Effect of dissolved gases in water on acoustic cavitation and bubble growth rate in 0.83 MHz megasonic of interest to wafer cleaning

Changes in the cavitation intensity of gases dissolved in water, including H₂, N₂, and Ar, have been established in studies of acoustic bubble growth rates under ultrasonic fields. Variations in the acoustic properties of dissolved gases in water affect the cavitation intensity at a high frequency (0.83 MHz) due to changes in the rectified diffusion and bubble coalescence rate. It has been proposed that acoustic bubble growth rates rapidly increase when water contains a gas, such as hydrogen faster single bubble growth due to rectified diffusion, and a higher rate of coalescence under Bjerknes forces. The change of acoustic bubble growth rate in rectified diffusion has an effect on the damping constant and diffusivity of gas at the acoustic bubble and liquid interface. It has been suggested that the coalescence reaction of bubbles under Bjerknes forces is a reaction determined by the compressibility and density of dissolved gas in water associated with sound velocity and density in acoustic bubbles. High acoustic bubble growth rates also contribute to enhanced cavitation effects in terms of dissolved gas in water. On the other hand, when Ar gas dissolves into water under ultrasound field, cavitation behavior was reduced remarkably due to its lower acoustic bubble growth rate. It is shown that change of cavitation intensity in various dissolved gases were verified through cleaning experiments in the single type of cleaning tool such as particle removal and pattern damage based on numerically calculated acoustic bubble growth rates.     

声致发光气泡内水蒸气的影响

提出了一个单气泡声致发光的简单计算模型.这个模型是在均匀压强近似下，考虑质量和温度在气泡内的非均匀分布，同时考虑了水蒸气在气泡壁上的凝结与蒸发以及水蒸气在气泡内相对惰性气体的质量扩散.通过Saha方程估算气体电离密度，利用电子与离子、电子与中性粒子的轫致辐射，电子与离子的复合辐射公式估算气泡的辐射强度.不考虑化学反应，计算了不同水温时的气泡发光强度，发现当水温在0 ℃时轫致辐射发光模型比较符合实验结果，水温升高时，如水温为20 ℃或以上，轫致辐射发光模型的计算与实验结果出现数量级差别.考虑化学反应，轫致辐射发光模型的计算则总是比实验结果低2个数量级.     

Numerical simulations of acoustic cavitation noise with the temporal fluctuation in the number of bubbles

Numerical simulations of cavitation noise have been performed under the experimental conditions reported by Ashokkumar et al. (2007) [26]. The results of numerical simulations have indicated that the temporal fluctuation in the number of bubbles results in the broad-band noise. “Transient” cavitation bubbles, which disintegrate into daughter bubbles mostly in a few acoustic cycles, generate the broad-band noise as their short lifetimes cause the temporal fluctuation in the number of bubbles. Not only active bubbles in light emission (sonoluminescence) and chemical reactions but also inactive bubbles generate the broad-band noise. On the other hand, “stable” cavitation bubbles do not generate the broad-band noise. The weaker broad-band noise from a low-concentration surfactant solution compared to that from pure water observed experimentally by Ashokkumar et al. is caused by the fact that most bubbles are shape stable in a low-concentration surfactant solution due to the smaller ambient radii than those in pure water. For a relatively high number density of bubbles, the bubble–bubble interaction intensifies the broad-band noise. Harmonics in cavitation noise are generated by both “stable” and “transient” cavitation bubbles which pulsate nonlinearly with the period of ultrasound.     

An alternative technique for determining the number density of acoustic cavitation bubbles in sonochemical reactors

The present paper introduces a novel semi-empirical technique for the determination of active bubbles’ number in sonicated solutions. This method links the chemistry of a single bubble to that taking place over the whole sonochemical reactor (solution). The probe compound is CCl₄, where its eliminated amount within a single bubble (though pyrolysis) is determined via a cavitation model which takes into account the non-equilibrium condensation/evaporation of water vapor and heat exchange across the bubble wall, reactions heats and liquid compressibility and viscosity, all along the bubble oscillation under the temporal perturbation of the ultrasonic wave. The CCl₄ degradation data in aqueous solution (available in literature) are used to determine the number density through dividing the degradation yield of CCl₄ to that predicted by a single bubble model (at the same experimental condition of the aqueous data). The impact of ultrasonic frequency on the number density of bubbles is shown and compared with data from the literature, where a high level of consistency is found.     

