A simple ice nucleation spectrometer

The construction of a simple ice nucleation spectrometer is described. It uses 10 microliter droplets loaded into glass capillary tubes which are then inserted into an aluminium holder. Each holder takes six capillary tubes surrounding a central thermocouple. Four holders are placed into a cooling block, cooled by fluid from a programmable refrigerated circulator, and the thermocouples interfaced to a computer to record temperatures. Freezing of each sample is detected by an exotherm on the temperature recording, with 24 samples recorded per run. The spectrometer was tested using deionized water, an extract from a New Zealand alpine cockroach and an extract of lawn grass. The cockroach extract is estimated to contain about 10(3) more nucleators, active at -5 degrees C, than the grass extract.     

Two-dimensional nucleation of ice from supercooled water

We report the temperature dependent nucleation rates of ice from single water drops supporting aliphatic alcohol Langmuir films. Analysis in the context of a classical theory of heterogeneous nucleation suggests that the critical nucleus is essentially a monolayer, and that the rate-limiting steps in these nucleation processes are therefore not merely influenced by, but instead dictated by, the physics of the water-alcohol interface. Consequently, reduced dimensionality may be much more important in heterogeneous nucleation than has previously been believed.     

氘氚冰籽晶的形核行为

为了实现激光约束核聚变(ICF)的自持聚变目标,对靶壳内氘氚冰的质量提出了极其苛刻的要求,冰层内表面和靶壳的同心度要求大于99.9%,冰层内表面均方根粗糙度(RMS)优于1μm.高质量的冷冻氘氚靶建立在靶壳内高质量氘氚冰层的前提之上.单晶是冰层的最好形态,在靶壳内获得氘氚冰籽晶是基础条件.本文通过采用逐渐降低升温速率的台阶控温方法,开展了充气微管内保留籽晶的研究,揭示了充气微管内保留籽晶的形核机理,实验结果表明,利用充气管口可保留稳定、单一的籽晶,在相同的过冷度下,当氘氚籽晶c轴方向与充气管轴向平行时,生长速度较c轴垂直于充气管轴向时的速度慢约1—2个量级,为获得高质量的籽晶从而形成高质量的氘氚冰提供了参考和支撑.     

Normal processes which inhibit superconductivity

The effective interaction strength for the establishment of Cooper pairs in a degenerate Fermion gas is shown to be reduced by a second-order exchange process. In physical terms, the reduction is a consequence of the normal polarization clouds surrounding the individual Fermions. Because of the Pauli exclusion principle, these polarization clouds block the approach of further quasi-particles and thereby tend to prevent Cooper pairing. The effect is related to but simpler than that studied byHenley andWilets in connection with the energy gap of nuclear matter. The second-order suppressive effect is considerable for strong interaction and large state density, and may even prevent the superconducting transition from occurring at all.     

The sonocrystallisation of ice in sucrose solutions: primary and secondary nucleation

Two investigations of the sonocrystallisation of ice are reported for solutions in the concentration range of 0-45 wt.% sucrose. The first, carried out at 20 kHz using a commercial sonicator shows clear evidence of the stimulation of primary nucleation, by increasing the temperature at which nucleation takes place. The nucleation temperature is also increased as the ultrasonic power output level or duty cycles are increased. The second uses a novel measurement cell which permits the direct visualisation of the crystallisation and cavitation with a light microscope while different levels of alternating pressures at a frequency of 67 kHz are applied to the sample, whose heating and cooling is carefully controlled and monitored. This provides confirmation of the fragmentation of ice dendrites growing in a sucrose solution to produce smaller new ice crystals (secondary nucleation). These observations show that the primary and secondary nucleation of ice are both possible during the sonocrystallisation of ice.     

Ultrasonic-induced nucleation of ice in water containing air bubbles

Cavitation induced by ultrasonic vibrations can cause nucleation of ice in supercooled water. In this study, the time required for ultrasonic-induced nucleation of ice was measured for water containing two different size distributions of air bubbles. When the water was supersaturated with air bubbles, there was a time lag of about 0.5 s between the onset of ultrasonic irradiation and the onset of ice nucleation, and the probability of ice nucleation was unusually high within 0.5-1.1 s after the onset of ultrasonic irradiation. These results cannot be explained by conventional models alone, in which the collapse of a cavitation bubble triggers the nucleation of ice. Secondary effects appear to also influence ice nucleation.     

Theoretical model of ice nucleation induced by inertial acoustic cavitation. Part 2: Number of ice nuclei generated by a single bubble

In the preceding paper (part 1), the pressure and temperature fields close to a bubble undergoing inertial acoustic cavitation were presented. It was shown that extremely high liquid water pressures but quite moderate temperatures were attained near the bubble wall just after the collapse providing the necessary conditions for ice nucleation. In this paper (part 2), the nucleation rate and the nuclei number generated by a single collapsing bubble were determined. The calculations were performed for different driving acoustic pressures, liquid ambient temperatures and bubble initial radius. An optimal acoustic pressure range and a nucleation temperature threshold as function of bubble radius were determined. The capability of moderate power ultrasound to trigger ice nucleation at low undercooling level and for a wide distribution of bubble sizes has thus been assessed on the theoretical ground.     

