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.     

Influence of bubble clustering on multibubble sonoluminescence

Influence of clustering of cavitation bubbles on multibubble sonoluminescence (MBSL) in standing wave fields is studied through measurement of MBSL intensity with a photomultiplier tube and observation of corresponding bubble behavior with a high-speed video camera and an intensified charge-coupled device one. It is clarified that, when the SL is quenched suddenly at excessive ultrasonic power, the behavior of bubbles clearly changes; the bubbles which form dendritic branches of filaments change into clusters due to the secondary Bjerknes force. The cluster is composed of several bubbles surrounded by many tiny bubbles, in which bubbles repeatedly coalesce and fragment, and run away from pressure antinodes. When the clusters are broken up by forced fluid motion, the quenching of MBSL is suppressed.     

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.     

Characterization of cavitation in a flow-through exposure chamber by means of a resonant bubble detector

Ultrasonic cavitation at frequencies of 0.514, 0.866, 1.03 and 1.61 MHz in water flowing through tubes was observed by counting bubbles downstream with a resonant bubble detector (RBD) operated at 0.89 or 1.7 MHz. In a 21 mm diameter, thin-walled tube, cavitation thresholds in tap water flowing at 5.3 cm s^?1 ranged from 2.0 – 2.5 bar at 0.514 MHz to 3 – 4 bar at 1.61 MHz. When high speed injections were employed to trigger the ultrasonic cavitation with hydrodynamically-generated bubbles, the thresholds were reduced to about 2 bar and bubble production was enhanced for 1.03 and 1.61 MHz exposures. Ultrasonic radiation forces on the bubbles and bubble coalescence appeared to cause, under some conditions, a reduction in bubble counts during subthreshold exposures when bubbles were injected into the flow. The RBD method is a useful tool for detecting and semi-quantitatively observing cavitation in a flow-through exposure system.     

The influence of pressure on the acoustic cavitation in saturated CO2-expanded N,N-dimethylformamide

CO₂-expanded organic solvent is a kind of important fluid medium and has broad applications in chemical industry, environmental protection and other fields. Ultrasonic cavitation in gas expanded liquids (GXLs) is conducive to enhancing mass transfer and producing many exciting phenomena. In this paper, the ultrasonic cavitations and streaming in the saturated CO₂-expanded liquid N, N-dimethylformamide (DMF) at 4.2 MPa and 5.2 MPa are observed by a high-speed camera. The cavitation intensity and time trace of pressure pulses are recorded using a PZT hydrophone. The influences of gas–liquid equilibrium pressure and ultrasonic power on the cluster dynamics of transient and stable cavitation are examined. The excess molar enthalpies required for CO₂ dissociation from DMF are calculated by Peng-Robinson equations of state and the change of surface free energy of CO₂-expanded DMF is predicted. The results show that the excess enthalpy of the mixture is one of the key factors to control ultrasonic cavitation at high pressurized conditions, while the surface tension is the key factor for low pressure. As the increase of applied ultrasonic power, the formation and collapsing frequency of bubble clusters increases, and the amplitude and cyclic frequency of pressure pulse are enhanced. The transient cavitation intensity increases as it reaches a maximum value at a certain ultrasonic power and then decreases. The change trends of stable cavitation intensity under different pressures are basically same. It can be concluded from the evidence that ultrasonic cavitation in CO₂-expanded DMF is affected by the combined effect of compression and substitution: compression depresses the nucleation and growth of bubbles, while the high solubility of CO₂ in DMF is conducive to the generation of bubbles in cavitation.     

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.     

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.     

Sonoluminescence and sonochemiluminescence from a microreactor

Micromachined pits on a substrate can be used to nucleate and stabilize microbubbles in a liquid exposed to an ultrasonic field. Under suitable conditions, the collapse of these bubbles can result in light emission (sonoluminescence, SL). Hydroxyl radicals (OH()) generated during bubble collapse can react with luminol to produce light (sonochemiluminescence, SCL). SL and SCL intensities were recorded for several regimes related to the pressure amplitude (low and high acoustic power levels) at a given ultrasonic frequency (200kHz) for pure water, and aqueous luminol and propanol solutions. Various arrangements of pits were studied, with the number of pits ranging from no pits (comparable to a classic ultrasound reactor), to three-pits. Where there was more than one pit present, in the high pressure regime the ejected microbubbles combined into linear (two-pits) or triangular (three-pits) bubble clouds (streamers). In all situations where a pit was present on the substrate, the SL was intensified and increased with the number of pits at both low and high power levels. For imaging SL emitting regions, Argon (Ar) saturated water was used under similar conditions. SL emission from aqueous propanol solution (50mM) provided evidence of transient bubble cavitation. Solutions containing 0.1mM luminol were also used to demonstrate the radical production by attaining the SCL emission regions.     

