Oscillations of polymeric microbubbles: effect of the encapsulating shell

A model for the oscillation of gas bubbles encapsulated in a thin shell has been developed. The model depends on viscous and elastic properties of the shell, described by thickness, shear modulus, and shear viscosity. This theory was used to describe an experimental ultrasound contrast agent from Nycomed, composed of air bubbles encapsulated in a polymer shell. Theoretical calculations were compared with measurements of acoustic attenuation at amplitudes where bubble oscillations are linear. A good fit between measured and calculated results was obtained. The results were used to estimate the viscoelastic properties of the shell material. The shell shear modulus was estimated to between 10.6 and 12.9 MPa, the shell viscosity was estimated to between 0.39 and 0.49 Pas. The shell thickness was 5% of the particle radius. These results imply that the particles are around 20 times more rigid than free air bubbles, and that the oscillations are heavily damped, corresponding to Q-values around 1. We conclude that the shell strongly alters the acoustic behavior of the bubbles: The stiffness and viscosity of the particles are mainly determined by the encapsulating shell, not by the air inside.     

Modeling non-spherical oscillations and stability of acoustically driven shelled microbubbles

The oscillation and destruction of microbubbles under ultrasound excitation form the basis of contrast enhanced ultrasound imaging and microbubble assisted drug and gene delivery. A typical microbubble has a size of a few micrometers and consists of a gas core encapsulated by a shell. These bubbles can be driven into surface mode oscillations, which not only contribute to the measured acoustic signal but can lead to bubble destruction. Existing models of surface model oscillations have not considered the effects of a bubble shell. In this study a model was developed to study the surface mode oscillations in shelled bubbles. The effects of shell viscosity and elasticity on the surface mode oscillations were modeled using a Boussinesq-Scriven approach. Simulation was conducted using the model with various bubble sizes and driving acoustic pressures. The occurrence of surface modes and the number of ultrasound cycles needed for the occurrence were calculated. The simulation results show a significant difference between shelled bubbles and shell free bubbles. The shelled bubbles have reduced surface mode amplitudes and a narrower bubble size range within which these modes develop compared to shell free bubbles. The clinical implications were also discussed.     

Ultrasonic scattering cross sections of shell-encapsulated gas bubbles immersed in a viscoelastic liquid: first and second harmonics

The oscillations of gas bubbles, without shell, immersed in viscoelastic liquids and driven by an acoustic wave have been the subject of several investigations. They demonstrate that the viscosity coefficient and the spring constant of the liquid have significant influence on the scattering cross section of the gas bubble. For shell-encapsulated gas bubbles, the investigations have been concentrated to bubbles immersed in a pure viscous liquid. This present work computes the ultrasonic scattering cross section, first and second harmonics, of shell-encapsulated gas bubbles immersed in a viscoelastic liquid. The theoretical model of the bubble oscillation is based on the generalized Rayleigh-Plesset equation of motion of a spherical cavity immersed in a viscoelastic liquid represented by a three-parameter linear Oldroyd model. The scattering cross section is computed for Albunex type of bubble (shell thickness=15 nm, shell shear viscosity=1.77 Pas, shell modulus of rigidity=88.8 MPa) irradiated by a 3.5 MHz ultrasonic pressure wave with an amplitude of 30 kPa. The results demonstrate that encapsulated bubbles respond independently of the surrounding liquid being pure viscous or viscoelastic as long as the surrounding liquid shear viscosity is as low as 10(-3) Pas. Nevertheless, for higher shear viscosities, the bubble responds differently if the surrounding liquid is pure viscous or viscoelastic. In general, the scattering cross sections of first and second harmonics are larger for the viscoelastic liquid.     

