Enhancement of cavitation activity and particle removal with pulsed high frequency ultrasound and supersaturation

Megasonic cleaning as applied in leading edge semiconductor device manufacturing strongly relies on the phenomenon of acoustic cavitation. As the occurrence of acoustic cavitation is incorporating a multitude of interdependent effects, the amount of cavitation activity in the cleaning liquid strongly depends on the sonication conditions. It is shown that cavitation activity as measured by means of ultraharmonic cavitation noise can be significantly enhanced when pulsed sonication is applied to a gas supersaturated liquid under traveling wave conditions. It is demonstrated that this enhancement coincides with a dramatic increase in particle removal and is therefore of great interest for megasonic cleaning applications. It is demonstrated that the optimal pulse parameters are determined by the dissolution time of the active bubbles, whereas the amount of cavitation activity depends on the ratio between pulse-off and pulse-on time as well as the applied acoustic power. The optimal pulse-off time is independent of the corresponding pulse-on time but increases significantly with increasing gas concentration. We show that on the other hand, supersaturation is needed to enable acoustic cavitation at aforementioned conditions, but has to be kept below values, for which active bubbles cannot dissolve anymore and are therefore lost during subsequent pulses. For the applicable range of gas contents between 100% and 130% saturation, the optimal pulse-off time reaches values between 150 and 340 ms, respectively. Full particle removal of 78 nm-diameter silica particles at a power density of 0.67 W/cm² is obtained for the optimal pulse-off times. The optimal pulse-off time values are derived from the dissolution time of bubbles with a radius of 3.3 μm and verified experimentally. The bubble radius used in the calculations corresponds to the linear resonance size in a 928 kHz sound field, which demonstrates that the recycling of active bubbles is the main enhancement mechanism. The optimal choice of the pulsing conditions however is constrained by the trade-off between the effective sonication time and the desire to have a sufficient amount of active bubbles at lower powers, which might be necessary if very delicate structures have to be cleaned.     

Influence of dissolved-air concentration on spatial distribution of bubbles for sonochemistry

The pulsation of ultrasonic cavitation bubbles at various dissolved-air concentration in a sonochemical reaction field of standing-wave type is investigated experimentally by laser-light scattering. When a thin light sheet, finer than half the wavelength of sound, is introduced into the cavitation bubbles at an antinode of sound pressure, the scattered light intensity oscillates. The peak-to-trough light intensity is correlated with the number of bubbles that contribute to the sonochemical reaction. It is shown that as the dissolved air concentration becomes higher, the weighted center of the spatial distribution of the peak-to-trough intensity tends to shift towards the liquid surface. At higher concentration of the dissolved air, a great deal of bubbles with size distribution generated due to coalescence between bubbles disturbs sound propagation to change the sound phase easily. A standing wave to trap tiny oscillating bubbles is established only at the side which is nearer to the liquid surface. Also at higher concentration, liquid flow induced by drag motion of bubbles by the action of radiation force becomes apparent and position-unstable region of bubble is enlarged from the side of sound source towards the liquid surface. Therefore, the position of oscillating bubbles active for sonochemical reaction is limited at the side which is nearer to the liquid surface at higher concentration of the dissolved air.     

Ultrasonic cavitation at liquid/solid interface in a thin Ga–In liquid layer with free surface

Cavitation in thin layer of liquid metal has potential applications in chemical reaction, soldering, extraction, and therapeutic equipment. In this work, the cavitation characteristics and acoustic pressure of a thin liquid Ga–In alloy were studied by high speed photography, numerical simulation, and bubble dynamics calculation. A self-made ultrasonic system with a TC4 sonotrode, was operated at a frequency of 20 kHz and a max output power of 1000 W during the cavitation recording experiment. The pressure field characteristic inside the thin liquid layer and its influence on the intensity, types, dimensions, and life cycles of cavitation bubbles and on the cavitation evolution process against experimental parameters were systematically studied. The results showed that acoustic pressure inside the thin liquid layer presented alternating positive and negative characteristics within 1 acoustic period (T). Cavitation bubbles nucleated and grew during the negative-pressure stage and shrank and collapsed during the positive-pressure stage. A high bubble growth speed of 16.8 m/s was obtained and evidenced by bubble dynamics calculation. The maximum absolute pressure was obtained at the bottom of the thin liquid layer and resulted in the strongest cavitation. Cavitation was divided into violent and weak stages. The violent cavitation stage lasted several hundreds of acoustic periods and had higher bubble intensity than the weak cavitation stage. Cavitation cloud preferentially appeared during the violent cavitation stage and had a life of several acoustic periods. Tiny cavitation bubbles with life cycles shorter than 1 T dominated the cavitation field. High cavitation intensities were observed at high ultrasonication power and when Q235B alloy was used because such conditions lead to high amplitudes on the substrate and further high acoustic pressure inside the liquid.     