竖直矩形通道内液体流动

通过对沸腾气泡在液体中的受力分析,建立了沸腾气泡长大过程的动力学方程;进而获得了沸腾气泡的生长速率与脱离直径的计算方法.采用图象捕集与处理系统,对竖直矩形通道内液体流动沸腾气泡长大与脱离行为进行实验测定,结合模型求解,获得了气泡生长速率、气泡脱离直径、气泡与加热壁面的接触角等参数随操作条件的变化;由模型计算所得的气泡脱离直径与实测值较为符合.     

A molecular dynamics simulation study on the cavitation inception of water with dissolved gases

The promotion/prevention mechanism of dissolved gases on cavitation inception is essential for many high-tech industries and research. In the present study, large-scale molecular dynamics simulations are performed to investigate the effects of water cavitation caused by different gas types by using nitrogen and oxygen gases with TIP4P/2005 water. The cavitation inception behaviour is analyzed via Mean First Passage Time method. Water with dissolved gases has a higher nucleation rate and is easier to cavitate than pure water. At the same gas concentration, the cavitation of water with nitrogen is promoted to a greater extent than that with oxygen. The number and energy of hydrogen bond (HB) are further calculated by the Acceptor-Hydrogen-Donor method to explain this promotion mechanism. The number and energy of HB in water with gases decrease compared with those in pure water. The introduction of gases weakens the HB network and promotes cavitation inception because of weaker interactions between gas and water molecules. A model is developed to describe the relationship between nucleation rate and HB energy. Gas molecules assemble on the surface of bubbles during water cavitation, which may decrease the free energy of bubble surface, maintain the existing bubble, and contribute to the growth process.     

Segregation of vapor and gas in a sonoluminescing bubble

Computer simulations of bubble oscillations in water are performed for various noble gases taking into account the segregation of water vapor and noble gas inside a collapsing bubble, which was predicted by Storey and Szeri [J. Fluid Mech. 396 (1999) 203]. It is clarified that the number of water vapor molecules dissociated inside a collapsing bubble is larger for heavier noble gases because of the lower thermal conductivity and the segregation of vapor and noble gas. It is also clarified that the temperature inside a helium bubble at the collapse increases considerably by the mixture segregation because a lesser amount of vapor is trapped inside a collapsing bubble. It is also clarified that multibubble sonoluminescence (MBSL) from heavier noble gases is brighter because of the lower ionization potential which results in the higher electron density and stronger plasma emissions.     

Thermodynamic crisis of boiling

The procedure of calculation of the dynamics of rapid near-wall vaporization near a metallic heater is considered. A physical model of explosive boiling-up on bubbles of fluctuation origin is used. The model is limited to regimes when the motion of bubbles can be ignored and convective flows do not have enough time to develop. It is assumed that the dry spot under a bubble thermally insulates the heater wall. The heat removal is provided by the vicinity of the wetting line (WL). An analytical calculation has become possible on the basis of the well-known exact solution to the problem of the temperature field near the wetting line. Generalization of this solution has led to two new problems. These are the problem of allowance for the difference of the dynamic wetting angle from the right angle and that of allowance for thermocapillary flows. A numerical comparison of the results of calculation of the dry area with the use of different methods of allowing for the “tightness” effect in the dynamics of bubble generation and growth has been made. The evolution of bubbles from their generation to growth limited by the heat supply has been investigated. It has been found that the transition stage in the development of bubbles from Rayleigh to thermal ones is of considerable importance in the processes of explosive boiling-up. The dynamics of change in the dry area and wetting line length prior to the stage of bubble merging into a vapor film has been calculated. A condition of passage of the heat flux through a maximum is found. The applicability of the idea of thermodynamic crisis to calculations of miniature devices is justified. The problem of constructing a model to calculate the interphase surface shape near the wetting line under a developed thermocapillary flow and considerable reactive forces of the vapor flow is formulated. The model is in good agreement with the results of experiments on pulsed superheating of liquids at a rate higher than 1 K/μs.     