Contributions to the acoustic excitation of bubbles released from a nozzle

It has recently been demonstrated that air bubbles released from a nozzle are excited into volume mode oscillations by the collapse of the neck of air formed at the moment of bubble detachment. A pulse of sound is caused by these breathing mode oscillations, and the sound of air-entraining flows is made up of many such pulses emitted as bubbles are created. This paper is an elaboration on a JASA-EL paper, which examined the acoustical excitation of bubbles released from a nozzle. Here, further details of the collapse of a neck of air formed at the moment of bubble formation and its implications for the emission of sound by newly formed bubbles are presented. The role of fluid surface tension was studied using high-speed photography and found to be consistent with a simple model for neck collapse. A re-entrant fluid jet forms inside the bubble just after detachment, and its role in acoustic excitation is assessed. It is found that for slowly-grown bubbles the jet does make a noticeable difference to the total volume decrease during neck collapse, but that it is not a dominant effect in the overall acoustic excitation.     

Subharmonic behavior of phospholipid-coated ultrasound contrast agent microbubbles

Coated microbubbles, unlike tissue are able to scatter sound subharmonically. Therefore, the subharmonic behavior of coated microbubbles can be used to enhance the contrast in ultrasound contrast imaging. Theoretically, a threshold amplitude of the driving pressure can be calculated above which subharmonic oscillations of microbubbles are initiated. Interestingly, earlier experimental studies on coated microbubbles demonstrated that the threshold for these bubbles is much lower than predicted by the traditional linear viscoelastic shell models. This paper presents an experimental study on the subharmonic behavior of differently sized individual phospholipid coated microbubbles. The radial subharmonic response of the microbubbles was recorded with the Brandaris ultra high-speed camera as a function of both the amplitude and the frequency of the driving pulse. Threshold pressures for subharmonic generation as low as 5 kPa were found near a driving frequency equal to twice the resonance frequency of the bubble. An explanation for this low threshold pressure is provided by the shell buckling model proposed by Marmottant et al. [J. Acoust. Soc. Am. 118, 3499-3505 (2005)]. It is shown that the change in the elasticity of the bubble shell as a function of bubble radius as proposed in this model, enhances the subharmonic behavior of the microbubbles.     

多层膜磁性微泡的非线性声振动特性

超顺磁性氧化铁纳米粒子与造影剂微泡结合形成磁性微泡,用于产生多模态造影剂,以增强医学超声和磁共振成像.将装载有纳米磁性颗粒的微泡包膜层看作由磁流体膜与磷脂膜组合而成的双层膜结构,同时考虑磁性纳米颗粒体积分数a对膜密度及黏度的影响,从气泡动力学基本理论出发,构建多层膜结构磁性微泡非线性动力学方程.数值分析了驱动声压和频率等声场参数、颗粒体积分数、膜层厚度以及表面张力等膜壳参数对微泡声动力学行为的影响.结果表明,当磁性颗粒体积分数较小且a≤0.1时,磁性微泡声响应特性与普通包膜微泡相似,微泡的声频响应与其初始尺寸和驱动压有关;当驱动声场频率f为磁性微泡共振频率f0的2倍(f=2f0)时,微泡振动失稳临界声压最低;磁性颗粒的存在抑制了泡的膨胀和收缩但抑制效果非常有限;磁性微泡外膜层材料的表面张力参数K及膜层厚度d也会影响微泡的振动,当表面张力参数及膜厚取值分别为0.2—0.4 N/m及50—150 nm时,可观察到气泡存在不稳定振动响应区.     

Dynamics of a bubble cluster in an acoustic field

A mathematical model describing the dynamics of clustered gas bubbles under the effect of an acoustic field is presented. The proposed model is used as the basis for an analytical study of small bubble oscillations in monodisperse and polydisperse clusters and for a numerical study of nonlinear bubble oscillations under high-amplitude external pressures. The following effects are found to occur in a polydisperse cluster: a synchronization of the collapse phases of bubbles with different radii and a collapse intensification for bubbles of one size in the presence of bubbles of another size. These effects are explained by the interaction between bubbles of different radii in the cluster.     

