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Tim Segers

Publications and source records attributed to Tim Segers.

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Role of surfactants on droplet formation in piezoacoustic inkjet printing across microsecond-to-second timescales

In piezo acoustic drop-on-demand inkjet printing a single droplet is produced for each piezo driving pulse. This droplet is typically multicomponent, including surfactants to control the spreading and drying of the droplet on the substrate. However, the role of these surfactants on the droplet formation process remains rather elusive. Surfactant concentration gradients may manifest across microsecond-to-second timescales, spanning both the rapid ejection of ink from the nozzle exit and the comparatively slower idling timescale governing the firing of successive droplets. In the present work, we study the influence of surfactants on droplet formation across 6 orders of magnitude in time. To this end, we visualize the microsecond droplet formation process using stroboscopic laser-induced fluorescence microscopy while we vary the nozzle idle time. Our results show that increasing the idle time up to O(1) s affects only the break-up dynamics of the inkjet but not its velocity. By contrast, for idle times $>$ O(1) s, both the break-up dynamics are altered and the velocity of the inkjet increases. We show that the increased velocity results from a decreased surface tension of the ejected droplet, which we extracted from the observed shape oscillations of the jetted droplets in flight. The measured decrease in surface tension is surprising as the $\mu$s timescale of droplet formation is much faster than the typical ms-to-s timescale of surfactant adsorption. By varying the bulk surfactant concentration, we show that the fast decrease in surface tension results from a local surfactant concentration increase to more than 200 times the CMC. Our results suggest that a local high concentration of surfactant allows for surfactant adsorption to the interface of an inkjet at the $\mu$s-to-ms timescale, which is much faster than the typical ms-to-s timescale of surfactant adsorption.

physics.flu-dyn

Resonance behavior of a compliant piezo-driven inkjet channel with an entrained microbubble

Microbubbles entrained in a piezo-driven drop-on-demand (DOD) printhead disturb the acoustics of the microfluidic ink channel and thereby the jetting behavior. Here, the resonance behavior of an ink channel as a function of the microbubble size and the number of bubbles is studied through theoretical modeling and experiments. The system is modeled as a set of two coupled harmonic oscillators: one corresponding to the compliant ink channel and one to the microbubble. The predicted and measured eigenfrequencies are in excellent agreement. It was found that the resonance frequency is independent of the bubble size as long as the compliance of the bubble dominates over that of the piezo actuator. An accurate description of the eigenfrequency of the coupled system requires the inclusion of the increased inertance of the entrained microbubble due to confinement. We show that the inertance of a confined bubble can be accurately obtained by using a simple potential flow approach. The model is further validated by the excellent agreement between the modeled and measured microbubble resonance curves. The present work therefore provides physical insight in the coupled dynamics of a compliant ink channel with an entrained microbubble.

physics.flu-dyn

Buckling of lipidic ultrasound contrast agents under quasi-static load

Collapse of lipidic ultrasound contrast agents under high-frequency compressive load has been historically interpreted by the vanishing of surface tension. By contrast, buckling of elastic shells is known to occur when costly compressible stress is released through bending. Through quasi-static compression experiments on lipidic shells, we analyze the buckling events in the framework of classical elastic buckling theory and deduce the mechanical characteristics of these shells. They are then compared to that obtained through acoustic characterization.

cond-mat.soft

Vorticity-induced flow-focusing leads to bubble entrainment in an inkjet printhead: synchrotron X-ray and volume-of-fluid visualizations

The oscillatory flows present in an inkjet printhead can lead to strong deformations of the air-liquid interface at the nozzle exit. Such deformations may lead to an inward directed air jet with bubble pinch-off and the subsequent entrainment of an air bubble, which is highly detrimental to the stability of inkjet printing. Understanding the mechanisms of bubble entrainment is therefore crucial in improving print stability. In the present work, we use ultrafast X-ray phase-contrast imaging and direct numerical simulations based on the Volume-of-Fluid method to study the mechanisms underlying the bubble entrainment in a piezo-acoustic printhead. We first demonstrate good agreement between experiments and numerics. We then show the different classes of bubble pinch-off obtained in experiments, and that those were also captured numerically. The numerical results are then used to show that the baroclinic torque, which is generated at the gas-liquid interface due to the misalignment of density and pressure gradients, results in a flow-focusing effect that drives the formation of the air jet from which a bubble can pinch-off.