The effect of preparation time and aeration rate on the properties of bulk micro-nanobubble water using hydrodynamic cavitation

Fundamental research on bulk micro-nanobubbles (BMNBs) has grown rapidly due to the demand for their industrial applications and potential role in interfacial sciences. This work focuses on examining properties of such bubbles, including the number, concentration, zeta potential, and surface tension in water. For this purpose, BMNBs were generated by the hydrodynamic cavitation (HC) mechanism. Distilled water and air in the experiments were the liquid and gas phases, respectively. The characterization of bulk microbubbles (BMBs) and bulk nanobubbles (BNBs) were performed through focused beam reflectance measurement (FBRM) and nanoparticle tracking analysis (NTA) techniques, respectively. Zeta potential and surface tension of aqueous solutions were measured at different time and aeration rates. The results showed that aeration rate and preparation time had an important role in the properties of BNBs (concentration, bubble size, and surface charge) and BMBs (number, and bubble size). The instability of BMBs led to the rapid changes in the dissolved oxygen (DO) content in the water. The number of BMBs decreased when preparation time and aeration rate increased, but their size remained constant. By enhancing the preparation time and aeration rate, the concentration of BNBs improved first and then reduced. Additionally, the surface tension of an aqueous solution containing BNBs was significantly lower than that of pure water.     

Skin formation and bubble growth during drying process of polymer solution

When a polymer solution with volatile solvent is dried, skins are often formed at the surface of the solution. It has been observed that after the skin is formed, bubbles often appear in the solution. We conducted experiments to clarify the relation between the skin formation and the bubble formation. We measured the time dependence of the thickness of the skin layer, the size of the bubbles, and the pressure in the solution. From our experiments, we concluded that i) the gas in the bubble is a mixture of solvent vapor and air dissolved in the solution, ii) the bubble nucleation is assisted by the pressure decrease in the solution covered by the skin layer, and iii) the growth of the bubbles is diffusion limited, mainly limited by the diffusion of air molecules dissolved in the solution.     

Phase transitions of perfluorocarbon nanoemulsion induced with ultrasound: A mathematical model

While ultrasound has been used in many medical and industrial applications, only recently has research been done on phase transformations induced by ultrasound. This paper presents a numerical model and the predicted results of the phase transformation of a spherical nanosized droplet of perfluorocarbon in water. Such a model has applications in acoustic droplet vaporization, the generation of gas bubbles for medical imaging, therapeutic delivery and other biomedical applications.The formation of a gas phase and the subsequent bubble dynamics were studied as a function of acoustic parameters, such as frequency and amplitude, and of the physical aspects of the perfluorocarbon nanodroplets, such as chemical species, temperature, droplet size and interfacial energy. The model involves simultaneous applications of mass, energy and momentum balances to describe bubble formation and collapse, and was developed and solved numerically. It was found that, all other parameters being constant, the maximum bubble size and collapse velocity increases with increasing ultrasound amplitude, droplet size, vapor pressure and temperature. The bubble size and collapse velocity decreased with increasing surface tension and frequency. These results correlate with experimental observations of acoustic droplet vaporization.     

Nucleation and growth of bubbles in He ion-implanted V/Ag multilayers

Microstructures of He ion-implanted pure Ag, pure V and polycrystalline V/Ag multilayers with individual layer thickness ranging from 1?nm to 50?nm were investigated by transmission electron microscopy (TEM). The bubbles in the Ag layer were faceted and larger than the non-faceted bubbles in the V layer under the same implantation conditions for both pure metals and multilayers. The substantially higher single defects surviving the spike phase and lower mobility of trapped He in bcc than those in fcc could account for this difference. For multilayers, the bubbles nucleate at interfaces but grow preferentially in Ag layers due to high mobility of trapped He in fcc Ag. In addition, the He concentration above which bubbles can be detected in defocused TEM images increases with decreasing layer thickness, from 0 for pure Ag to 4–5 at. % for 1?nm V/1?nm Ag multilayers. In contrast, the bubble size decreases with decreasing layer thickness, from approximately 4?nm in diameter in pure Ag to 1?nm in the 1?nm V/1?nm Ag multilayers. Elongated bubbles confined in the Ag layer by the V–Ag interfaces were observed in 1?nm multilayers. These observations show that bubble nucleation and growth can be suppressed to high He concentrations in nanoscale composites with interfaces that have high He solubility.     

