Diffusion of Impurity Excitations in Superfluid and Solid 3He–4He Mixtures

Starting from the system of linearized kinetic equations, the exact expressions for the spin and mass diffusion coefficients and thermal diffusion ratio in quantum mixtures of helium isotopes with any degree of degeneration is obtained. From the general expression the various limiting expressions have been obtained, which are determined by various relations between collision rates of quasiparticles. The results of the calculations are compared with available experimental data. It is shown that in the low-temperature region, where an impuriton gas is one-component, the relaxation of concentration of ³ He in superfluid ³ He– ⁴ He mixtures is determined by the acoustic and dissipative collective modes with an effective diffusion coefficient. From the general relation, the expression for a spin diffusion coefficient in solid ³ He– ⁴ He quantum mixtures is derived. The comparison of the results obtained with the experimental data makes it possible to find a numerical value for the width of the impuriton energy zone.     

3He Impurity Effects on the Growth Kinetics of 4He Crystals

We report the growth kinetics of the⁴He crystals with a small amount of³He impurities around 0.8 K. The growth resistance was measured using the response of the charged interface with respect to an externally applied voltage. In 5 ppm and 10 ppm³He mixtures, it is found that (1) the relaxation process can be expressed as an exponential behavior, (2) the growth resistance becomes larger compared to pure⁴He and does not have a strong³He concentration dependence, and (3) the temperature dependence of the growth resistance is much the same as pure⁴He. We discuss several possible explanations of the present experiment.     

Effects of 3He Impurity on the Non-classical Rotational Inertia of Solid 4He Studied by Double Resonance Torsional Oscillator

We have carried out systematic measurements of the ³He-impurity effect using a compound torsional pendulum, which allows probing “non-classical rotational inertia” (NCRI) of the identical solid ⁴He sample at two different frequencies at 495 Hz and 1172 Hz. The measurements have shown significant differences in the temperature dependence of the NCRI signal as well as the energy dissipation peak positions between the two frequencies. The NCRI fraction derived from the higher frequency mode is greater than that derived from the lower frequency mode at all temperatures. The normalized NCRI fraction shows that T ₅₀ (≡temperature at which NCRI fraction decreases to 50% of the maximum) is greater in the higher frequency mode by ～9, 18, 30 and 35 mK when the nominal ³He impurity added is 0.3, 6, 12 and 25 ppm, respectively. The systematic changes in the inverse quality factor (Q ^?1) were also measured at the same ³He-impurity concentrations.     

Acoustic Properties of Solid 4He in the Limit of Zero Impurity

We have studied the elasticity of solid ⁴He in relation with its possible supersolidity. For this we have measured acoustic resonance frequencies in a 1 cm³ cell filled either with polycrystals or with single crystals of ⁴He. We have observed a large stiffening at low temperature as first observed by Day and Beamish in polycrystals. The ³He impurity content has been varied from 300 ppb to 0.4 ppb. When kept in equilibrium with liquid helium, single crystals should be impurity free. In these crystals, a large stiffening is observed, which should not be the result of the pinning of dislocations by impurities.     

4He Impurity Effect on the Positive Ion Mobility in Liquid 3He

The behaviour of ⁴ He impurities has been investigated through positive ion mobility measurements in liquid ³ He at milliKelvin temperatures. In spite of the enormous surface area of the cell, the influence of ⁴ He lasted for hundreds of hours at temperatures of 20 mK. However below 10 mK, the ⁴ He impurities were quickly frozen out on the cell walls and we were free from the impurity problem. Nevertheless the multiple ion signal occasionally appeared even at a few mK, although it disappeared for a number of ionization pulses.     

Response of a Mechanical Oscillator in Solid 4He

We present the first measurements of the response of a mechanical oscillator in solid ⁴He. We use a lithium niobate tuning fork operating in its fundamental resonance mode at a frequency of around 30 kHz. Measurements in solid ⁴He were performed close to the melting pressure. The tuning fork resonance shows substantial frequency shifts on cooling from around 1.5 K to below 10 mK. The response shows an abrupt change at the bcc-hcp transition. At low temperatures, below around 100 mK, the resonance splits into several overlapping resonances.     

Variational Study of a 3He Impurity Near a 4He Vortex Core

The system of kinetic equations for distribution functions of impurity excitations in solid 3He–⁴ He mixtures in the presence of phonons is solved. The results obtained allows us to calculate the spin diffusion coefficient of ³ He–⁴ He quantum crystals. The found expression differs from the results of the previous theoretical studies. A comparison of the obtained diffusion coefficient with experimental data makes it possible to determine the numerical values of the energy band width of impurity excitations.     