Optical visualization of non-linear acoustic propagation in cavitating liquids

Non-linearity effects on sound propagation induced by cavitation bubbles are investigated. The convergence of an acoustic wave due to the interaction with the microbubbles produced in the cavitation zone is shown experimentally. In these conditions the theoretical analysis shows that the self-focusing primarily depends on the effective microbubble volume fraction. This fraction turns out to be about 10^?6 with a corresponding self-focusing distance of about 9 cm in the Fraunhofer region of a plane circular transducer.     

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.     

Influence of frequency sweep on sonochemiluminescence and sonoluminescence

Bubbles generated by acoustic cavitation may be efficient in light production by direct emission (sonoluminescence) or indirect emission (sonochemiluminescence) depending on operating parameters such as acoustic pressure and surface tension. These conditions are quite difficult to reach at very high frequencies, even by concentrating the acoustic power at a given location via focusing the acoustic field thanks to the transducer shape (High Intensity Focused Ultrasound). The current work aims at probing the cavitation bubble behaviour under short frequency sweeps by monitoring sonochemiluminescence and sonoluminescence activities. When the frequency was swept in reverse (negative sweep), an enhancement in the SCL, relative to the SCL observed under a single frequency irradiation, was observed. Conversely, a positive frequency sweep resulted in the quenching of SCL intensity. The degree of SCL enhancement and quenching was also dependent on the rate at which the frequency was being swept and on the change in the size of cavitation bubbles. The size of cavitation bubbles varied with varying starting sweep frequency (3.4, 3.6 and 4.2 MHz), affecting both SCL and sonoluminescence (SL) emissions. The addition of a surfactant (sodium dodecyl sulphate) affected the observed results, possibly due to its influence on coalescence between cavitation bubbles. The results suggest that the enhancement and quenching are related to the response of bubbles generated by the starting frequency to the direction of the frequency sweep and the influence of the sweep rate on growth and coalescence of bubbles, which affected the population of the active bubbles.     

Cavitation mapping by sonochemiluminescence with less bubble displacement induced by acoustic radiation force in a 1.2 MHz HIFU

An acoustic radiation force counterbalanced appliance was employed to map the cavitation distribution in water. The appliance was made up of a focused ultrasound transducer and an aluminum alloy reflector with the exactly same shape. They were centrosymmetry around the focus of the source transducer. Spatial–temporal dynamics of cavitation bubble clouds in the 1.2 MHz ultrasonic field within this appliance were observed in water. And they were mapped by sonochemiluminescence (SCL) recordings and high-speed photography. There were significant differences in spatial distribution and temporal evolution between normal group and counterbalanced group. The reflector could avoid bubble directional displacement induced by acoustic radiation force under certain electric power (⩽50 W). As a result, the SCL intensity in the pre-focal region was larger than that of normal group. In event of high electric power (⩾70 W), most of the bubbles were moving in acoustic streaming. When electric power decreased, bubbles kept stable and showed stripe structure in SCL images. Both stationary bubbles and moving bubbles have been captured, and exhibited analytical potential with respect to bubbles in therapeutic ultrasound.     

Studies of a novel sensor for assessing the spatial distribution of cavitation activity within ultrasonic cleaning vessels

This paper describes investigations of the spatial distribution of cavitation activity generated within an ultrasonic cleaning vessel, undertaken using a novel cavitation sensor concept. The new sensor monitors high frequency acoustic emissions (>1 MHz) generated by micron-sized bubbles driven into acoustic cavitation by the applied acoustic field. Novel design features of the sensor, including its hollow, cylindrical shape, provide the sensor with spatial resolution, enabling it to associate the megahertz acoustic emissions produced by the cavitating bubbles with specific regions of space within the vessel. The performance of the new sensor has been tested using a 40 kHz ultrasonic cleaner employing four transducers and operating at a nominal electrical power of 140 W under controlled conditions. The results demonstrate the ability of the sensors to identify 'hot-spots' and 'cold-spots' in cavitation activity within the vessel, and show good qualitative agreement with an assessment of the spatial distribution of cavitation determined through erosion monitoring of thin sheets of aluminium foil. The implications of the studies for the development of reliable methods of quantifying the performance of cleaning vessels are discussed in detail.     

