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.     

The effect of bulk viscosity on single bubble dynamics and sonoluminescence

In our previous paper, we derived a new single bubble model including the effect of bulk viscosity. To confront it to experiments, single bubble dynamics was measured here in 30% (v/v) glycerol-water mixture under different acoustic amplitudes and compared to models including or not the effect of bulk viscosity. The results showed that calculated bubble dynamics were not significantly affected by the bulk viscosity within the experimental conditions used in this study. However, there was a noticeable delay for the first rebound when bulk viscosity was considered. The corresponding sonoluminescence intensities were collected and compared with theoretical predictions. The results did not allow to discriminate between the two models (one includes the effect of bulk viscosity, the other does not), confirming the negligible effect of bulk viscosity in this condition (30% (v/v) glycerol-water mixture). Due to the instability of a single bubble in higher viscosity solutions, we could not implement experiments that can discriminate between the two models.     

稀土盐水溶液单泡声致发光中的特征光谱

在溶有稀有气体的稀土盐氯化铽水溶液中进行了单泡声致发光光谱的研究. 在固定驱动超声频率、不同驱动声压下, 观察到了一系列OH自由基从第一激发态A²∑⁺到基态X²Π 各振动能级跃迁所产生的谱线, 包括波长307 nm处的(0, 0)跃迁谱线, 335 nm处的(0, 1)跃迁谱线以及276 nm处的(1, 0) 跃迁谱线等. 实验结果表明较高的驱动声压有利于 276 nm处谱线的产生, 而较低的驱动声压则有利于 307 与 335 nm 处谱线的产生. 通过定义线状光谱与连续谱的光强比, 定量地表征了线状光谱在总光谱中的相对强度, 并给出了驱动声压对各跃迁谱线光强比的影响. 关键词： 单泡声致发光 驱动声压 线状光谱 光强比     

Sonoluminescence and dynamics of cavitation bubble populations in sulfuric acid

The detailed link of liquid phase sonochemical reactions and bubble dynamics is still not sufficiently known. To further clarify this issue, we image sonoluminescence and bubble oscillations, translations, and shapes in an acoustic cavitation setup at 23 kHz in sulfuric acid with dissolved sodium sulfate and xenon gas saturation. The colour of sonoluminescence varies in a way that emissions from excited non-volatile sodium atoms are prominently observed far from the acoustic horn emitter (“red region”), while such emissions are nearly absent close to the horn tip (“blue region”). High-speed images reveal the dynamics of distinct bubble populations that can partly be linked to the different emission regions. In particular, we see smaller strongly collapsing spherical bubbles within the blue region, while larger bubbles with a liquid jet during collapse dominate the red region. The jetting is induced by the fast bubble translation, which is a consequence of acoustic (Bjerknes) forces in the ultrasonic field. Numerical simulations with a spherical single bubble model reproduce quantitatively the volume oscillations and fast translation of the sodium emitting bubbles. Additionally, their intermittent stopping is explained by multistability in a hysteretic parameter range. The findings confirm the assumption that bubble deformations are responsible for pronounced sodium sonoluminescence. Notably the observed translation induced jetting appears to serve as efficient mixing mechanism of liquid into the heated gas phase of collapsing bubbles, thus potentially promoting liquid phase sonochemistry in general.     

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.     

High-speed video microscopy and computer enhanced imagery in the pursuit of bubble dynamics

The equipment and method for studying transient bubble dynamics are described in simple sonochemical reactors and presented using still frames from high-speed video microscopy (500 fps). Effects on aeration bubbles (mean size 1–3 mm diameter) and the cavitation induced species (<0.5 mm diameter) are studied. The images are computer enhanced to improve interpretation of such features as the maximum ellipsoidal distortion at the nodal sound plane and spherical shape regain with due consideration of energy involved and expansion effects at the nodal sound plane. Also immersion depth/pressure effects, as the bubbles transcend the sound field column, in the cylindrical reactor, are recorded for evaluation of nodal and antinodal sound wave effects. Positions of the nodal and antinodal regions are marked using a novel tungsten halogen bulb technique and verified using the sonoelectroluminescent approach with the classical luminol/hydrogen peroxide chemistry which is enhanced under the sound field conditions.     

