamma depends on the correlator. We also study the temperature dependence of the rotational diffusion constant D_r and demonstrate that at high temperatures D_r is proportional to the translational diffusion constant D and that when the system starts to become supercooled the former shows an Arrhenius behavior whereas the latter exhibits a power-law dependence. We discuss the origin for the difference in the temperature dependence of D (or the relaxation times of C_l^(s) and D_r. Finally we present results which show that at low temperatures 180 degree flips of the molecule are an important component of the relaxation dynamics for the orientational degrees of freedom.

cond-mat.stat-mech↗