Properties of sound attenuation around a two-dimensional underwater vehicle with a large cavitation number

Due to the high speed of underwater vehicles,cavitation is generated inevitably along with the sound attenuation when the sound signal traverses through the cavity region around the underwater vehicle.The linear wave propagation is studied to obtain the influence of bubbly liquid on the acoustic wave propagation in the cavity region.The sound attenuation coefficient and the sound speed formula of the bubbly liquid are presented.Based on the sound attenuation coefficients with various vapor volume fractions,the attenuation of sound intensity is calculated under large cavitation number conditions.The result shows that the sound intensity attenuation is fairly small in a certain condition.Consequently,the intensity attenuation can be neglected in engineering.     

High-speed imaging of ultrasound driven cavitation bubbles in blind and through holes

The interest in application of ultrasonic cavitation for cleaning and surface treatment processes has increased greatly in the last decades. However, not much is known about the behavior of cavitation bubbles inside the microstructural features of the solid substrates. Here we report on an experimental study on dynamics of acoustically driven (38.5 kHz) cavitation bubbles inside the blind and through holes of PMMA plates by using high-speed imaging. Various diameters of blind (150, 200, 250 and 1000 µm) and through holes (200 and 1000 µm) were investigated. Gas bubbles are usually trapped in the holes during substrate immersion in the liquid thus preventing their complete wetting. We demonstrate that trapped gas can be successfully removed from the holes under ultrasound agitation. Besides the primary Bjerknes force and acoustic streaming, the shape oscillations of the trapped gas bubble seem to be a driving force for bubble removal out of the holes. We further discuss the bubble dynamics inside microholes for water and Cu²⁺ salt solution. It is found that the hole diameter and partly the type of liquid media influences the number, size and dynamics of the cavitation bubbles. The experiments also showed that a large amount of the liquid volume inside the holes can be displaced within one acoustic cycle by the expansion of the cavitation bubbles. This confirmed that ultrasound is a very effective tool to intensify liquid exchange processes, and it might significantly improve micro mixing in small structures. The investigation of the effect of ultrasound power on the bubble density distribution revealed the possibility to control the cavitation bubble distribution inside the microholes. At a high ultrasound power (31.5 W) we observed the highest bubble density at the hole entrances, while reducing the ultrasound power by a factor of ten shifted the bubble locations to the inner end of the blind holes or to the middle of the through holes.     

Spatial distribution of sonoluminescence and sonochemiluminescence generated by cavitation bubbles in 1.2 MHz focused ultrasound field

An intensified charge coupled device (ICCD) camera was used to observe the spatial distribution of sonoluminescence (SL) and sonochemiluminescence (SCL) generated by cavitation bubbles in a 1.2 MHz focused ultrasound (FU) field in order to investigate the mechanisms of acoustic cavitation under different sonication conditions for FU therapeutic applications.It was found that SL emissions were located in the post-focal region. When the intensity of SL and SCL increased as the power rose, the growth of SCL was much higher than that of SL. In the post-focal region, the SCL emissions moved along specific paths and formed branch-like streamers. At the beginning of the ultrasound irradiation, cavitation bubbles generated SCL in both the pre-focal and the post-focal region. When the electrical power or the sonication time increased, the SCL in the post-focal region increased and became higher than that in the pre-focal region. The intensity of SCL in the focal region is usually the weakest because of “oversaturation”.The spatial distribution of SCL near a tissue boundary differed from that obtained in free fields. It organized into special structures under different acoustic amplitudes. When the electrical power was relatively low, the SCL emission was conical shape which suggested a standing wave formation at the tissue-fluid boundary. When the electrical power exceeded a certain threshold, only a bright spot could be captured in the focus. The cavitation bubbles which centralized in the focus concentrated energy and hindered the formation of standing waves. With rising electrical power at high levels, besides a bright spot in the focus, there were some irregular light spots in pre-focal region, which indicated some cavitation bubbles or small bubble clusters achieved the threshold of SCL and induced the reaction with the luminol solution.     

Spatial-temporal dynamics of cavitation bubble clouds in 1.2 MHz focused ultrasound field

Cavitation bubbles have been recognized as being essential to many applications of ultrasound. Temporal evolution and spatial distribution of cavitation bubble clouds induced by a focused ultrasound transducer of 1.2 MHz center frequency are investigated by high-speed photography. It is revealed that at a total acoustic power of 72 W the cavitation bubble cloud first emerges in the focal region where cavitation bubbles are observed to generate, grow, merge and collapse during the initial 600 μs. The bubble cloud then grows upward to the post-focal region, and finally becomes visible in the pre-focal region. The structure of the final bubble cloud is characterized by regional distribution of cavitation bubbles in the ultrasound field. The cavitation bubble cloud structure remains stable when the acoustic power is increased from 25 W to 107 W, but it changes to a more violent form when the acoustic power is further increased to 175 W.     

