Oscillations and accelerations of ice crystal growth rates in microgravity in presence of antifreeze glycoprotein impurity in supercooled water.

The free growth of ice crystals in supercooled bulk water containing an impurity of glycoprotein, a bio-macromolecule that functions as 'antifreeze' in living organisms in a subzero environment, was observed under microgravity conditions on the International Space Station. We observed the acceleration and oscillation of the normal growth rates as a result of the interfacial adsorption of these protein molecules, which is a newly discovered impurity effect for crystal growth. As the convection caused by gravity may mitigate or modify this effect, secure observations of this effect were first made possible by continuous measurements of normal growth rates under long-term microgravity condition realized only in the spacecraft. Our findings will lead to a better understanding of a novel kinetic process for growth oscillation in relation to growth promotion due to the adsorption of protein molecules and will shed light on the role that crystal growth kinetics has in the onset of the mysterious antifreeze effect in living organisms, namely, how this protein may prevent fish freezing.

Oscillatory growth for twisting crystals.

We demonstrate the oscillatory phenomenon for the twisting growth of a triclinic crystal through in situ observation of the concentration field around the growing tip of a needle by high-resolution phase-shift interferometry.

Stable growth mechanisms of ice disk crystals in heavy water.

Ice crystal growth experiments in heavy water were carried out under microgravity to investigate the morphological transition from a disk crystal to a dendrite. Surprisingly, however, no transition was observed, namely, the disk crystal or dendrite maintained its shape throughout the experiments, unlike the results obtained on the ground. Therefore, we introduce a growth model to understand disk growth. The Gibbs-Thomson effect is taken into account as a stabilization mechanism. The model is numerically solved by varying both an interfacial tension of the prism plane and supercooling so that the final sizes of the crystals can become almost the same to determine the interfacial tension. The results are compared with the typical experimental ones and thus the interfacial tension is estimated to be 20 mJ/m(2). Next, the model is solved under two supercooling conditions by using the estimated interfacial tension to understand stable growth. Comparisons between the numerical and experimental results show that our model explains well the microgravity experiments. It is also found that the experimental setup has the capability of controlling temperature on the order of 1/100 K.

Measurements of growth rates of an ice crystal from supercooled heavy water under microgravity conditions: basal face growth rate and tip velocity of a dendrite.

The growth of single ice crystals from supercooled heavy water was studied under microgravity conditions in the Japanese Experiment Module ''KIBO'' of the International Space Station (ISS). The velocities of dendrite tips parallel to the a axis and the growth rates of basal faces parallel to the c axis were both analyzed under supercooling ranging from 0.03 to 2.0 K. The velocities of dendrite tips agree with the theory for larger amounts of supercooling when the growth on the basal faces are not zero. At very low supercooling there is no growth on the basal faces. With increasing supercooling the basal faces start to grow, the growth rate changing as a function of supercooling with a power law with an exponent of about 2, with the exponent approaching 1 as supercooling increases further. We interpret the growth on the basal faces as being controlled by two-dimensional nucleation under low supercooling, with a change in the growth kinetics to spiral growth with the aid of screw dislocations with increasing supercooling then to a linear growth law. We discuss the combined effect of tip velocity and basal face kinetics on pattern formation during the growth of ice.

Elementary steps at the surface of ice crystals visualized by advanced optical microscopy.

Due to the abundance of ice on earth, the phase transition of ice plays crucially important roles in various phenomena in nature. Hence, the molecular-level understanding of ice crystal surfaces holds the key to unlocking the secrets of a number of fields. In this study we demonstrate, by laser confocal microscopy combined with differential interference contrast microscopy, that elementary steps (the growing ends of ubiquitous molecular layers with the minimum height) of ice crystals and their dynamic behavior can be visualized directly at air-ice interfaces. We observed the appearance and lateral growth of two-dimensional islands on ice crystal surfaces. When the steps of neighboring two-dimensional islands coalesced, the contrast of the steps always disappeared completely. We were able to discount the occurrence of steps too small to detect directly because we never observed the associated phenomena that would indicate their presence. In addition, classical two-dimensional nucleation theory does not support the appearance of multilayered two-dimensional islands. Hence, we concluded that two-dimensional islands with elementary height (0.37 and 0.39 nm on basal and prism faces, respectively) were visualized by our optical microscopy. On basal and prism faces, we also observed the spiral growth steps generated by screw dislocations. The distance between adjacent spiral steps on a prism face was about 1/20 of that on a basal face. Hence, the step ledge energy of a prism face was 1/20 of that on a basal face, in accord with the known lower-temperature roughening transition of the prism face.

Oscillation and synchronization in the combustion of candles.

We investigate a simple experimental system using candles; stable combustion is seen when a single candle burns, while oscillatory combustion is seen when three candles burn together. If we consider a set of three candles as a component oscillator, two oscillators, that is, two sets of three candles, can couple with each other, resulting in both in-phase and antiphase synchronization depending on the distance between the two sets. The mathematical model indicates that the oscillatory combustion in a set of three candles is induced by a lack of oxygen around the burning point. Furthermore, we suggest that thermal radiation may be an essential factor of the synchronization.

Growth of an ice disk: dependence of critical thickness for disk instability on supercooling of water.

The appearance of an asymmetrical pattern that occurs when a disk crystal of ice grows from supercooled water was studied by using an analysis of growth rates for radius and thickness. The growth of the radius is controlled by transport of latent heat and is calculated by solving the diffusion equation for the temperature field surrounding the disk. The growth of the thickness is governed by the generation and lateral motion of steps and is expressed as a power function of the supercooling at the center of a basal face. Symmetry breaking with respect to the basal face of an ice disk crystal is observed when the thickness reaches a critical value; then one basal face becomes larger than the other and the disk loses its cylindrical shape. Subsequently, morphological instability occurs at the edge of the larger basal face of the asymmetrical shape (Shimada, W.; Furukawa, Y. J. Phys. Chem. 1997, B101, 6171-6173). We show that the critical thickness is related to the critical condition for the stable growth of a basal face. A difference of growth rates between two basal faces is a possible mechanism for the appearance of the asymmetrical shape.