Two components of Na emission in sonoluminescence spectrum from surfactant aqueous solutions

Sonoluminescence from sodium dodecyl sulfate (SDS) aqueous solutions exhibits Na emission. The spectrum of Na emission was measured as a function of sonication time for a total of 30 min at an ultrasonic frequency of 148 kHz. The spectral line profiles changed with the sonication time, suggesting that the Na emission consists of two components: broadened lines, which are shifted from the original D lines, and unshifted narrow lines. The intensity of the unshifted narrow lines decreased at a greater rate than that of the broadened lines with increasing sonication time. This effect was enhanced at a higher acoustic power. The shifted broadened lines remained after sonication for 30 min. We propose that these quenching effects are caused by the accumulation of gases decomposed from SDS molecules inside bubbles. The CO₂ gas dependence of Na emission in NaCl aqueous solutions showed a similar change in the line profiles to that in SDS aqueous solutions, which supported this proposition. The unshifted narrow lines are easily affected by foreign gases. The results suggest that the two components originate from different environments around the emitting species, although both of them originate from the gas phase inside bubbles. The generation mechanisms of the two components are discussed.     

Experimental investigation on the effects of the standoff distance and the initial radius on the dynamics of a single bubble near a rigid wall in an ultrasonic field

Bubble behaviors near a boundary in an ultrasonic field are the fundamental forms of acoustic cavitation and of substantial importance in various applications, such as industry cleaning, chemical engineering and food processing. The effects of two important factors that strongly affect the dynamics of a single acoustic cavitation bubble, namely, the initial bubble radius and the standoff distance, were investigated in this work. The temporal evolution of the bubble was recorded using high speed microphotography. Meanwhile, the time of bubble collapse and the characteristics of the liquid jets were analyzed. The results demonstrate that the intensity of the acoustic cavitation, which is characterized by the time of bubble collapse and the liquid jet speed, reaches the optimum level under suitable values of the initial bubble radius and the normalized standoff distance. As the initial bubble radius and the normalized standoff distance increase or decrease from the optimal values, the time of the bubble collapse increases, and the first liquid jet’s speed decreases substantially, whereas the speeds of the second and third liquid jets exhibit no substantial changes. These results on bubble dynamics in an ultrasonic field are important for identifying or correcting the mechanisms of acoustic cavitation and for facilitating its optimization and application.     

Effects of extracellular matrix rigidity on sonoporation facilitated by targeted microbubbles: Bubble attachment,bubble dynamics,and cell membrane permeabilization

In this study, we investigated the effects of extracellular matrix rigidity, an important physical property of microenvironments regulating cell morphology and functions, on sonoporation facilitated by targeted microbubbles, highlighting the role of microbubbles. We conducted mechanistic studies at the cellular level on physiologically relevant soft and rigid substrates. By developing a unique imaging strategy, we first resolved details of the 3D attachment configurations between targeted microbubbles and cell membrane. High-speed video microscopy then unveiled bubble dynamics driven by a single ultrasound pulse. Finally, we evaluated the cell membrane permeabilization using a small molecule model drug. Our results demonstrate that: (1) stronger targeted microbubble attachment was formed for cells cultured on the rigid substrate, while six different attachment configurations were revealed in total; (2) more violent bubble oscillation was observed for cells cultured on the rigid substrate, while one third of bubbles attached to cells on the soft substrate exhibited deformation shortly after ultrasound was turned off; (3) higher acoustic pressure was needed to permeabilize the cell membrane for cells on the soft substrate, while under the same ultrasound condition, acoustically-activated microbubbles generated larger pores as compared to cells cultured on the soft substrate. The current findings provide new insights to understand the underlying mechanisms of sonoporation in a physiologically relevant context and may be useful for the clinical translation of sonoporation.     