球状泡群内气泡的耦合振动

振动气泡形成辐射场影响其他气泡的运动, 故多气泡体系中气泡处于耦合振动状态. 本文在气泡群振动模型的基础上, 考虑气泡间耦合振动的影响, 得到了均匀球状泡群内振动气泡的动力学方程, 以此为基础分析了气泡的非线性声响应特征. 气泡间的耦合振动增加了系统对每个气泡的约束, 降低了气泡的自然共振频率, 增强了气泡的非线性声响应. 随着气泡数密度的增加, 振动气泡受到的抑制增强; 增加液体静压力同样可抑制泡群内气泡的振动, 且存在静压力敏感区(1–2 atm, 1 atm=1.01325×10⁵ Pa); 驱动声波对气泡振动影响很大, 随着声波频率的增加, 能够形成空化影响的气泡尺度范围变窄. 在同样的声条件、泡群尺寸以及气泡内外环境下, 初始半径小于5 μm 的气泡具有较强的声响应. 气泡耦合振动会削弱单个气泡的空化影响, 但可延长多气泡系统空化泡崩溃发生的时间间隔和增大作用范围, 整体空化效应增强.     

Nonlinear raman-type acoustic scattering in three-phase marine sediments

Stimulated Raman-type acoustic scattering by bubble oscillations in three-phase marine sediments, which consist of a solid frame, the pore water, and air bubbles, is considered. A model is developed for the case of the bubbles surrounded by water. The acoustic properties of the sediments are described on the basis of the Biot theory of sound propagation in a fluid-saturated porous medium. Nonlinear wave equations are obtained for marine sediments containing air bubbles. Expressions for the nonlinear scattering coefficient and the threshold intensity of the exciting sound wave are derived. A possibility of an experimental observation of the scattering process is discussed.     

Nonlinear oscillation and acoustic scattering of bubbles

The scattered acoustic pressure and scattered cross section of bubbles is studied using the scattered theory of bubbles. The nonlinear oscillations of bubbles and the scattering acoustic fields of a spherical bubble cluster are numerically simulated based on the bubble dynamic and fluid dynamic. The influences of the interaction between bubbles on scattering acoustic field of bubbles are researched. The results of numerical simulation show that the oscillation phases of bubbles are delayed to a certain extent at different positions in the bubble cluster, but the radii of bubbles during oscillation do not differ too much at different positions. Furthermore, directivity of the acoustic scattering of bubbles is obvious. The scattered acoustic pressures of bubbles are different at the different positions inside and outside of the bubble cluster. The scattering acoustic fields of a spherical bubble cluster depend on the driving pressure amplitude, driving frequency, the equilibrium radii of bubbles, bubble number and the radius of the spherical bubble cluster. These theoretical predictions provide a further understanding of physics behind ultrasonic technique and should be useful for guiding ultrasonic application.     

The dependence of ultrasound contrast agents backscatter on acoustic pressure: theory versus experiment

Experimental investigations have not fully explored the interaction between ultrasound beams and microbubble contrast agents. Moreover theoretical investigations have not solved the problem of the microbubble oscillation. A simple in-vitro system based on a commercial scanner (ATL UM9) was used to insonate (3 MHz transmission) diluted contrast suspensions of Definity and Quantison at different acoustic pressures (0.27-1.52 MPa). The experimental data were referred to a blood mimicking fluid in order to extract an estimate of their scattering cross-section. The results were compared with the solutions of the three main bubble oscillatidn models, Rayleigh-Plesset, Herring and Gilmore. Non-linear solutions of the above models were produced numerically using the Mathematica Package Software. The experiments showed that both agents provided a linear increase in scattering cross-section with increasing acoustic pressure. The thick shelled Quantison provided an increasing number of scatterers with increasing acoustic pressure, which proved that free bubbles leaked out of the shell. At high acoustic pressures both Quantison and Definity scattering cross-sections were almost identical, and were probably that of a free bubble. The Rayleigh-Plesset model provided a scattering cross-section almost independent of acoustic pressure. On the contrary the scattering cross-sections calculated by the Herring and Gilmore models solutions displayed a definite dependence on acoustic pressure of an order higher than one, which is slightly higher than the order of dependence exhibited by the experimental data. However, the increase of the experimentally measured scattering cross-section with acoustic pressure was sharper than the calculated one by the above two models. This is most probably due to the fact that the models simulated damped and not free bubble oscillations. In conclusion the Rayleigh-Plesset model was inadequate in describing the bubble oscillations even at small diagnostic acoustic pressures. The Herring and Gilmore models could simulate the dependence of the scattering cross-section of encapsulated microbubbles on acoustic pressure. However the contribution of free bubble oscillations has still to be modelled.     

