Dielectric Susceptibility and Heat Capacity of Ultra-Cold Glasses in Magnetic Field

Recent experiments demonstrated unexpected, even intriguing properties of certain glassy materials in magnetic field at low temperatures. We have studied the magnetic field dependence of the static dielectric susceptibility and the heat capacity of glasses at low temperatures. We present a theory in which we consider the coupling of the tunnelling motion to nuclear quadrupoles in order to evaluate the static dielectric susceptibility. In the limit of weak magnetic field we find the resonant part of the susceptibility increasing like $B^2$ while for the large magnetic field it behaves as 1/B. In the same manner we consider the coupling of the tunnelling motion to nuclear quadrupoles and angular momentum of tunnelling particles in order to find the heat capacity. Our results show the Schotky peak for the angular momentum part, and $B^2$ dependence for nuclear quadrupoles part of heat capacity, respectively. We discuss whether or not this approach can provide a suitable explanation for such magnetic properties.Comment: 10 pages, 1 figur

Elastic response of [111]-tunneling impurities

We study the dynamic response of a [111] quantum impurity, such as lithium or cyanide in alkali halides, with respect to an external field coupling to the elastic quadrupole moment. Because of the particular level structure of a eight-state system on a cubic site, the elastic response function shows a biexponential relaxation feature and a van Vleck type contribution with a resonance frequency that is twice the tunnel frequency $\Delta/\hbar$. This basically differs from the dielectric response that does not show relaxation. Moreover, we show that the elastic response of a [111] impurity cannot be reduced to that of a two-level system. In the experimental part, we report on recent sound velocity and internal friction measurements on KCl doped with cyanide at various concentrations. At low doping (45 ppm) we find the dynamics of a single [111] impurity, whereas at higher concentrations (4700 ppm) the elastic response rather indicates strongly correlated defects. Our theoretical model provides a good description of the temperature dependence of $\delta v/v$ and $Q^{-1}$ at low doping, in particular the relaxation peaks, the absolute values of the amplitude, and the resonant contributions. From our fits we obtain the value of the elastic deformation potential $\gamma_t=0.192$ eV.Comment: 19 pages, 5 figure

On the theory of resonant susceptibility of dielectric glasses in magnetic field

The anomalous magnetic field dependence of dielectric properties of insulating glasses in the temperature interval $10mK<T<50mK$ is considered. In this temperature range, the dielectric permittivity is defined by the resonant contribution of tunneling systems. The external magnetic field regulates nuclear spins of tunneling atoms. This regulation suppresses a nuclear quadrupole interaction of these spins with lattice and, thus, affects the dielectric response of tunneling systems. It is demonstrated that in the absence of an external magnetic field the nuclear quadrupole interaction $b$ results in the correction to the permittivity $\delta\chi\sim| b| /T$ in the temperature range of interest. An application of a magnetic field results in a sharp increase of this correction approximately by a factor of two when the Zeeman splitting $m$ approaches the order of $| b|$. Further increase of the magnetic field results in a relatively smooth decrease in the correction until the Zeeman splitting approaches the temperature. This smooth dependence results from tunneling accompanied by a change of the nuclear spin projection. As the magnetic field surpasses the temperature, the correction vanishes. The results obtained in this paper are compared with experiment. A new mechanism of the low temperature nuclear spin-lattice relaxation in glasses is considered.Comment: 9 Pages, 5 Figures, To be submitted to the Physical Review B, please send comment

Four-well tunneling states and elastic response of clathrates

We present resonant ultrasound elastic constant measurements of the clathrate compounds Eu8Ga16Ge30 and Sr8Ga16Ge30. The elastic response of the Eu clathrate provides clear evidence for the existence of a new type of four-well tunneling states, described by two nearly degenerate four level systems (FLS). The FLS's are closely linked with the fourfold split positions of Eu known from neutron diffraction density profiles. Using a realistic potential we estimate the tunneling frequencies and show that the energy gap between the two FLS's is of the same order as the Einstein oscillator frequency. This explains why the observed harmonic oscillator type specific heat is not modified by tunneling states. In addition the quadrupolar interaction of FLS's with elastic strains explains the pronounced depression observed in elastic constant measurements. In the case of the Sr clathrate, we show that the shallow dip in the elastic constant c44 is explained using the same type of quadrupolar interaction with a soft Einstein mode instead of a FLS.Comment: 4 pages, 4 figures; accepted for publication in Physical Review Letter

Interacting quantum rotors in oxygen-doped germanium

We investigate the interaction effect between oxygen impurities in crystalline germanium on the basis of a quantum rotor model. The dipolar interaction of nearby oxygen impurities engenders non-trivial low-lying excitations, giving rise to anomalous behaviors for oxygen-doped germanium (Ge:O) below a few degrees Kelvin. In particular, it is theoretically predicted that Ge:O samples with oxygen-concentration of 10$^{17-18}$cm$^{-3}$ show (i) power-law specific heats below 0.1 K, and (ii) a peculiar hump in dielectric susceptibilities around 1 K. We present an interpretation for the power-law specific heats, which is based on the picture of local double-well potentials randomly distributed in Ge:O samples.Comment: 13 pages, 11 figures; to be published in Phys. Rev.