Effects of radiator shapes on the bubble diving and dispersion of ultrasonic argon process

In this work, three ultrasonic radiators in different shapes have been designed in order to investigate the effects of radiator shapes on the argon bubble dispersion and diving as well as the degassing efficiency on magnesium melt. The radiator shape has a strong influence on the bubble diving and dispersion by ultrasound. A massive argon bubble slowly flows out from the radiator with the hemispherical cap, due to the covering hemispherical cap. Using a concave radiator can intensively crush the argon bubbles and drive them much deep into the water/melt, depending on the competition between the argon flow and opposite joint shear force from the concave surface. The evolution of wall bubbles involves the ultrasonic cavities carrying dissolved gas, migrating to the vessel wall, and escaping from the liquid. Hydrogen removal can be efficiently achieved using a concave radiator. The hydrogen content can be reduced from 22.3 μg/g down to 8.7 μg/g. Mechanical properties are significantly promoted, due to the structure refinement and efficient hydrogen removal.     

Nonlinear dynamics and acoustic emissions of interacting cavitation bubbles in viscoelastic tissues

The cavitation-mediated bioeffects are primarily associated with the dynamic behaviors of bubbles in viscoelastic tissues, which involves complex interactions of cavitation bubbles with surrounding bubbles and tissues. The radial and translational motions, as well as the resultant acoustic emissions of two interacting cavitation bubbles in viscoelastic tissues were numerically investigated. Due to the bubble–bubble interactions, a remarkable suppression effect on the small bubble, whereas a slight enhancement effect on the large one were observed within the acoustic exposure parameters and the initial radii of the bubbles examined in this paper. Moreover, as the initial distance between bubbles increases, the strong suppression effect is reduced gradually and it could effectively enhance the nonlinear dynamics of bubbles, exactly as the bifurcation diagrams exhibit a similar mode of successive period doubling to chaos. Correspondingly, the resultant acoustic emissions present a progressive evolution of harmonics, subharmonics, ultraharmonics and broadband components in the frequency spectra. In addition, with the elasticity and/or viscosity of the surrounding medium increasing, both the nonlinear dynamics and translational motions of bubbles were reduced prominently. This study provides a comprehensive insight into the nonlinear behaviors and acoustic emissions of two interacting cavitation bubbles in viscoelastic media, it may contribute to optimizing and monitoring the cavitation-mediated biomedical applications.     

Effects of concentrated NaCl and KCl solutions on the behaviour of aqueous peptide bond environment: single-particle dynamics and H-bond structural relaxation

The effects of salt concentrations on the structure, dynamics and hydrogen bond structural relaxation properties of ～1.10 M aqueous N-methylacetamide (NMA) solution at 308 K are studied by classical molecular dynamics simulations. We have considered the concentration range of salts solution from 0.222 to 3.756 M to investigate the behaviour of aqueous environment of peptide bonds in the presence of concentrated NaCl and KCl solution. It is found that the addition of salt solution facilitates the structural breaking of aqueous NMA hydrogen bonds, as a result the number of hydrogen bonds per NMA molecule and their stability decreases. The water and NMA molecule shows slower translational and rotational dynamics with increasing salt concentrations due to additional ion atmospheric friction. Our result shows that the cation–O_NMA radial distribution function decreases whereas the Cl^?─H_NMA radial distribution function increases with ion concentration. On the other hand, the cation–O_water and Cl^?─H_water radial distribution function shows very negligible change with respect to ion concentration. We have also calculated NMA–water and water–water hydrogen bond structural relaxation times. It is observed that the hydrogen bond structural relaxation of O_NMA─H_water is comparatively slower than the H_NMA─O_water hydrogen bond, which can be attributed to higher number and greater stability of the former hydrogen bond than the latter. The change of the dynamical quantities observed here is more prominent in addition of NaCl rather than the KCl solution.     