Comparisons of sonoluminescence from single-bubbles and cavitation fields: bridging the gap

Sonoluminescence (SL) refers to the generation of light through the energetic pulsations of acoustic cavitation bubbles in a liquid. For years, SL was observed primarily in cavitation fields. These bubbles are believed by many to undergo near-adiabatic compression, resulting in the heating of the bubble contents and the subsequent emission of light. Recently, researchers have discovered a 'new' form of sonoluminescence in which light is observed to emanate from a single bubble undergoing very large volume excursions. The mechanism for light production is unknown, but many believe it is due to a rapid heating of the central core by an imploding shock wave. Based in part on the emission time scales, there is a common belief that the two forms of SL are quite distinct. We address this issue by comparing the two phenomena with regards to their light-flash durations and emission spectra--leading to some surprising differences and similarities.     

A two-dimensional nonlinear model for the generation of stable cavitation bubbles

Bubbles appear by acoustic cavitation in a liquid when rarefaction pressures attain a specific threshold value in a liquid. Once they are created, the stable cavitation bubbles oscillate nonlinearly and affect the ultrasonic field. Here we present a model developed for the study of bubble generation in a liquid contained in a two-dimensional cavity in which a standing ultrasonic field is established. The model considers dissipation and dispersion due to the bubbles. It also assumes that both the ultrasonic field and the bubble oscillations are nonlinear. The numerical experiments predict where the bubbles are generated from a population of nuclei distributed in the liquid and show how they affect the ultrasonic field.     

Acoustic cavitation mechanism: a nonlinear model

During acoustic cavitation process, bubbles appear when acoustic pressure reaches a threshold value in the liquid. The ultrasonic field is then submitted to the action of the bubbles. In this paper we develop a model to analyze the cavitation phenomenon in one-dimensional standing waves, based on the nonlinear code SNOW-BL. Bubbles are produced where the minimum rarefaction pressure peak exceeds the cavitation threshold. We show that cavitation bubbles appear at high amplitude and drastically affect (dissipation, dispersion, and nonlinearity) the ultrasonic field. This paper constitutes the first work that associates the nonlinear ultrasonic field to a bubble generation process.     

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.     

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.     

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.     

Acoustic power dependences of sonoluminescence and bubble dynamics

The decreasing effect of sonoluminescence (SL) in water at high acoustic powers was investigated in relation to bubble dynamics and acoustic emission spectra. The intensity of SL was measured in the power range of 1–18 W at 83.8 kHz for open-end (free liquid surface and film-covered surface) and fixed-end boundaries of sound fields. The power dependence of the SL intensity showed a maximum and then decrease to zero for all the boundaries. Similar results were obtained for sonochemiluminescence in luminol solution. The power dependence of the SL intensity was strongly correlated with the bubble dynamics captured by high-speed photography at 64 k fps. In the low-power range where the SL intensity increases, bubble streamers were observed and the population of streaming bubbles increased with the power. At powers after SL maximum occurred, bubble clusters came into existence. Upon complete SL reduction, only bubble clusters were observed. The subharmonic in the acoustic emission spectra increased markedly in the region where bubble clusters were observed. Nonspherical oscillations of clustering bubbles may make a major contribution to the subharmonic.     