Nonlinear radial oscillations of encapsulated microbubbles subject to ultrasound: the effect of membrane constitutive law

The nonlinear radial oscillations of bubbles that are encapsulated in an elastic shell are investigated numerically subject to three different constitutive laws describing the viscoelastic properties of the shell: the Mooney-Rivlin (MR), the Skalak (SK), and the Kelvin-Voigt (KV) models are used in order to describe strain-softening, strain-hardening and small displacement (Hookean) behavior of the shell material, respectively. Due to the isotropic nature of the acoustic disturbances, the area dilatation modulus is the important parameter. When the membrane is strain softening (MR) the resonance frequency decreases with increasing sound amplitude, whereas the opposite happens when the membrane is strain hardening (SK). As the amplitude of the acoustic disturbance increases the total scattering cross section of a microbubble with a SK membrane tends to decrease, whereas that of a KV or a MR membrane tends to increase. The importance of strain-softening behavior in the abrupt onset of volume pulsations, that is often observed with small insonated microbubbles at moderately large sound amplitudes, is discussed.     

Resonance frequencies of lipid-shelled microbubbles in the regime of nonlinear oscillations

Knowledge of resonant frequencies of contrast microbubbles is important for the optimization of ultrasound contrast imaging and therapeutic techniques. To date, however, there are estimates of resonance frequencies of contrast microbubbles only for the regime of linear oscillation. The present paper proposes an approach for evaluating resonance frequencies of contrast agent microbubbles in the regime of nonlinear oscillation. The approach is based on the calculation of the time-averaged oscillation power of the radial bubble oscillation. The proposed procedure was verified for free bubbles in the frequency range 1-4 MHz and then applied to lipid-shelled microbubbles insonified with a single 20-cycle acoustic pulse at two values of the acoustic pressure amplitude, 100 kPa and 200 kPa, and at four frequencies: 1.5, 2.0, 2.5, and 3.0 MHz. It is shown that, as the acoustic pressure amplitude is increased, the resonance frequency of a lipid-shelled microbubble tends to decrease in comparison with its linear resonance frequency. Analysis of existing shell models reveals that models that treat the lipid shell as a linear viscoelastic solid appear may be challenged to provide the observed tendency in the behavior of the resonance frequency at increasing acoustic pressure. The conclusion is drawn that the further development of shell models could be improved by the consideration of nonlinear rheological laws.     

Theoretical estimation of sonochemical yield in bubble cluster in acoustic field

In order to learn more about the physical phenomena occurring in cloud cavitation, the nonlinear dynamics of a spherical cluster of cavitation bubbles and cavitation bubbles in cluster in an acoustic field excited by a square pressure wave are numerically investigated by considering viscosity, surface tension, and the weak compressibility of the liquid.The theoretical prediction of the yield of oxidants produced inside bubbles during the strong collapse stage of cavitation bubbles is also investigated. The effects of acoustic frequency, acoustic pressure amplitude, and the number of bubbles in cluster on bubble temperature and the quantity of oxidants produced inside bubbles are analyzed. The results show that the change of acoustic frequency, acoustic pressure amplitude, and the number of bubbles in cluster have an effect not only on temperature and the quantity of oxidants inside the bubble, but also on the degradation types of pollutants, which provides a guidance in improving the sonochemical degradation of organic pollutants.     

