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.     

Membrane cleaning with ultrasonically driven bubbles

A laboratory filtration plant for drinking water treatment is constructed to study the conditions for purely mechanical in situ cleaning of fouled polymeric membranes by the application of ultrasound. The filtration is done by suction of water with defined constant contamination through a membrane module, a stack of five pairs of flat-sheet ultrafiltration membranes. The short cleaning cycle to remove the cake layer from the membranes includes backwashing, the application of ultrasound and air flushing. A special geometry for sound irradiation of the membranes parallel to their surfaces is chosen. Two frequencies, 35 kHz and 130 kHz, and different driving powers are tested for their cleaning effectiveness. No cleaning is found for 35 kHz, whereas good cleaning results are obtained for 130 kHz, with an optimum cleaning effectiveness at moderate driving powers. Acoustic and optic measurements in space and time as well as analytical considerations and numerical calculations reveal the reasons and confirm the experimental results. The sound field is measured in high resolution and bubble structures are high-speed imaged on their nucleation sites as well as during their cleaning work at the membrane surface. The microscopic inspection of the membrane surface after cleaning shows distinct cleaning types in the cake layer that are related to specific bubble behaviour on the membrane. The membrane integrity and permeate quality are checked on-line by particle counting and turbidity measurement of the permeate. No signs of membrane damage or irreversible membrane degradation in permeability are detected and an excellent water permeate quality is retained.     

Physical and chemical effects of acoustic cavitation in selected ultrasonic cleaning applications

Acoustic cavitation in a liquid medium generates several physical and chemical effects. The oscillation and collapse of cavitation bubbles, driven at low ultrasonic frequencies (e.g., 20 kHz), can generate strong shear forces, microjets, microstreaming and shockwaves. Such strong physical forces have been used in cleaning and flux improvement of ultrafiltration processes. These physical effects have also been shown to deactivate pathogens. The efficiency of deactivation of pathogens is not only dependent on ultrasonic experimental parameters, but also on the properties of the pathogens themselves. Bacteria with thick shell wall are found to be resistant to ultrasonic deactivation process. Some evidence does suggest that the chemical effects (radicals) of acoustic cavitation are also effective in deactivating pathogens. Another aspect of cleaning, namely, purification of water contaminated with organic and inorganic pollutants, has also been discussed in detail. Strong oxidising agents produced within acoustic cavitation bubbles could be used to degrade organic pollutants and convert toxic inorganic pollutants to less harmful substances. The effect of ultrasonic frequency and surface activity of solutes on the sonochemical degradation efficiency has also been discussed in this overview.     

Study and optimization of the ultrasound-enhanced cleaning of an ultrafiltration ceramic membrane through a combined experimental–statistical approach

Membrane fouling is one of the main drawbacks of ultrafiltration technology during the treatment of dye-containing effluents. Therefore, the optimization of the membrane cleaning procedure is essential to improve the overall efficiency. In this work, a study of the factors affecting the ultrasound-assisted cleaning of an ultrafiltration ceramic membrane fouled by dye particles was carried out. The effect of transmembrane pressure (0.5, 1.5, 2.5 bar), cross-flow velocity (1, 2, 3 m s⁻¹), ultrasound power level (40%, 70%, 100%) and ultrasound frequency mode (37, 80 kHz and mixed wave) on the cleaning efficiency was evaluated. The lowest frequency showed better results, although the best cleaning performance was obtained using the mixed wave mode.A Box–Behnken Design was used to find the optimal conditions for the cleaning procedure through a response surface study. The optimal operating conditions leading to the maximum cleaning efficiency predicted (32.19%) were found to be 1.1 bar, 3 m s⁻¹ and 100% of power level.Finally, the optimized response was compared to the efficiency of a chemical cleaning with NaOH solution, with and without the use of ultrasound. By using NaOH, cleaning efficiency nearly triples, and it improves up to 25% by adding ultrasound.     