Suppression of ice nucleation in supercooled water under temperature gradients

Understanding the behaviours of ice nucleation in non-isothermal conditions is of great importance for the preparation and retention of supercooled water. Here ice nucleation in supercooled water under temperature gradients is analyzed thermodynamically based on classical nucleation theory (CNT). Given that the free energy barrier for nucleation is dependent on temperature, different from a uniform temperature usually used in CNT, an assumption of linear temperature distribution in the ice nucleus was made and taken into consideration in analysis. The critical radius of the ice nucleus for nucleation and the corresponding nucleation model in the presence of a temperature gradient were obtained. It is observed that the critical radius is determined not only by the degree of supercooling, the only dependence in CNT, but also by the temperature gradient and even the Young's contact angle. Effects of temperature gradient on the change in free energy, critical radius, nucleation barrier and nucleation rate with different contact angles and degrees of supercooling are illustrated successively. The results show that a temperature gradient will increase the nucleation barrier and decrease the nucleation rate, particularly in the cases of large contact angle and low degree of supercooling. In addition, there is a critical temperature gradient for a given degree of supercooling and contact angle, at the higher of which the nucleation can be suppressed completely.     

Neutrons for probing the ice nucleation on atmospheric soot particles

Soot resulting from combustion of kerosene in aircraft engines can act as condensation nuclei for water/ice in the atmosphere and promote the formation of contrails that turn into artificial cirrus clouds and affect the climate. The mechanisms of nucleation of water/ice particles are not well identified. Studies ??in situ?? are difficult to realize, so we try to determine by neutron diffraction the nucleation of water/ice adsorbed on soot collected at the outlet of an aircraft engine combustor within the conditions of the upper troposphere. The results are compared with those obtained on model laboratory soot. The comparison highlights the role of chemical impurities and structural defects of original aircraft engine soot on the nucleation of water/ice in atmospheric conditions.     

A theoretical model for ice primary nucleation induced by acoustic cavitation

The modelling and simulation of ice nucleation triggered by acoustic cavitation was addressed in this study. The objective was to evaluate the number of nuclei generated by a single gas bubble and afterwards by a multi-bubble system as function of the acoustic pressure (ultrasound wave amplitude) and supercooling level (liquid temperature). According to our calculations, the nucleation could be initiated with moderated acoustic pressure amplitude (around one bar) even at low supercooling levels (around few degrees). These results may provide a sound basis for the control of ice crystal size and morphology which is a key issue in industrial freezing and freeze-drying processes.     

The effect of antifreeze proteins and poly(vinyl alcohol) on the nucleation of ice: a preliminary study

Three substances have been tested for ice nucleation inhibition. These were an antifreeze protein AFP III from the fish Macrozoarces americanus, an antifreeze glycoprotein AFGP from the fish Dissostichus mawsoni, and an 80% hydrolysed poly(vinyl alcohol) with a molecular weight of 9 to 10 kD. A nucleation spectrometer was used to test nucleation inhibition at a range of concentrations against two types of ice nuclei: those present in tap water and a bacterial nucleator from Pseudomonas syringae. The PVA reduced the nucleation temperature of tap water and the bacterial dispersions at all the concentrations which were tested. The AFGP reduced the nucleation temperature of tap water but enhanced the nucleation activity of the bacterial nucleators. At low concentrations the AFP III reduced the nucleation temperature of both tap water and the bacterial nucleator. At high concentrations the AFP III enhanced the nucleation temperature of the bacterial nucleator and broadened the nucleation spectrum of the tap water to encompass the nucleation spread of the control. The possible mechanisms of nucleation suppression and enhancement are discussed.     

Theoretical model of ice nucleation induced by acoustic cavitation. Part 1: Pressure and temperature profiles around a single bubble

This paper deals with the inertial cavitation of a single gas bubble in a liquid submitted to an ultrasonic wave. The aim was to calculate accurately the pressure and temperature at the bubble wall and in the liquid adjacent to the wall just before and just after the collapse. Two different approaches were proposed for modeling the heat transfer between the ambient liquid and the gas: the simplified approach (A) with liquid acting as perfect heat sink, the rigorous approach (B) with liquid acting as a normal heat conducting medium. The time profiles of the bubble radius, gas temperature, interface temperature and pressure corresponding to the above models were compared and important differences were observed excepted for the bubble size. The exact pressure and temperature distributions in the liquid corresponding to the second model (B) were also presented. These profiles are necessary for the prediction of any physical phenomena occurring around the cavitation bubble, with possible applications to sono-crystallization.     