Molecular dynamics simulations of carbon dioxide hydrate growth in electrolyte solutions of NaCl and MgCl2

Molecular dynamics simulations are performed to study the growth of carbon dioxide (CO₂) hydrate in electrolyte solutions of NaCl and MgCl₂. The kinetic behaviour of the hydrate growth is examined in terms of cage content, density profile, and mobility of ions and water molecules, and how these properties are influenced by added NaCl and MgCl₂. Our simulation results show that both NaCl and MgCl₂ inhibit the CO₂ hydrate growth. With a same mole concentration or ion density, MgCl₂ exhibits stronger inhibition on the growth of CO₂ hydrate than NaCl does. The growth rate of the CO₂ hydrate in NaCl and MgCl₂ solutions decreases slightly with increasing pressure. During the simulations, the Na⁺, Mg²⁺, and Cl^? ions are mostly excluded by the growing interface front. We find that these ions decrease the mobility of their surrounding water molecules, and thus reduce the opportunity for these water molecules to form cage-like clusters toward hydrate formation. We also note that during the growth processes, several 5¹²6³ cages appear at the hydrate/solution interface, although they are finally transformed to tetrakaidecahedral (5¹²6²) cages. Structural defects consisting of one water molecule trapped in a cage with its hydrogen atoms being attracted by two Cl^? ions have also been observed.     

Electron absorption spectra of univalent copper-, silver-, and gold-thiourea complexes in aqueous solutions

Using data on the stability of complex forms, electron absorption spectra of copper (I)-, silver (I)-, and gold (I)—thiourea complexes in an aqueous solution M_itu_j (Ag: i=1, 2, j=1–3; Cu: j=1, 2; Au: j=2) are calculated from the spectra of solutions of a known analytical composition. Parameters of particular bands of the absorption spectra of these complexes are given. It is found that the integral intensity of the spectra of the solutions is proportional to the concentration of thiourea in the solution with high accuracy. The same is also valid for the spectra in solutions that contain mercury (II) and thiourea. The total intensity of longwave bands in the spectra of the complexes is proportional to the number of ligands in a molecule of the complex. Institute of Ionorganic Chemistry, Siberian Branch of the Russian Academy of Sciences, 3, Lavrent’ev Ave., 630090, Novosibirsk-90, Russia, Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 64, No. 4, pp. 458–462, July–August, 1997.     

The structure,dynamics and solvation mechanisms of ions in water from long time molecular dynamics simulations: a case study of CaCl2 (aq) aqueous solutions

Systematic long time (5–20 ns) molecular dynamics (MD) simulations have been carried out to study the structural and dynamical properties of CaCl₂ aqueous solutions over a wide range of concentrations (≤9.26 m) in this study. Our simulations reveal totally different structural characteristics of those yielded from short time (≤1 ns) MD simulations [A.A. Chialvo and J.M. Simonson, J. Chem. Phys. 119, 8052 (2003); T. Megyes, I. Bako, S. Balint, T. Grosz, and T. Radnai, J. Mol. Liq. 129, 63 (2006)]. An apparent discontinuity was found at 4–5 m of CaCl₂ in various properties including ion–water coordination number and self-diffusion coefficient of ions, which were first noticed by Phutela and Pitzer in their thermodynamic modelling [R.C. Phutela and K.S. Pitzer, J. Sol. Chem. 12, 201 (1983)]. In this study, residence time was first taken into consideration in the study of Ca²⁺–Cl^? ion pairing, and it was found that contact ion pair and solvent-sharing ion pair start to form at the CaCl₂(aq) concentrations of about 4.5 and 4 m, respectively, which may be responsible for the apparent discontinuity. In addition, the residence time of water molecules around Ca²⁺ or Cl^? showed that the hydration structures of Ca²⁺ and Cl^? are flexible with short residence time (<1 ns). It needs to be pointed out that it takes much longer simulation time for the CaCl₂–H₂O system to reach equilibrium than what was assumed in previous studies.     