Fluorescent microscope system to monitor real-time interactions between focused ultrasound,echogenic drug delivery vehicles,and live cell membranes

Rapid development in the field of ultrasound triggered drug delivery has made it essential to study the real-time interaction between the membranes of live cells and the membranes of echogenic delivery vehicles under exposure to focused ultrasound. The objective of this work was to design an analysis system that combined fluorescent imagining, high speed videography, and definable pulse sequences of focused ultrasound to allow for real time observations of both cell and vehicle membranes. Documenting the behavior of the membranes themselves has not previously been possible due to limitations with existing optical systems used to understand the basic physics of microbubble/ultrasound interaction and the basic interaction between microbubbles and cells. The performance of this new system to monitor membrane behavior was demonstrated by documenting the modes of vehicle fragmentation at different ultrasound intensity levels. At 1.5 MPa the membranes were shown to completely fragment while at intensities below 1 MPa the membranes pop open and slowly unfold. The interaction between these vehicles and cell membranes was also documented by the removal of fluorescent particles from the surfaces of live cells out to 20 μm from the microbubble location. The fluid flow created by microstreaming around ensonated microbubbles was documented at video recording speeds from 60 to 18,000 frames per second. This information about membrane behavior allows the chemical and physical properties of the drug delivery vehicle to be designed along with the ultrasound pulse sequence to cause the most efficient drug delivery.     

Effect of non-ionic surfactants on transient cavitation in a megasonic field

High resolution chronoamperometry has been used to characterize the effect of two non-ionic surfactants, Triton® X-100 and NCW®-1002, on cavitation in aqueous solutions exposed to ～1 MHz sound field. Specifically, using ferricyanide as the electroactive species, temporal variation of current during its reduction on a 25 μm Pt microelectrode has been measured and is used to elucidate transient cavity behavior. The chronoamperograms for solutions exposed to megasonic field show current ‘peaks’ riding on the baseline current. These current ‘peaks’ have been attributed to the diffusion of ferricyanide species concentrated at the liquid–vapor interface of a transient cavity at the end of its collapse. In the presence of surfactants, the frequency of occurrence of current ‘peaks’ with magnitude ?0.3 μA is found to increase indicating a higher number of transient cavity collapses. A simple mathematical model based on diffusion developed previously by the authors has been used to extract the maximum cavity size and range of distances between the center of the collapsing cavity and the electrode surface in the surfactant solutions.     

Cavitation distribution within large phantom vessel and mechanical damage formed on surrounding vessel wall

Blood vessel is one of the most important targets encountered during focused ultrasound (FU) therapy. The lasting high temperature caused by continuous FU can result in structural modification of small vessel. For the vessel with a diameter larger than 2 mm, convective cooling can significantly weaken the thermal effect of FU. Meanwhile, the continued presence of ultrasound will cause repetitive cavitation and acoustic microstreaming, making comprehension of continuous wave induced cavitation effect in large vessels necessary. The Sonoluminescence (SL) method, mechanical damage observation and high-speed camera were used in this study to investigate the combination effect of ultrasound contrast agents (UCAs) and continuous FU in large phantom vessels with a diameter of 10 mm without consideration of thermal effect. When the focus was positioned at the proximal wall, cylindrical hole along the acoustic axis opposite the ultrasound wave propagation direction was observed at the input power equal to or greater than 50 W. When the focus was located at the distal wall, only small tunnels can be found. The place where the cylindrical hole formed was corresponding to where bubbles gathered and emitted brilliant light near the wall. Without UCAs neither such bright SL nor cylindrical hole can be found. However, the UCAs concentration had little influence on the SL distribution and the length of cylindrical hole. The SL intensity near the proximal vessel wall and the length of the cylindrical hole both increased with the input power. It is suggested that these findings need to be considered in the large vessel therapy and UCAs usage.     

Computational study of the adsorption of dimethyl methylphosphonate (DMMP) on the (0 1 0) surface of anatase TiO2 with and without faceting

The adsorption of dimethyl methylphosphonate (DMMP) on the (0 1 0) surface of anatase TiO₂, which is isostructural with the (1 0 0), has been studied using density functional theory and two-dimensionally-periodic slab models. The experimentally-observed faceting of this surface has, for the first time, been included in the modeling. The relaxations of bare surfaces both with and without faceting are similar, leading to an atomic-scale roughening due to inward (outward) displacement of fivefold-coordinated Ti_5c (sixfold-coordinated T_6c) atoms together with outward displacement of threefold-coordinated O_3c atoms. Molecular adsorption occurs by formation of a Ti_5c?OP dative bond with one or more CH?O_2c bonds between CH₃ groups and unsaturated, twofold-coordinated (O_2c) sites. The energies for molecular adsorption, obtained using the B3LYP functional, are virtually identical (about ?21.0 kcal/mol) for the two surfaces and are also close to those found elsewhere for the rutile (1 1 0) and anatase (1 0 1) surfaces. A possible first step in the dissociative adsorption of DMMP has also been modeled and is found to be thermodynamically favored over molecular adsorption to a degree which depends on faceting.     