A two-frequency acoustic technique for bubble resonant oscillation studies

A two-frequency acoustic apparatus has been developed to study the dynamics of a single gas or vapor bubble in water. An advantage of the apparatus is its capability of trapping a bubble by an ultrasonic standing wave while independently driving it into oscillations by a second lower frequency acoustic wave. For a preliminary application, the apparatus is used to study resonant oscillations. First, near-resonant coupling between the volume and the n = 3 shape oscillation modes of air bubbles at room temperature is studied, where n is the mode number. The stability boundary, amplitude versus frequency, of the volume oscillation forms a wedge centered at the resonant frequency, which qualitatively agrees with a theoretical prediction based on a phase-space analysis. Next, the resonant volume oscillations of vapor bubbles are studied. The resonant radius of vapor bubbles at 80 degrees C driven at 1682 Hz is determined to be 0.7 mm, in agreement with a prediction obtained by numerical simulation.     

Mathematical simulation of the compression process of a vapor bubble at a pressure increase in the surrounding liquid

The thermophysical and hydrodynamic processes in a spherical vapor bubble and the surrounding liquid at increasing external pressure are investigated by using a numerical simulation method. The investigation is performed on the basis of a new mathematical model belonging to the class of models of homobaric bubbles (the pressure in the bubble is homogeneous at nonhomogeneous temperature and density). The model takes into account the following main physical effects: the viscosity of the liquid, the heat conductivity of the liquid and vapor, the surface tension, and the phase transitions at the bubble surface. An energy equation taking into account convective heat transfer and viscous dissipation in the liquid is used to calculate the temperature fields in the liquid and vapor. The model also takes into account the dependence of the thermophysical properties on the temperature. A distinctive feature of the proposed model is that the integral conservation law of the system’s total energy (including the kinetic energy of the liquid, the surface energy, and the internal energy of the liquid and vapor) is exactly satisfied (without allowance for the kinetic energy of the vapor). As a result of the numerical simulation of the compression of vapor bubbles in water, we obtained data for the major characteristics of the process at considerable degrees of compression. It is shown that the heat and mass transfer between the vapor in a bubble and the surrounding liquid considerably slow down the temperature increase in the bubble.     

快速降压下Tween20 液滴真空闪蒸特性

为探究闪蒸喷雾冷却的微观机理, 设计并搭建了液滴悬挂式真空闪蒸实验装置, 利用可视化窗口探究Tween20 液滴闪蒸过程中的闪蒸特性及气泡生长机理. 液滴在快速降压过程中形态会经历气泡成核、气泡生长、伴随气泡生长、爆裂这四个阶段的变化, 并反复循环这一过程直至液滴稳定蒸发. 对于液滴温度的变化, 闪蒸室的终态压力起到了决定性的作用, 并且其终态温度随压力的升高明显上升. 同时通过液滴闪蒸过程形态图分析发现, 液滴在剧烈爆炸阶段其温度也发生明显下降; 在稳定蒸发阶段, 其温度也将开始稳定不变. 因此可知液滴的剧烈爆炸会带走其自身的大量热量. 而 Tween20 浓度对液滴温度的影响微乎其微, 但其会使液滴内气泡的初始成核时间发生明显滞后, 并抑制液滴内的气泡发生破裂.     

Dependence of the characteristics of bubbles on types of sonochemical reactors

Computer simulations of bubble oscillations in liquid water irradiated by an ultrasonic wave have revealed that the characteristic of bubbles depends on types of sonochemical reactors: a horn-type reactor and a standing-wave type reactor. When the acoustic amplitude is large at 20 kHz, the bubble content is mostly water vapor even at the end of the bubble collapse and the temperature inside a bubble at the collapse is relatively low. On the other hand, when the acoustic amplitude is relatively low, the bubble content is mostly noncondensable gas at the end of the bubble collapse and the bubble temperature is relatively high. In a horn-type sonochemical reactor, the former type of bubbles are dominant because many bubbles exist near the horn-tip where the acoustic amplitude is large, while in a standing-wave type reactor the latter type of bubbles are dominant because the Bjerknes force gathers bubbles at a region where acoustic amplitude is relatively low.     