physics.flu-dyn

Selective evaporation at the nozzle exit in piezoacoustic inkjet printing

In practical applications of inkjet printing the nozzles in a printhead have intermittent idle periods, during which ink can evaporate from the nozzle exit. Inks are usually multicomponent where each component has its own characteristic evaporation rate resulting in concentration gradients within the ink. These gradients may directly and indirectly (via Marangoni flows) alter the jetting process and thereby its reproducibility and the resulting print quality. In the present work, we study selective evaporation from an inkjet nozzle for water-glycerol mixtures. Through experiments, analytical modeling, and numerical simulations, we investigate changes in mixture composition with drying time. By monitoring the acoustics within the printhead, and subsequently modeling the system as a mass-spring-damper system, the composition of the mixture can be obtained as a function of drying time. The results from the analytical model are validated using numerical simulations of the full fluid mechanical equations governing the printhead flows and pressure fields. Furthermore, the numerical simulations reveal that the time independent concentration gradient we observe in the experiments is due to the steady state of water flux through the printhead. Finally, we measure the number of drop formation events required in this system before the mixture concentration within the nozzle attains the initial (pre-drying) value, and find a stronger than exponential trend in the number of drop formations required. These results shed light on the complex physiochemical hydrodynamics associated with the drying of ink at a printhead nozzle, and help in increasing the stability and reproducibility of inkjet printing.

physics.flu-dyn

The asymmetric coalescence of two droplets with different surface tensions is caused by capillary waves

When two droplets with different surface tensions collide, the shape evolution of the merging droplets is asymmetric. Using experimental and numerical techniques, we reveal that this asymmetry is caused by asymmetric capillary waves, which are the result of the different surface tensions of the droplets. We show that the asymmetry is enhanced by increasing the surface tension difference, and suppressed by increasing the inertia of the colliding droplets. Furthermore, we study capillary waves in the limit of no inertia. We reveal that the asymmetry is not directly caused by Marangoni forces. In fact, somehow counterintuitive, asymmetry is strongly reduced by the Marangoni effect. Rather, the different intrinsic capillary wave amplitudes and velocities associated with the different surface tensions of the droplets lie at the origin of the asymmetry during droplet coalescence.

physics.flu-dyn

Time-resolved velocity and pressure field quantification in a flow-focusing device for ultrafast microbubble production

Flow-focusing devices have gained great interest in the past decade, due to their capability to produce monodisperse microbubbles for diagnostic and therapeutic medical ultrasound applications. However, up-scaling production to industrial scale requires a paradigm shift from single chip operation to highly parallelized systems. Parallelization gives rise to fluidic interactions between nozzles that, in turn, may lead to a decreased monodispersity. Here, we study the velocity and pressure field fluctuations in a single flow-focusing nozzle during bubble production. We experimentally quantify the velocity field inside the nozzle at 100 ns time resolution, and a numerical model provides insight into both the oscillatory velocity and pressure fields. Our results demonstrate that, at the length scale of the flow focusing channel, the velocity oscillations propagate at fluid dynamical time scale (order of microseconds) whereas the dominant pressure oscillations are linked to the bubble pinch-off and propagate at a much faster time scale (order of nanoseconds).

physics.flu-dyn

Higher-order meniscus oscillations driven by flow-focusing leading to bubble pinch off and entrainment in a piezo acoustic inkjet nozzle

The stability of high-end piezo-acoustic drop-on-demand (DOD) inkjet printing is sometimes compromised by the entrainment of an air bubble inside the ink channel. Here, bubble pinch-off from an acoustically driven meniscus is studied in an optically transparent DOD printhead as a function of the driving waveform. We show that bubble pinch-off follows from low-amplitude higher-order meniscus oscillations on top of the global high-amplitude meniscus motion that drives droplet formation. In a certain window of control parameters, phase inversion between the low and high frequency components leads to the enclosure of an air cavity and bubble pinch-off. Although phenomenologically similar, bubble pinch-off is not a result of capillary wave interaction such as observed in drop impact on a liquid pool. Instead, we reveal geometrical flow focusing as the mechanism through which at first, an outward jet is formed on the retracted concave meniscus. When the subsequent high-frequency pressure wave hits the now toroidal-shaped meniscus, it accelerates the toroidal ring outward resulting in the formation of an air cavity that can pinch off. The critical control parameters for pinch off are the pulse timing and amplitude. To cure the bubble entrainment problem, the threshold for bubble pinch-off can be increased by suppressing the high frequency acoustic waves through appropriate waveform design. The present work therefore aids the improvement of the stability of inkjet printers through a physical understanding of meniscus instabilities.

physics.flu-dyn

Feedback-controlled microbubble generator producing one million monodisperse bubbles per second