A study on the primary and secondary nucleation of ice by power ultrasound

Several different investigations have been carried out to study the primary and secondary nucleation of ice by sonocrystallisation. Firstly, the primary nucleation of discrete ice crystals in a supercooled sucrose solution has been observed. For increasing concentrations of sucrose solutions from 0 to 45 wt%, the nucleation temperature consistently occurs at a higher nucleation temperature in the presence of ultrasound. The nucleation temperature also increases as the power output and duty cycle of a commercial ultrasonic horn are increased. Snap shot images of the bubble clouds obtained from the ultrasonic horn also show that the number of bubbles appears to increase as the ultrasonic output is increased. This suggests that the nucleation of ice is related to the power output and number of cavitation bubbles. The effect of a single bubble on the sonocrystallisation of ice is discussed. High-speed movies (1120 fps) have shown that the crystallisation appears to occur in the immediate vicinity of the single bubble. In most cases, many crystals are observed and it is not known whether a single ice crystal is being fragmented by the bubble or whether many crystals are being initiated. The bubble appears to undergo a dancing regime, frequently splitting and rejoining and also emitting some small microbubbles. A study on the secondary nucleation of ice in sucrose solutions has been carried out using a unique ultrasonic cold stage device. Images taken using a microscope system show that the pre-existing ice dendrite crystals can be broken up into smaller fragments by an ultrasonic field. Cavitation bubbles appear to be important during the fragmentation process, possibly melting any ice crystals in their path. Flow patterns around cavitation bubbles have also been observed, and these may be responsible for the fragmentation of ice crystals.     

静磁场对冰晶成核过程影响的机理分析

常规的冷冻方式会在材料中形成大冰晶从而导致材料品质下降,在冷冻过程中加以磁场辅助可以改善冻结效果。从热力学原理出发,研究静磁场对冰晶成核过程的影响,将静磁场作用以附加自由能引入冰晶成核过程。研究结果表明,静磁场作用可以减小冰晶成核的临界半径和临界功,提高均相成核率,且磁场强度越大,临界半径和临界功越小,成核率越高;水的附加过冷度也随磁场强度的增大而增大,与相关实验数据趋势吻合较好。     

The phase coexistence method to obtain surface free energies and nucleation barriers: a brief review

ABSTRACT

A recently developed method where one analyses the finite size effects associated with liquid–solid phase equilibria including vapour–crystal coexistence is briefly reviewed. It is shown that the estimation of the chemical potential of the vapour surrounding the crystal as function of the crystal volume yields information on the bulk coexistence conditions, when an extrapolation to the thermodynamic limit is performed. Estimating the pressure of the fluid surrounding the crystal nucleus in the finite simulation box and the volume of this nucleus that coexists with the fluid in thermal equilibrium, an estimate for the total surface excess free energy can be obtained, which to a very good approximation is independent of the size of the simulation box. The free energy barrier against homogeneous nucleation of crystals thus can be estimated as a function of the nucleus volume. Monte Carlo simulations for the soft effective Asakura–Oosawa model of colloid-polymer mixtures which form face-centered cubic colloidal crystals are used to exemplify this method, computing the surface excess free energy of these crystals over a wide range of crystal volumes, without the need to characterise the non-spherical crystal shape. A possible extension of these concepts to heterogeneous nucleation is also briefly discussed.     

Unsteady nucleation in layers of amorphous ice in the presence of artificially injected crystalline centers

The role of thermal conditions under which crystallization of an amorphous substance occurs is analyzed theoretically with allowance for unsteady nucleation.     

Thermodynamics of high-pressure ice polymorphs: ice II

Thermodynamic properties of high-pressure solid phase ice II are studied theoretically. The P-V-T equation of state of ice II is derived and its thermodynamic functions are calculated based on the available experimental data. New results are presented concerning the equilibrium solid-solid phase transitions between ice II and ice Ih, ice II and III, and ice II and V.     

Quantum ice: a quantum Monte Carlo study

Ice states, in which frustrated interactions lead to a macroscopic ground-state degeneracy, occur in water ice, in problems of frustrated charge order on the pyrochlore lattice, and in the family of rare-earth magnets collectively known as spin ice. Of particular interest at the moment are "quantum spin-ice" materials, where large quantum fluctuations may permit tunnelling between a macroscopic number of different classical ground states. Here we use zero-temperature quantum Monte Carlo simulations to show how such tunnelling can lift the degeneracy of a spin or charge ice, stabilizing a unique "quantum-ice" ground state-a quantum liquid with excitations described by the Maxwell action of (3+1)-dimensional quantum electrodynamics. We further identify a competing ordered squiggle state, and show how both squiggle and quantum-ice states might be distinguished in neutron scattering experiments on a spin-ice material.