Preparation of resveratrol-enriched grape juice from ultrasonication treated grape fruits

Grape (Vitis spp.) is a major source of resveratrol that can be eaten directly or after making jam, jelly, wine and juice. Resveratrol (3,5,4′-trihydroxystilbene) has a profound positive influence on human health, including anti-carcinogenic, anti-cancer, anti-inflammatory, and anti-ageing effects and the ability to lower blood sugar. During industrial production of grape juice, resveratrol is lost because of the use of clarifying agents and filtration; therefore, commercial grape juice contains very low amounts of resveratrol. In this study, we investigated the accumulation of resveratrol in grape juice prepared from three varieties of grape, viz. Campbell Early, Muscat Bailey A (MBA) and Kyoho, following post-harvest ultrasonication cleaning for 5 min and 6 h of incubation in the dark at 25 °C. This process resulted in the amounts of resveratrol increasing by 1.53, 1.15 and 1.24 times in juice prepared from Campbell Early, MBA and Kyoho, respectively, without changing the amounts of total soluble solids. Overall, our results indicate that ultrasonication treatment of post-harvested grape fruits can be an effective method for producing resveratrol-enriched grape juice as well as cleaning grapes thoroughly.     

Chemical etchant dependence of surface structure and morphology on GaN(0001) substrates

We studied the procedure of cleaning GaN(0001) substrate surfaces by wet etching and subsequent annealing in ultrahigh vacuum for two different types of freestanding GaN wafers: hydride vapor phase epitaxy (HVPE) crystal and Na flux liquid phase epitaxy (LPE) crystal wafers. A flat surface containing GaN(0001)2 × 2 reconstruction was successfully achieved on both HVPE and LPE surfaces by etching in HF and subsequent annealing at ～ 550 °C but was not achieved by etching in HCl, NaOH, and HNO₃.     

Production of particulates from transducer erosion: Implications on food safety

The formation of metallic particulates from erosion was investigated by running a series of transducers at various frequencies in water. Two low frequency transducer sonotrodes were run for 7.5 h at 18 kHz and 20 kHz. Three high frequency plates operating at megasonic frequencies of 0.4 MHz, 1 MHz, and 2 MHz were run over a 7 days period. Electrical conductivity and pH of the solution were measured before and after each run. A portion of the non-sonicated and treated water was partially evaporated to achieve an 80-fold concentration of particles and then sieved through nano-filters of 0.1 μm, 0.05 μm, and 0.01 μm. An aliquot of the evaporated liquid was also completely dried on strips of carbon tape to determine the presence of finer particles post sieving. An aliquot was analyzed for detection of 11 trace elements by Inductively Coupled Plasma Mass Spectroscopy (ICPMS). The filters and carbon tapes were analyzed by FE-SEM imaging to track the presence of metals by EDS (Energy Dispersive Spectroscopy) and measure the particle size and approximate composition of individual particles detected. Light microscopy visualization was used to calculate the area occupied by the particles present in each filter and high resolution photography was used for visualization of sonotrode surfaces. The roughness of all transducers before and after sonication was tested through profilometry. No evidence of formation of nano-particles was found at any tested frequency. High amounts of metallic micron-sized particles at 18 kHz and 20 kHz formed within a day, while after 7 day runs only a few metallic micro particles were detected above 0.4 MHz. Erosion was corroborated by an increase in roughness in the 20 kHz tip after ultrasound. The elemental analysis showed that metal leach occurred but values remained below accepted drinking water limits, even after excessively long exposure to ultrasound. With the proviso that the particles measured here were only characterized in two dimensions and could be nanoparticulate in terms of the third dimension, this research suggests that there are no serious health implications resulting from the formation of nanoparticles under the evaluation conditions. Therefore, high frequency transducer plates can be safely operated in direct contact with foods. However, due to significant production of metallic micro-particulates, redesign of lower frequency sonotrodes and reaction chambers is advised to enable operation in various food processing direct-contact applications.     