Effect of Nuclear Quadrupole Interaction on the Relaxation in Amorphous Solids

Recently it has been experimentally demonstrated that certain glasses display an unexpected magnetic field dependence of the dielectric constant. In particular, the echo technique experiments have shown that the echo amplitude depends on the magnetic field. The analysis of these experiments results in the conclusion that the effect seems to be related to the nuclear degrees of freedom of tunneling systems. The interactions of a nuclear quadrupole electrical moment with the crystal field and of a nuclear magnetic moment with magnetic field transform the two-level tunneling systems inherent in amorphous dielectrics into many-level tunneling systems. The fact that these features show up at temperatures $T<100mK$, where the properties of amorphous materials are governed by the long-range $R^{-3}$ interaction between tunneling systems, suggests that this interaction is responsible for the magnetic field dependent relaxation. We have developed a theory of many-body relaxation in an ensemble of interacting many-level tunneling systems and show that the relaxation rate is controlled by the magnetic field. The results obtained correlate with the available experimental data. Our approach strongly supports the idea that the nuclear quadrupole interaction is just the key for understanding the unusual behavior of glasses in a magnetic field.Comment: 18 pages, 9 figure

Cubic Defects: Comparing the Eight-State-System with its Two-Level-Approximation

Substitutional defects in a cubic symmetry (such as a lithium defect in a KCl host crystal) can be modeled appropriately by an eight-state-system. Usually this tunneling degree of freedom is approximated by a two-level-system. We investigate the observable differences between the two models in three contexts. First we show that the two models predict different relations between the temperature dependence of specific heat and static susceptibility. Second we demonstrate that in the presence of external forces (pressure and electric field) the eight-state-system shows features that cannot be understood within the framework of the two-level-approximation. In this context we propose an experiment for measuring the parameter for tunneling along the face diagonal. Finally we discuss the differences between the models appearing for strongly coupled pairs. Geometric selection rules and particular forms of asymmetry lead to clear differences between the two models.Comment: 19 pages, Latex, submitted to J. of Phys., some small supplement

Evidence for Magnetic Field Induced Changes of the Phase of Tunneling States: Spontaneous Echoes in (KBr)1−x_{1-x}(KCN)x_x in Magnetic Fields

Recently, it has been discovered that in contrast to expectations the low-temperature dielectric properties of some multi-component glasses depend strongly on magnetic fields. In particular, the low-frequency dielectric susceptibility and the amplitude of coherent polarization echoes show striking non-monotonic magnetic field dependencies. The low-temperature dielectric response of these materials is governed by atomic tunneling systems. We now have investigated the coherent properties of tunneling states in a crystalline host in magnetic fields up to 230$$mT. Two-pulse echo experiments have been performed on a KBr crystal containing about 7.5% CN$^-$. Like in glasses, but perhaps even more surprising in the case of a crystalline system, we observe a very strong magnetic field dependence of the echo amplitude. Moreover, for the first time we have direct evidence that magnetic fields change the phase of coherent tunneling systems in a well-defined way. We present the data and discuss the possible origin of this intriguing effect.Comment: 4 pages, 3 figures, submitted to PR

Free energy of colloidal particles at the surface of sessile drops

The influence of finite system size on the free energy of a spherical particle floating at the surface of a sessile droplet is studied both analytically and numerically. In the special case that the contact angle at the substrate equals $\pi/2$ a capillary analogue of the method of images is applied in order to calculate small deformations of the droplet shape if an external force is applied to the particle. The type of boundary conditions for the droplet shape at the substrate determines the sign of the capillary monopole associated with the image particle. Therefore, the free energy of the particle, which is proportional to the interaction energy of the original particle with its image, can be of either sign, too. The analytic solutions, given by the Green's function of the capillary equation, are constructed such that the condition of the forces acting on the droplet being balanced and of the volume constraint are fulfilled. Besides the known phenomena of attraction of a particle to a free contact line and repulsion from a pinned one, we observe a local free energy minimum for the particle being located at the drop apex or at an intermediate angle, respectively. This peculiarity can be traced back to a non-monotonic behavior of the Green's function, which reflects the interplay between the deformations of the droplet shape and the volume constraint.Comment: 24 pages, 19 figure

Effective interactions of colloids on nematic films

The elastic and capillary interactions between a pair of colloidal particles trapped on top of a nematic film are studied theoretically for large separations $d$. The elastic interaction is repulsive and of quadrupolar type, varying as $d^{-5}$. For macroscopically thick films, the capillary interaction is likewise repulsive and proportional to $d^{-5}$ as a consequence of mechanical isolation of the system comprised of the colloids and the interface. A finite film thickness introduces a nonvanishing force on the system (exerted by the substrate supporting the film) leading to logarithmically varying capillary attractions. However, their strength turns out to be too small to be of importance for the recently observed pattern formation of colloidal droplets on nematic films.Comment: 13 pages, accepted by EPJ