Monodisperse lipid-coated microbubbles are a promising route to unlock the full potential of ultrasound contrast agents for medical diagnosis and therapy. Here, we present a stand-alone lab-on-a-chip instrument that allows microbubbles to be formed with high monodispersity at high production rates. Key to maintaining a long-term stable, controlled, and safe operation of the microfluidic device with full control over the output size distribution is an optical transmission based measurement technique that provides real-time information on production rate and bubble size. We feed the data into a feedback loop and demonstrate that this system can control the on-chip bubble radius (2.5 to 20 $\mu$m) and the production rate up to $10^6$ bubbles/s. The freshly formed phospholipid-coated bubbles stabilize after their formation to a size approximately two times smaller than their initial on-chip bubble size without loss of monodispersity. The feedback control technique allows for full control over the size distribution of the agent and can aid the development of microfluidic platforms operated by non-specialist end users.

cond-mat.soft

High-frequency acoustic droplet vaporization is initiated by resonance

Vaporization of low-boiling point droplets has numerous applications in combustion, process engineering and in recent years, in clinical medicine. However, the physical mechanisms governing the phase conversion are only partly explained. Here, we show that an acoustic resonance can arise from the large speed of sound mismatch between a perfluorocarbon microdroplet and its surroundings. The fundamental resonance mode obeys a unique relationship $kR$~$\sim$ 0.65 between droplet size and driving frequency that leads to a 3-fold pressure amplification inside the droplet. Classical nucleation theory shows that this pressure amplification increases the nucleation rate by several orders of magnitude. These findings are confirmed by high-speed imaging performed at a timescale of ten nanoseconds. The optical recordings demonstrate that droplets exposed to intense acoustic waves generated by inter-digital-transducers nucleate only if they match the theoretical resonance size.

physics.flu-dyn

The retraction of jetted slender viscoelastic liquid filaments

Long and slender liquid filaments are produced during inkjet printing, which can subsequently either retract to form a single droplet, or break up to form a primary droplet and one or more satellite droplets. These satellite droplets are undesirable since they degrade the quality and reproducibility of the print. Existing strategies for the suppression of satellite droplet formation include, among others, adding viscoelasticity to the ink. In the present work, we aim to improve the understanding of the role of viscoelasticity in suppressing satellite droplets in inkjet printing. We demonstrate that very dilute viscoelastic aqueous solutions (concentrations $\sim$ 0.003\% wt. polyethylene oxide (PEO), corresponding to nozzle Deborah number $De_{n}$ $\sim$ 3) can suppress satellite droplet formation. Furthermore, we show that, for a given driving condition, upper and lower bounds of polymer concentration exist, within which satellite droplets are suppressed. Satellite droplets are formed at concentrations below the lower bound, while jetting ceases for concentrations above the upper bound (for fixed driving conditions). Moreover, we observe that, with concentrations in between the two bounds, the filaments retract at velocities larger than the corresponding Taylor-Culick velocity for the Newtonian case. We show that this enhanced retraction velocity can be attributed to the elastic tension due to polymer stretching, which builds up during the initial jetting phase. These results shed some light on the complex interplay between inertia, capillarity, and viscoelasticity for retracting liquid filaments, which is important for the stability and quality of inkjet printing of polymer solutions.

physics.flu-dyn

Rayleigh-Taylor instability by segregation in an evaporating multi-component microdroplet

The evaporation of multi-component droplets is relevant to various applications but challenging to study due to the complex physicochemical dynamics. Recently, Li (2018) reported evaporation-triggered segregation in 1,2-hexanediol-water binary droplets. In this present work, we added 0.5 wt% silicone oil into the 1,2-hexanediol-water binary solution. This minute silicone oil concentration dramatically modifies the evaporation process as it triggers an early extraction of the 1,2-hexanediol from the mixture. Surprisingly, we observe that the segregation of 1,2-hexanediol forms plumes, rising up from the rim of the sessile droplet towards the apex during the droplet evaporation. By orientating the droplet upside down, i.e., by studying a pendant droplet, the absence of the plumes indicates that the flow structure is induced by buoyancy, which drives a Rayleigh-Taylor instability (i.e., driven by density differences & gravitational acceleration). From micro-PIV measurement, we further prove that the segregation of the non-volatile component (1,2-hexanediol) hinders the evaporation near the contact line, which leads to a suppression of the Marangoni flow in this region. Hence, on long time scales, gravitational effects play the dominant role in the flow structure, rather than Marangoni flows. We compare the measurement of the evaporation rate with the diffusion model of Popov (2005), coupled with Raoult's law and the activity coefficient. This comparison indeed confirms that the silicone-oil-triggered segregation of the non-volatile 1,2-hexanediol significantly delays the evaporation. With an extended diffusion model, in which the influence of the segregation has been implemented, the evaporation can be well described.