Sonoluminescence

Sonoluminescence (SL) is the name given to the light emitted when a liquid is cavitated in a particular (rather violent) manner. The appropriate cavitation conditions can be realized by using high intensity ultrasound, a spark discharge, a laser pulse, or by flowing the liquid through a Venturi tube. SL occurs in a wide variety of liquids, its intensity and spectrum depending on the nature of the solvent and the solute (including dissolved gas). The intensity, but apparently not the spectrum, also depends on the frequency of the sound and on the temperature and hydrostatic pressure of the liquid. In a standing wave sound field the SL originates from bubbles attracted to the pressure antinodes and has its maximum intensity when the bubble volume is a minimum. The phase of the sound cycle at which this occurs depends on the amplitude and frequency of the sound field. Spectral measurements show that SL originates mainly from the recombination of free radicals created within the high temperature and high pressure environment of a bubble undergoing an adiabatic compression, as may happen either during transient cavitation or during highly non-linear, but stable, cavitation. In discussing these, and other, attributes of SL this review emphasizes developments over the past 20 years. Because of the importance of the dynamical theory of bubbles to a full understanding of SL, it includes an account of bubble dynamics. In addition, it describes the various experimental techniques employed in the creation and analysis of SL. Although the review lays particular stress on the SL produced via acoustic cavitation, it also examines the characteristics of the SL produced using other methods of cavitation.     

The size of active bubbles for the production of hydrogen in sonochemical reaction field

The sonication of aqueous solution generates microscopic cavitation bubbles that may growth and violently collapse to produce highly reactive species (i.e. OH, HO₂ and H₂O₂), hydrogen and emit light, sonoluminescence. The bubble size is a key parameter that influences the chemical activity of the system. This wok aims to study theoretically the size of active bubbles for the production of hydrogen in ultrasonic cavitation field in water using a single bubble sonochemistry model. The effect of several parameters such as frequency of ultrasound, acoustic intensity and liquid temperature on the range of sonochemically active bubbles for the production of hydrogen was clarified. The numerical simulation results showed that the size of active bubbles is an interval which includes an optimum value at which the production rate of H₂ is maximal. It was shown that the range of ambient radius for an active bubble as well as the optimum bubble radius for the production of hydrogen increased with increasing acoustic intensity and decreased with increasing ultrasound frequency and bulk liquid temperature. It was found that the range of ambient bubble radius dependence of the operational conditions followed the same trend as those reported experimentally for sonoluminescing bubbles. Comparison with literature data showed a good agreement between the theoretical determined optimum bubble sizes for the production of hydrogen and the experimental reported sizes for sonoluminescing bubbles.     

Uniform Acoustic Cavitation of Liquid in a Disk

A dynamical propagation model coupled to the oscillation of cavitation bubbles is applied to describe the imploding acoustic field in a cavitating liquid where the acoustic waves transmit from the outside to the inside of a circle disk. Numerical simulation shows that the imploding ability of a ring source can elevate the sound pressure or partly eliminate the decay due to both the bulk attenuation and the attenuation caused by cavitation. However,the imploding ability is limited and there exists a critical radius. When the radius of the disk is larger than the critical one, the imploding ability is not enough to eliminate the attenuation. Fortunately, the cavitation region can be effectively expanded if a hot plate is attached under the center of the disk because the cavitation threshold is related to the temperature of the liquid, which means that a region with good uniformity of cavitation can be enhanced by adjusting the temperature difference between the central and side liquid.     

Synchrotron quantification of ultrasound cavitation and bubble dynamics in Al–10Cu melts

Knowledge of the kinetics of gas bubble formation and evolution under cavitation conditions in molten alloys is important for the control casting defects such as porosity and dissolved hydrogen. Using in situ synchrotron X-ray radiography, we studied the dynamic behaviour of ultrasonic cavitation gas bubbles in a molten Al–10 wt% Cu alloy. The size distribution, average radius and growth rate of cavitation gas bubbles were quantified under an acoustic intensity of 800 W/cm² and a maximum acoustic pressure of 4.5 MPa (45 atm). Bubbles exhibited a log-normal size distribution with an average radius of 15.3 ± 0.5 μm. Under applied sonication conditions the growth rate of bubble radius, R(t), followed a power law with a form of R(t) = αt^β, and α = 0.0021 & β = 0.89. The observed tendencies were discussed in relation to bubble growth mechanisms of Al alloy melts.     