Automatic detection of impact damage in carbon fiber composites using active thermography

Accidental impacts can severely reduce the structural strength and stability of composite materials, which can lead to severe consequences due to the degradation of the mechanical properties of components designed to perform for decades. Because accidental impacts are difficult to avoid, robust and reliable inspection methods to detect impact damage are required. Many methods have been proposed recently. However, most of them require an experienced technician to analyze the data, which leads to a significant decrease in manufacturing productivity. This work proposes a method to automatically detect impact damage in carbon fiber composites using active thermography. The proposed system detects defects caused by impact damage in the infrared images without human intervention. Impact damage detection is performed using a robust method based on an active thermographic inspection. Thermographic data is preprocessed to improve signal-to-noise ratio and to remove non-uniform background caused by non-uniform heating. Then, peaks and edges are identified and clustered, and regions corresponding to impact damage are detected. The proposed procedure has been applied to three specimens that contain 6 and 12 plies, different types of cores, and damage caused by energies from 6 J to 50 J. All defects are detected correctly.     

Femtosecond laser ablation of cadmium tungstate for scintillator arrays

Ultrafast pulsed laser ablation has been investigated as a technique to machine CdWO₄ single crystal scintillator and segment it into small blocks with the aim of fabricating a 2D high energy X-ray imaging array. Cadmium tungstate (CdWO₄) is a brittle transparent scintillator used for the detection of high energy X-rays and γ-rays. A 6 W Yb:KGW Pharos-SP pulsed laser of wavelength 1028 nm was used with a tuneable pulse duration of 10 ps to 190 fs, repetition rate of up to 600 kHz and pulse energies of up to 1 mJ was employed. The effect of varying the pulse duration, pulse energy, pulse overlap and scan pattern on the laser induced damage to the crystals was investigated. A pulse duration of ≥500 fs was found to induce substantial cracking in the material. The laser induced damage was minimised using the following operating parameters: a pulse duration of 190 fs, fluence of 15.3 J cm⁻² and employing a serpentine scan pattern with a normalised pulse overlap of 0.8. The surface of the ablated surfaces was studied using scanning electron microscopy, energy dispersive X-ray spectroscopy, atomic force microscopy and X-ray photoelectron spectroscopy. Ablation products were found to contain cadmium tungstate together with different cadmium and tungsten oxides. These laser ablation products could be removed using an ammonium hydroxide treatment.     

Growth of 〈1 0 0〉 directed ADP crystal with slotted ampoule

Good quality ammonium dihydrogen phosphate single crystals have been grown by: (i) Sankaranarayanan–Ramasamy (SR) method and (ii) SR method with slotted ampoule. The grown crystals were subjected to UV–Vis spectroscopy, high-resolution X-ray diffractometer, dielectric, piezoelectric and laser damage threshold studies. Compared to the (1 0 0) plane of the conventional method grown ADP crystal and 〈1 0 0〉 directed SR method grown ADP crystal, the crystal grown by SR method with slotted ampoule has higher growth rate, higher optical transparency, high crystalline perfection, low dielectric loss, high piezoelectric charge coefficient and high laser damage threshold due to diffusion of segregated impurities away from the growing crystal in the slotted ampoule growth.     

Defects induced ferromagnetism in Mn doped ZnO

Single phase Mn doped (2 at%) ZnO samples have been synthesized by the solid-state reaction technique. Before the final sintering at 500 °C, the mixed powders have been milled for different milling periods (6, 24, 48 and 96 h). The grain sizes of the samples are very close to each other (～32±4 nm). However, the defective state of the samples is different from each other as manifested from the variation of magnetic properties and electrical resistivity with milling time. All the samples have been found to be ferromagnetic with clear hysteresis loops at room temperature. The maximum value for saturation magnetization (0.11 μ_B/Mn atom) was achieved for 96 h milled sample. Electrical resistivity has been found to increase with increase in milling time. The most resistive sample bears the largest saturation magnetization. Variation of average positron lifetime with milling time bears a close similarity with that of the saturation magnetization. This indicates the key role played by open volume vacancy defects, presumably zinc vacancies near grain surfaces, in inducing ferromagnetic order in Mn doped ZnO. To attain optimum defect configuration favorable for ferromagnetism in this kind of samples proper choice of milling period and annealing conditions is required.     