Vortex-Loops and Solid Nucleation in Superfluid 4He and 3He

We propose a new model for the nature of the nucleation of solid from the superfluid phases of ⁴He and ³He. Unique to the superfluid phases the solid nucleation involves an extremely fast solidification front. We depart from the usual quasi-static treatment of solid nucleation by proposing that the nucleation of a solid seed is helped by the simultaneous nucleation of vortex-loops in the superfluid around it. It is the composite entity which is nucleated out of the over-pressurized liquid. This occurs when the local release of pressure creates a velocity field in the superfluid which in turn facilitates the nucleation of vortex-loops. The kinetic energy gain of this process balances the surface tension, as the solid surface is quickly covered by many vortex-loops (hairy snow-ball). We show that this scenario gives good agreement with many experiments on heterogeneous nucleation, where the energy barrier is found to differ with the classical theory of homogeneous nucleation by 8 orders of magnitude. We propose several experiments that could show the involvement of vortices with solid nucleation.     

Dynamical Response of Liquid 3He Films Adsorbed on Solid Substrates

Within the general framework of linear response theory, we investigate the excitation spectrum of ³He films adsorbed on substrates. Starting from the quasiparticle spectrum and the effective interaction derived in a finite range density functional scheme, we analyze the properties of the particle-hole (ph) excitations as well as the collective modes in the Random Phase Approximation. On the one hand, the most important features of the ph spectrum, originated in the band structure of the single particle spectrum together with the fermionic character of the quasiparticles, are clearly exhibited when the free response to a probe parallel or transverse to the film is considered. On the other hand, for any film, the collective spectrum presents various branches which, in many situations, can be associated with predominantly intraband longitudinal transitions or with almost pure interband transitions. Analyzing the RPA response of a monolayer on substrates of very different adsorbing power (cesium and graphite) we can interpret the nature of the existing collective excitations and determine the influence of the geometrical features of the film on the effective quasiparticle interaction responsible of these oscillations.     

The Glassy Response of Solid 4He to Torsional Oscillations

We calculated the glassy response of solid ⁴He to torsional oscillations assuming a phenomenological glass model. Making only a few assumptions about the distribution of glassy relaxation times in a small subsystem of otherwise rigid solid ⁴He, we can account for the magnitude of the observed period shift and concomitant dissipation peak in several torsion oscillator experiments. The implications of the glass model for solid ⁴He are threefold: (1) The dynamics of solid ⁴He is governed by glassy relaxation processes. (2) The distribution of relaxation times varies significantly between different torsion oscillator experiments. (3) The mechanical response of a torsion oscillator does not require a supersolid component to account for the observed anomaly at low temperatures, though we cannot rule out its existence.     

Kinetics of Liquid 3He Droplets in Solid 4He Matrix

Precise measurements of pressure in the crystal at constant volume were used to obtain the data on growth and dissolution kinetics of liquid ³ He droplets formed as a result of isotopic phase separation of solid ³ He- ⁴ He Mixtures. We studied several crystals with an initial ³ He concentration of 2.05% in the pressure range of 26–27 bar. It is shown that the growth of the liquid droplets during the stepwise cooling of the two-phase crystal is correctly described by the superposition of two exponential processes: diffusion decomposition with a small time constant and strain relaxation with a big time constant. The strain layer near the droplet boundaries is due to a great difference in molar volume between the droplets and the matrix, and leads to a plastic deformation of the matrix and to a non-equilibrium ³ He concentration in the matrix. Under such conditions quantum diffusion is significantly suppressed and ³ He atom transport occurs only as the strain is relaxed.     

Quartz Oscillator Study of Monolayer 4He and 3He - 4He Mixture Films Adsorbed on Solid H2

The superfluid transition in submonolayer and monolayer ⁴ He films and ³ He - ⁴ He mixture films on solid H ₂ has been studied using a quartz crystal microbalance technique. Kosterlitz-Thouless (KT) transitions were observed in submonolayer ⁴ He films with density greater than 0.062 ± 0.002 Å ^–2 . We determine a binding energy of ⁴ He to 0.241 Å ^–2 H ₂ of –15.7 K in the. presence of 1 monolayer of ⁴ He. At several ⁴ He coverages, a range of submonolayer ³ He coverages was studied (n ₃ 0.0567 Å ^–2 ). With each increase in the ³ He coverage, the KT transition temperature decreased. For the higher coverage mixture films studied (n ₄ 0.0726 Å ^–2 ) we observed an apparent second decoupling of the film from the quartz oscillator frequency in addition to the KT transition. We have studied the. coverage dependence of this new feature.     

Melting and Crystallization of 3He Inclusions in Two-phase Solid 3He-4He Mixtures

The peculiar features of the phase diagram for the ³ He- ⁴ He system make it possible to melt the ³ He inclusions formed during phase separation of the mixture by further cooling and to crystallize them in subsequent heating. The kinetics of these processes is studied on a sample with a molar volume of 20.54 cm ³ /mole (P=31.7 bar) using pressure measurements. The time dependence of the crystal pressure P(t) is measured on cooling at a rate of 10 mK/h followed by heating. The dependence P(t) has two distinct rises in pressure, the first rise being associated with the phase separation of the mixture and the second one with the melting of the ³ He inclusions formed. It is shown that the melting of the ³ He inclusions is almost complete after the fast cooling and the observed pressure jump is in good agreement with the corresponding change in the molar volume. The repeated crystallization of the inclusions is found to give rise to a large pressure gradient near the boundary of the inclusions, suppressing quantum diffusion considerably. This may result in an incomplete crystallization of the inclusions. The experimentally observed difference between the initial and final pressure in the sample corresponds to the fact that approximately 20% of the ³ He remains in the liquid state.     