Study on the bubble transport mechanism in an acoustic standing wave field

The use of bubbles in applications such as surface chemistry, drug delivery, and ultrasonic cleaning etc. has been enormously popular in the past two decades. It has been recognized that acoustically-driven bubbles can be used to disturb the flow field near a boundary in order to accelerate physical or chemical reactions on the surface. The interactions between bubbles and a surface have been studied experimentally and analytically. However, most of the investigations focused on violently oscillating bubbles (also known as cavitation bubble), less attention has been given to understand the interactions between moderately oscillating bubbles and a boundary. Moreover, cavitation bubbles were normally generated in situ by a high intensity laser beam, little experimental work has been carried out to study the translational trajectory of a moderately oscillating bubble in an acoustic field and subsequent interactions with the surface. This paper describes the design of an ultrasonic test cell and explores the mechanism of bubble manipulation within the test cell. The test cell consists of a transducer, a liquid medium and a glass backing plate. The acoustic field within the multi-layered stack was designed in such a way that it was effectively one dimensional. This was then successfully simulated by a one dimensional network model. The model can accurately predict the impedance of the test cell as well as the mode shape (distribution of particle velocity and stress/pressure field) within the whole assembly. The mode shape of the stack was designed so that bubbles can be pushed from their injection point onto a backing glass plate. Bubble radial oscillation was simulated by a modified Keller–Miksis equation and bubble translational motion was derived from an equation obtained by applying Newton’s second law to a bubble in a liquid medium. Results indicated that the bubble trajectory depends on the acoustic pressure amplitude and initial bubble size: an increase of pressure amplitude or a decrease of bubble size forces bubbles larger than their resonant size to arrive at the target plate at lower heights, while the trajectories of smaller bubbles are less influenced by these factors. The test cell is also suitable for testing the effects of drag force on the bubble motion and for studying the bubble behavior near a surface.     

High-speed imaging of ultrasonic emulsification using a water-gallium system

Aiming at elucidating ultrasonic emulsification mechanisms, the interaction between a single or multiple acoustic cavitation bubbles and gallium droplet interface was investigated using an high-speed imaging technique. To our best knowledge, the moment of emulsification and formation of fine droplets during ultrasound irradiation were observed for the first time. It was found that the detachment of fine gallium droplets occurs from the water-gallium interface during collapse of big cavitation bubbles. The results suggest that the maximum size of cavitation bubble before collapsing is of prime importance for emulsification phenomena. Previous numerical simulation revealed that the collapse of big cavitation bubble is followed by generation of high-velocity liquid jet directed toward the water-gallium interface. Such a jet is assumed to be the prime cause of liquid emulsification. The distance between cavitation bubbles and water-gallium interface was found to slightly affect the emulsification onset. The droplet fragmentation conditions are also discussed in terms of the balance between (1) interfacial and kinetic energies and (2) dynamic and Laplace pressure during droplet formation.     

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     

Effects of surface tension on the dynamics of a single micro bubble near a rigid wall in an ultrasonic field

Acoustic cavitation is a very important hydrodynamic phenomenon, and is often implicated in a myriad of industrial, medical, and daily living applications. In these applications, the effect mechanism of liquid surface tension on improving the efficiency of acoustic cavitation is a crucial concern for researchers. In this study, the effects of liquid surface tension on the dynamics of an ultrasonic driven bubble near a rigid wall, which could be the main mechanism of efficiency improvement in the applications of acoustic cavitation, were investigated at the microscale level. A synchronous high-speed microscopic imaging method was used to clearly record the temporary evolution of single acoustic cavitation bubble in the liquids with different surface tension. Meanwhile, the bubble dynamic characteristics, such as the position and time of bubble collapse, the size and stability of the bubbles, the speed of bubble boundaries and the micro-jets, were analyzed and compared. In the case of the single bubbles near a rigid wall, it was found that low surface tension reduces the stability of the bubbles in the liquid medium. Meanwhile, the bubbles collapse earlier and farther from the rigid wall in the liquids with lower surface tension. In addition, the surface tension has no significant influence on the speed of the first micro-jet, but it can substantially increase the speed of second and the third micro-jets after the first collapse of the bubble. These effects of liquid surface tension on the bubble dynamics can explain the mechanism of surfactants in numerous fields of acoustic cavitation for facilitating its optimization and application.     

Influence of bulk nanobubble concentration on the intensity of sonoluminescence

The present study mainly examined the effects of the volumetric concentration of nanobubbles (ultrafine bubbles) on the intensity of sonoluminescence (SL). The addition of nanobubbles at high acoustic amplitude enhanced the SL intensity for various bubble concentrations in comparison with that in pure water. This probably means that the resulting high amplitude is over the Blake threshold, and accordingly nanobubbles expand to some extent, leading to higher SL intensity. Therefore, nanobubbles have the potential to provide nucleation sites for sonochemistry. The influence of bubble size on the intensity of SL was also evaluated.