Observations of the collapses and rebounds of millimeter-sized lithotripsy bubbles

Bubbles excited by lithotripter shock waves undergo a prolonged growth followed by an inertial collapse and rebounds. In addition to the relevance for clinical lithotripsy treatments, such bubbles can be used to study the mechanics of inertial collapses. In particular, both phase change and diffusion among vapor and noncondensable gas molecules inside the bubble are known to alter the collapse dynamics of individual bubbles. Accordingly, the role of heat and mass transport during inertial collapses is explored by experimentally observing the collapses and rebounds of lithotripsy bubbles for water temperatures ranging from 20 to 60 °C and dissolved gas concentrations from 10 to 85% of saturation. Bubble responses were characterized through high-speed photography and acoustic measurements that identified the timing of individual bubble collapses. Maximum bubble diameters before and after collapse were estimated and the corresponding ratio of volumes was used to estimate the fraction of energy retained by the bubble through collapse. The rebounds demonstrated statistically significant dependencies on both dissolved gas concentration and temperature. In many observations, liquid jets indicating asymmetric bubble collapses were visible. Bubble rebounds were sensitive to these asymmetries primarily for water conditions corresponding to the most dissipative collapses.     

Numerical modelling of acoustic cavitation threshold in water with non-condensable bubble nuclei

Numerical modelling of acoustic cavitation threshold in water is presented taking into account non-condensable bubble nuclei, which are composed of water vapor and non-condensable air. The cavitation bubble growth and collapse dynamics are modeled by solving the Rayleigh-Plesset or Keller-Miksis equation, which is combined with the energy equations for both the bubble and liquid domains, and directly evaluating the phase-change rate from the liquid and bubble side temperature gradients. The present work focuses on elucidating acoustic cavitation in water with a wide range of cavitation thresholds (0.02–30 MPa) reported in the literature. Computations for different nucleus sizes and acoustic frequencies are performed to investigate their effects on bubble growth and cavitation threshold. The numerical predictions are observed to be comparable to the experimental data in the previous works and show that the cavitation threshold in water has a wide range depending on the bubble nucleus size.     

Effect of static pressure on acoustic energy radiated by cavitation bubbles in viscous liquids under ultrasound

The effect of static pressure on acoustic emissions including shock-wave emissions from cavitation bubbles in viscous liquids under ultrasound has been studied by numerical simulations in order to investigate the effect of static pressure on dispersion of nano-particles in liquids by ultrasound. The results of the numerical simulations for bubbles of 5 μm in equilibrium radius at 20 kHz have indicated that the optimal static pressure which maximizes the energy of acoustic waves radiated by a bubble per acoustic cycle increases as the acoustic pressure amplitude increases or the viscosity of the solution decreases. It qualitatively agrees with the experimental results by Sauter et al. [Ultrason. Sonochem. 15, 517 (2008)]. In liquids with relatively high viscosity (～200 mPa s), a bubble collapses more violently than in pure water when the acoustic pressure amplitude is relatively large (～20 bar). In a mixture of bubbles of different equilibrium radius (3 and 5 μm), the acoustic energy radiated by a 5 μm bubble is much larger than that by a 3 μm bubble due to the interaction with bubbles of different equilibrium radius. The acoustic energy radiated by a 5 μm bubble is substantially increased by the interaction with 3 μm bubbles.     

Does water vapor prevent upscaling sonoluminescence?

Experimental results for single-bubble sonoluminescence of air bubbles at very low frequency f = 7.1 kHz are presented: In contrast to the predictions of a recent model [S. Hilgenfeldt and D. Lohse, Phys. Rev. Lett. 82, 1036 (1999)], the bubbles are only as bright (10(4)-10(5) photons per pulse) and the pulses as long (approximately 150 ps) as at f = 20 kHz. We can theoretically account for this effect by incorporating water vapor into the model: During the rapid bubble collapse a large amount of water vapor is trapped inside the bubble, resulting in an increased heat capacity and hence lower temperatures, i.e., hindering upscaling. At this low frequency water vapor also dominates the light emission process.