Phase Separation Line for Solid Mixtures of 3He in 4He

The excess pressure due to the phase separation of solid mixtures of ³He in ⁴He held at a constant volume was measured and used for constructing the phase separation diagram of this system. We obtained high-quality homogeneous samples of the solid mixtures after several cycles of cooling down and heating up the two-phase crystal. This gave reliable and reproducible experimental data without hysteresis efects. We compared the phase diagram line obtained with various theoretical approaches, which describe the phase separation of the helium isotope mixtures. The regular solution model can not describe the experimental data well and neither can the asymmetrical Mullin's model. Good agreement is observed only with the theory of Edwards and Balibar which takes into account the difference between the crystal symmetry (hcp and bcc) of the coexisting phases.     

Lattice Relaxation in Solid 4He: Effect on Dynamics of 3He Impurities

We present a new simplified derivation of the effect of lattice relaxation that accompanies the quantum tunneling of ³He impurities in solid ⁴He on the nuclear spin-lattice relaxation of the ³He impurities for very low impurity concentrations. As a result of the larger zero point motion of the ³He impurity compared to the ⁴He atoms, a significant lattice distortion accompanies the impurity as it moves through the lattice and the dynamics of the impurity depends on both the interaction energy between two ³He atoms and on the relaxation of the lattice for the tunneling impurity. Using a phenomenological model for the lattice relaxation we compare the nuclear spin-lattice relaxation rates observed at low temperatures with the dependence on temperature expected for a ⁴He lattice relaxation comparable to that observed by Beamish et al. (Phys. Rev. Lett. 96:195304, 2006).     

Threshold Effect During Dissolution of 3He Inclusions in Solid 4He

A pressure jump has been found at the onset of the dissolution of bcc inclusions in separated solid ³ He - ⁴ He mixture if the crystal is overheated above a certain critical value. This effect can be explained in the framework of a multistage dissolution process model.     

Temperature and Concentration Relaxation in Phase-separated Superfluid 3He–4He Mixtures

The kinetics of the temperature and concentration variations in the superfluid ³He–⁴He mixtures with initial concentration of 9.8% ³He, and heated from below, was studied experimentally under the pressure of 0.38 bar over a temperature range of 150–400 mK. It is found that in contrast to homogeneous liquids, the temperature and concentration relaxation in phase-separated mixtures can be described by a superposition of two exponential processes in which the time constants of temperature and concentration variations coincide. If the initial mixture was homogeneous and phase separation was triggered by a heat flow, the temperature and concentration vary non-monotonically and exhibit anomalous features at the moment of phase separation. In this case the phase transition starts in the metastable superfluid, formed out of a quite supersaturated mixture where the nucleation of the new phase may be caused by quantized vortices. The results are analyzed in terms of two possible mechanisms of relaxation–the acoustic mechanism with the second sound velocity and the diffusive one connected with dissipative flows of impurity and thermal excitations. It is shown that the measured relaxation times agree with a prediction of the theory.      

NMR Study of Solid 3He Droplets In Phase-Separated 3He-4He Mixtures

We report measurements on solid ³ He droplets embedded in a solid ⁴ He matrix. A feature of our experiments is that the mixture crystals, of 1% ³ He concentration, are grown under constant pressure conditions to minimise the formation of defects. Upon cooling the mixture isotopic phase separation is clearly observed in both pressure and NMR data. At a pressure of 36 bar the ³ He separates as solid droplets. NMR measurements on these droplets indicate values of T ₁ and T ₂ similar to those in bulk solid ³ He at the same pressure in the temperature-independent régime. Measurements of the bounded diffusion in the droplets indicate a spin diffusion coefficient similar to that in bulk solid ³ He at the same pressure. These measurements also show the size of the droplets to be a few microns.     

NMR Studies of 3He Droplets in Dilute 3He-4He Solid Solutions

We have performed measurements of the temperature dependence of the nuclear spin-lattice relaxation times (T ₁) for a wide range of ³He concentrations for dilute mixtures of ³He in solid ⁴He. The temperatures for phase separation are determined for ³He concentrations 500<x ₃<2000 ppm for a molar volume V _M =20.7 cm³. We report the temperature dependence of the nuclear spin-lattice relaxation times for ³He in the droplets formed after phase separation at low temperatures. The temperature dependence suggests that the interface ³He atoms responsible for the relaxation are degenerate, not solid-like.     

Molar-Volume Dependence of the Pressure in hcp Solid 3He in Magnetic Fields

Pressure measurements have been made in a hcp solid ³ He at molar volumes from 18.90 to 19.45 cm ³ /mol, at temperatures down to 1 mK and in magnetic fields up to 0.16 Tesla. The results are analyzed by a high-temperature series expansion with multiple-exchange processes. The molar volume dependence of the multiple-exchange interactions has been determined by pressure measurements in magnetic fields. The results indicate that the exchange frequencies determined by the pressure measurements in a hcp solid ³ He are consistent with those obtained by magnetization measurements.