physics.flu-dyn

Wetting of two-component drops: Marangoni contraction versus autophobing

The wetting properties of multi-component liquids are crucial to numerous industrial applications. The mechanisms that determine the contact angles for such liquids remain poorly understood, with many intricacies arising due to complex physical phenomena, for example due to the presence of surfactants. Here, we consider two-component drops that consist of mixtures of vicinal alkane diols and water. These diols behave surfactant-like in water. However, the contact angles of such mixtures on solid substrates are surprisingly large. We experimentally reveal that the contact angle is determined by two separate mechanisms of completely different nature, namely Marangoni contraction (hydrodynamic) and autophobing (molecular). It turns out that the length of the alkyl tail of the alkane diol determines which mechanism is dominant, highlighting the intricate coupling between molecular physics and the macroscopic wetting of complex fluids.

physics.flu-dyn

Evaporation of dilute sodium dodecyl sulfate droplets on a hydrophobic substrate

Evaporation of surfactant laden sessile droplets is omnipresent in nature and industrial applications such as inkjet printing. Soluble surfactants start to form micelles in an aqueous solution for surfactant concentrations exceeding the critical micelle concentration (CMC). Here, the evaporation of aqueous sodium dodecyl sulfate (SDS) sessile droplets on hydrophobic surfaces were experimentally investigated for SDS concentrations ranging from 0.025 to 1 CMC. In contrast to the constant contact angle of an evaporating sessile water droplet, we observed that, at the same surface the contact angle of an SDS laden droplet with a concentration below 0.5 CMC first decreases, then increases, and finally decreases resulting in a local contact angle minimum. Surprisingly, the minimum contact angle was found to be substantially lower than the static receding contact angle and it decreased with decreasing initial SDS concentration. Furthermore, the bulk SDS concentration at the local contact angle minimum was found to decrease with a decrease in the initial SDS concentration. The location of the observed contact angle minimum relative to the normalized evaporation time and its minimum value proved to be independent of both the relative humidity and the droplet volume and thus, of the total evaporation time. We discuss the observed contact angle dynamics in terms of the formation of a disordered layer of SDS molecules on the substrate at concentrations below 0.5 CMC. The present work underlines the complexity of the evaporation of sessile liquid-surfactant droplets and the influence of surfactant-substrate interactions on the evaporation process.

cond-mat.soft

Optical verification and in-vitro characterization of two commercially available acoustic bubble counters for cardiopulmonary bypass systems

Gaseous microemboli (GME) introduced during cardiac surgery are considered as a potential source of morbidity, which has driven the development of the first bubble counters. Two new generation bubble counters claim correct sizing and counting of GME. This in-vitro study aims to validate the accuracy of two bubble counters using monodisperse bubbles in a highly controlled setting at low GME concentrations. Monodisperse GME with a radius of 43 {\mu}m were produced in a microfluidic chip. Directly after their formation, they were injected one-by-one into the BCC200 and the EDAC sensors. GME size and count were optically verified using high-speed imaging. During best-case scenarios or low GME concentrations of GME with a size of 43 {\mu}m in radius in an in-vitro setup, the BCC200 overestimates GME size by a factor of 2 to 3 while the EDAC underestimates the average GME size by at least a factor of two. The BCC200 overestimates the GME concentration by approximately 20% while the EDAC overestimates the concentration by nearly one order of magnitude. Nevertheless, the calculated total GME volume is only over-predicted by a factor 2 since the EDAC underestimates the actual GME size. For the BCC200, the total GME volume was over-predicted by 25 times due to the over-estimation of GME size. The measured errors in the absolute sizing/counting of GME do not imply that all results obtained using the bubble counters are insignificant or invalid. A relative change in bubble size or bubble concentration can accurately be measured. However, care must be taken in the interpretation of the results and their absolute values. Moreover, the devices cannot be used interchangeably when reporting GME activity. Nevertheless, both devices can be used to study the relative air removal characteristics of CPB components or for the quantitative monitoring of GME production during CPB interventions.

physics.med-ph

Monodisperse versus polydisperse ultrasound contrast agents: nonlinear response, sensitivity, and deep tissue imaging potential

Monodisperse microbubble ultrasound contrast agents have been proposed to further increase the signal-to-noise-ratio of contrast enhanced ultrasound imaging. Here, the sensitivity of a polydisperse preclinical agent was compared experimentally to that of its size- and acoustically-sorted derivatives by using narrowband pressure- and frequency-dependent scattering and attenuation measurements. The sorted monodisperse agents showed up to a two orders of magnitude increase in sensitivity, i.e. in the average scattering cross-section per bubble. Moreover, we demonstrate here, for the first time, that the highly nonlinear response of acoustically sorted microbubbles can be exploited to confine scattering and attenuation to the focal region of ultrasound fields used in clinical imaging. This property is a result of minimal prefocal scattering and attenuation and can be used to minimize shadowing effects in deep tissue imaging. Moreover, it potentially allows for more localized therapy using microbubbles through the spatial control of resonant microbubble oscillations.

physics.med-ph