Road condition analysis using NIR illumination and compensating for surrounding light

An investigation of a NIR camera system for road surface classification has been conducted for several road conditions. The surfaces were illuminated with three wavelengths, 980 nm, 1310 nm and 1550 nm and a halogen lamp, to simulate a real environment application with surrounding light. A measuring scheme to deal with surrounding light has been implemented enabling road condition classification from NIR images in a real environment. The retrieved camera images have been analyzed and an RGB representation of the different surfaces has been created to classify the different road conditions. The investigation shows that it is possible to distinguish between dry, moist, wet, frosty, icy and snowy road surfaces using a NIR camera system in a disturbed environment.     

Patterns in Ge cluster growth on clean and oxidized Si(111)-(7 × 7) surfaces

Ge atoms have been deposited on domain-patterned clean Si(111)-(7 × 7) and oxidized Si(111)-(7 × 7) surfaces. Clustering of Ge from the deposited Ge adatoms on these two kinds of surfaces shows contrasting patterns. On the clean Si surface, clustering predominantly occurs on domain boundaries, which include step edges on two sides. This leaves small domains denuded. Ge diffusion length has been estimated from the size of these denuded domains. For large domains, additional clustering is observed within the domains. For the oxidized Si surface, the pattern formation is in sharp contrast with that for the clean Si surface. In this case the domain boundaries remain relatively empty and there is strong clustering within the domains leading to the formation of dense Ge nanoislands within the domains. This contrasting pattern formation has been explained via a reaction diffusion model.     

Cu dimer diffusion on strained Cu(0 0 1)

Cu dimer diffusion energy barrier on strained Cu(0 0 1) surfaces has been studied with nudged elastic band method (NEB) and embedded atom method (EAM). Dimer exchange and hopping mechanisms are chosen as the initial diffusion paths in the NEB method. It is shown here that the dimer exchange is dominant on tensile surfaces and the dimer hopping is dominant on compressive surfaces. For most strain conditions Cu dimer diffusion energy barrier is lower than Cu monomer diffusion barrier. The concerted movement of the remaining adatom toward the hopping adatom lowers the dimer hopping barrier. The adsorption induced relaxation makes the dimer exchange barriers lower than the monomer exchange barriers on tensile surfaces. Transition state theory is used to calculate the diffusion frequencies as a function of temperature. No surface crowdion is observed on the shear strained surfaces for the dimer diffusion.     

Application of a He3Ne infrared laser source for detection of geometrical dimensions of cracks and scratches on finished surfaces of metals

In this study, the authors addressed a new method of measurement for microscratches and cracks on finished metallic surfaces. The technology proposed here can be used in aviation, automobile, machine-tools, bearings, electrical and thermal devices (detection of electrical and thermal contact resistance), and many other industrial fields where finished surfaces have to be inspected for quality before use. The technology is based on the application of He3Ne laser optics. This measurement method allows for the inspection of geometrical parameters such as depth and width of scratches and cracks and consists of a low-energy He3Ne red laser beam (wavelength 633 nm) with a cross-section of 0.48 mm, beam expander with special designed slit, multi-axis stage with sample holder and CCD (charge-coupled device) visual detection system. Using experimental data, a mathematical algorithm was created in order to calculate the depths and widths of the scratches and cracks where the method of center of gravity (centroid) of the imaged area was used. The results showed a good correlation between the experimental and calculated values of the dimensions of the scratches. Future work will deal with the determination of the geometrical dimensions of microcracks.     

Comparison of quantum,semi-classical and classical methods in the calculation of nitrogen self-broadened linewidths

We perform dynamical calculations on two robust N₂–N₂ potential energy surfaces in order to intercompare pressure broadening coefficients derived from close coupling and coupled states quantum dynamical methods, the semi-classical model of Robert and Bonamy and a full classical method. The coupled states and full classical results compare well with the experimental results or with close coupling values when available. This study confirms that the classical method is a good alternative at room and high temperatures to quantum dynamical methods. The results obtained using the semi-classical method however deviate from the other sets of data at all temperatures considered here (77–2400 K).