Effects of polyethylenimine on morphology and property of ZnO films grown in aqueous solutions

Morphologies and properties of well-aligned ZnO films were controlled using zinc nitrate-hexamethylenetetramine aqueous solutions with the addition of polyethylenimine as a surfactant. Porous and dense ZnO films were fabricated with and without polyethylenimine, respectively. The addition of polyethylenimine proceeded to form porous ZnO whiskers film by preferential adsorption to nonpolar crystal faces and modifications of the surface free energy and growth rate. Dense ZnO film showed high transmittance of 80%, and low intensity of fluorescence and photo-induced current. Porous ZnO whiskers film showed low transmittance of 70%, while high intensity of fluorescence and high photo-induced current were detected because the porous ZnO nanowhisker film possessed a large interior surface area which can capture large amounts of DNA molecules labeled with dye molecules on the surface of ZnO crystals. High performance dye-sensitized sensors can be produced using ZnO whisker films prepared from an aqueous solution.     

Molecular dynamics study on water self-diffusion in aqueous mixtures of methanol,ethylene glycol and glycerol: investigations from the point of view of hydrogen bonding

Molecular dynamics simulations have been performed to investigate the aqueous binary mixtures of alcohols, including methanol, ethylene glycol (EG) and glycerol of molalities ranging from 1 to 5 m at the temperatures of 273, 288 and 298 K, respectively. The primary purpose of this paper is to investigate the mechanism of water self-diffusion in water-alcohol mixtures from the point of view of hydrogen bonding. The effects of temperature and concentration on water self-diffusion coefficient are evaluated quantitatively in this work. Temperature and concentration to some extent affect the hydrogen bonding statistics and dynamics of the binary mixtures. It is shown that the self-diffusion coefficient of water molecules decreases as the concentration increases or the temperature decreases. Moreover, calculations of mean square displacements of water molecules initially with different number n of H-bonds indicate that the water self-diffusion coefficient decreases as n increases. We also studied the aggregation of alcohol molecules by the hydrophobic alkyl groups. The largest cluster size of the alkyl groups clearly increases as the concentration increases, implying the emergence of a closely connected network of water and alcohols. The clusters of water and alcohol that interacted could block the movement of water molecules in binary mixtures. These findings provide insight into the mechanisms of water self-diffusion in aqueous binary mixtures of methanol, EG and glycerol.     

Analysis of the impact of laser line width over RIN, power penalty and bit rate including higher-order dispersion in WDM systems

This paper investigated the effect of laser line width over relative intensity noise (RIN), power penalty and bit rate at optical distances in the range of 100-10,000 km both analytically and graphically. It is also proposed and analyzed that by reducing the laser line width to the range of KHz, we can minimize the impact of RIN and power penalty under the individual and combined impact of higher-order dispersion parameters.     

Sonocrystallisation of ZIF-8 in water with high excess of ligand: Effects of frequency,power and sonication time

A systematic study on the sonocrystallisation of ZIF-8 (zeolitic imidazolate framework-8) in a water-based system was investigated under different mixing speeds, ultrasound frequencies, calorimetric powers and sonication time. Regardless of the synthesis technique, pure crystals of ZIF-8 with high BET (Brunauer, Emmett and Teller) specific surface area (SSA) can be obtained in water after only 5 s. Furthermore, 5 s sonication produced even smaller crystals (~0.08 µm). The type of technique applied for producing the ZIF-8 crystals did not have any significant impact on crystallinity, purity and yield. Crystal morphology and size were affected by the use of ultrasound and mixing, obtaining nanoparticles with a more spherical shape than in silent condition (no ultrasound and mixing). However, no specific trends were observed with varying frequency, calorimetric power and mixing speed. Ultrasound and mixing may have an effect on the nucleation step, causing the fast production of nucleation centres. Furthermore, the BET SSA increased with increasing mixing speed. With ultrasound, the BET SSA is between the values obtained under silent condition and with mixing. A competition between micromixing and shockwaves has been proposed when sonication is used for ZIF-8 production. The former increases the BET SSA, while the latter could be responsible for porosity damage, causing a decrease of the surface area.