Theoretical prediction of the yield of strong oxides under acoustic cavitation

Considering liquid viscosity, surface tension, and liquid compressibility, the effects of dynamical behaviors of cavitation bubbles on temperature and the amount of oxides inside the bubble are numerically investigated by acoustic field,regarding water as a work medium. The effects of acoustic frequency, acoustic pressure amplitude, and driving waveforms on bubble temperature and the number of oxides inside the bubbles by rapid collapse of cavitation bubbles are analysed.The results show that the changes of acoustic frequency, acoustic pressure amplitude, and driving waveforms not only have an effect on temperature and the number of oxides inside the bubble, but also influence the degradation species of pollution,which provides guidance for improving the degradation of water pollution.     

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.     

Enhancement of oscillation amplitude of cavitation bubble due to acoustic wake effect in multibubble environment

Acoustic cavitation occurs in ultrasonic treatment causing various phenomena such as chemical synthesis, chemical decomposition, and emulsification. Nonlinear oscillations of cavitation bubbles are assumed to be responsible for these phenomena, and the neighboring bubbles may interact each other. In the present study, we numerically investigated the dynamic behavior of cavitation bubbles in multi-bubble systems. The results reveal that the oscillation amplitude of a cavitation bubble surrounded by other bubbles in a multi-bubble system becomes larger compared with that in the single-bubble case. It is found that this is caused by an acoustic wake effect, which reduces the pressure near a bubble surrounded by other bubbles and increases the time delay between the bubble contraction/expansion cycles and sound pressure oscillations. A new parameter, called “cover ratio” is introduced to quantitatively evaluate the variation in the bubble oscillation amplitude, the time delay, and the maximum bubble radius.     

Collective bubble dynamics near a surface in a weak acoustic standing wave field

The transport of bubbles to a neighboring surface is very important in surface chemistry, bioengineering, and ultrasonic cleaning, etc. This paper proposes a multi-bubble transport method by using an acoustic standing wave field and establishes a model that explains the multi-bubble translation by expressing the balance between Bjerknes forces and hydrodynamic forces on a bubble in a liquid medium. Results indicated that the influence of primary Bjerknes force, secondary Bjerknes force, and buoyancy force on the bubble translation depends on the position of the target bubble in the acoustic field. Moreover, it was found that increasing the size of a bubble or pressure amplitude can accelerate the bubble motion and enhance the bubble-bubble interaction. The secondary Bjerknes force between two bubbles can switch from an attractive one when they oscillate in phase to a repulsive one when the bubble oscillations are out of phase. These findings provide an insight into the multi-bubble translation near a surface and can be applied to future bubble motion control studies, especially in drug delivery, sonoporation, and ultrasonic cleaning.     

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.     

Nonlinear dynamics and bifurcation structure of ultrasonically excited lipid coated microbubbles

In many applications, microbubbles (MBs) are encapsulated by a lipid coating to increase their stability. However, the complex behavior of the lipid coating including buckling and rupture sophisticates the dynamics of the MBs and as a result the dynamics of the lipid coated MBs (LCMBs) are not well understood. Here, we investigate the nonlinear behavior of the LCMBs by analyzing their bifurcation structure as a function of acoustic pressure. We show that, the LC can enhance the generation of period 2 (P2), P3, higher order subharmonics (SH), superharmonics and chaos at very low excitation pressures (e.g. 1 kPa). For LCMBs sonicated by their SH resonance frequency and in line with experimental observations with increasing pressure, P2 oscillations exhibit three stages: generation at low acoustic pressures, disappearance and re-generation. Within non-destructive oscillation regimes and by pressure amplitude increase, LCMBs can also exhibit two saddle node (SN) bifurcations resulting in possible abrupt enhancement of the scattered pressure. The first SN resembles the pressure dependent resonance phenomenon in uncoated MBs and the second SN resembles the pressure dependent SH resonance. Depending on the initial surface tension of the LCMBs, the nonlinear behavior may also be suppressed for a wide range of excitation pressures.