A feasibility study of temperature rise measurement in a tissue phantom as an alternative way for characterization of the therapeutic high intensity focused ultrasonic field

The feasibility that temperature field measurements in vitro as an alternative way to characterize the high intensity focused ultrasound (HIFU) field used in therapeutic applications has been explored in a phantom study. Thermocouples (copper-constantan, diameter 0.125 mm) are embedded in a phantom filled with tissue mimicking material that simulates the thermal and acoustic properties of soft-tissue. The temperature rises as a function of ultrasound exposure time near the focus of a HIFU transducer (1.1 MHz, active radius a = 32 mm, geometric focal length = 62 mm) of various acoustic powers up to 30 W are measured and compared with predicted values using a simple nonlinear Gaussian model. The experimental results can be explained well by the model if no acoustic cavitation takes place. When the acoustic power become higher (>5 W) and the local temperature elevation >15 °C and the local temperature is >40 °C at the focal point, cavitation vapor bubbles appear. The presence of the cavitation bubbles may increase the temperature rise rate initially. The bubble aggregates may form along the beam axis under sonication and then eventually makes the temperature elevation reach a saturated value. When acoustic cavitation occurs, the bubble-assisted enhancement of the initial temperature rise (exposure time t < 2 s) can still be predicted by the theory.     

Boiling-up of liquid argon at high superheatings under the impact of weak ultrasonic fields

The technique of lifetime measurement for metastable liquid and continuous depressurization technique were applied for study of kinetics of spontaneous cavitation in superheated liquid argon under impact of weak ultrasonic fields. It was demonstrated that acoustic cavitation may occur through the mechanism of homogeneous generation of vapor phase or through “swinging” of vapor bubbles generated by high-energy particles and/or other kinds of initiative factors. The thresholds of acoustic cavitation are described by the theory of homogeneous nucleation.     

含气泡液体中气泡振动的研究

研究了含气泡液体中单个气泡在驱动声场一定情况下的振动过程. 让每次驱动声场作用的时间特别短, 使气泡半径发生微小变化后再将其变化反馈到气泡群对驱动声场的散射作用中去, 从而可以得到某单个气泡周围受气泡散射影响后的声场, 接着再让气泡在该声场作用下做短时振动, 如此反复. 通过这样的方法, 研究了液体中单个气泡的振动情况并对其半径变化进行了数值模拟, 结果发现, 在液体中含有大量气泡的情况下, 某单个气泡的振动过程明显区别于液体中只有一个气泡的情况. 由于大量气泡和驱动声场的相互作用, 使气泡半径的变化存在多种不同的振动情况, 在不同的气泡大小和含量的情况下, 半径变化过程分别表现为: 在平衡位置附近振荡的过程; 周期性的空化过程; 一次空化过程后保持某一大小振荡的过程; 增长后维持某一大小振荡的过程等. 所以, 对于含气泡液体中气泡振动的研究, 在驱动声场一定的情况下, 必须考虑气泡含量的因素. 关键词： 含气泡液体 超声空化 散射 数值模拟     

Numerical study on the desorption processes of oil droplets inside oil-contaminated sand under cavitation micro-jets

The removal of the adsorbed oil droplet is critical to deoiling treatment of oil-bearing solid waste. Ultrasonic cavitation is regarded as an extremely useful method to assist the oil droplets desorption in the deoiling treatment. In this paper, the effects of cavitation micro-jets on the oil droplets desorption were studied. The adsorbed states of oil droplets in the oil-contaminated sand were investigated using a microscope. Three representative absorbed states of the oil droplets can be summarized as: (1) the individual oil droplet adsorbed on the particle surface (2) the clustered oil droplets adsorbed on the particle surface; (3) the oil droplet adsorbed in a gap between particles. The micro-jet generation during the bubble collapse near a rigid wall under different acoustic pressure amplitudes at an ultrasonic frequency of 20 kHz was investigated numerically. The desorption processes of the oil droplets at the three representative absorbed states under micro-jets were also simulated subsequently. The results showed that the acoustic pressure has a great influence on the velocity of micro-jet, and the initial diameter of cavitation bubbles is significant for the cross-sectional area of micro-jets. The wall jet caused by a micro-jet impacting on the solid wall is the most important factor for the removal of the absorbed oil droplets. The oil droplet is broken by the jet impinging, and then it breaks away from the solid wall due to the shear force generated by the wall jet. In addition to a higher sound pressure, the cavitation bubble at a larger initial diameter is more important for the desorption of the clustered oil droplets. Conversely, the micro-jet generated by the cavitation bubble at a smaller initial diameter (0.1 mm) is more appropriate for the desorption of the oil droplet in a narrow or sharp-angled gap.