Laser ultrasonic imaging of subsurface defects with the linear sampling method.

Laser ultrasonics is a remote nondestructive evaluation technique suitable for real-time monitoring of fabrication processes in semiconductor metrology, advanced manufacturing, and other applications where non-contact, high fidelity measurements are required. Here we investigate laser ultrasonic data processing approaches to reconstruct images of subsurface side drilled holes in aluminum alloy specimens. We demonstrate through simulation that the model-based linear sampling method (LSM) can perform accurate shape reconstruction of single and multiple holes and produce images with well-defined boundaries. We experimentally confirm that LSM produces images that represent the internal geometric features of an object, some of which may be missed by conventional imaging.

Photoacoustic Vaporization of Endoskeletal Droplets Loaded with Zinc Naphthalocyanine.

Vaporizable endoskeletal droplets are solid hydrocarbons in liquid fluorocarbon droplets in which melting of the hydrocarbon phase leads to the vaporization of the fluorocarbon phase. In prior work, vaporization of the endoskeletal droplets was achieved thermally by heating the surrounding aqueous medium. In this work, we introduce a near-infrared (NIR) optically absorbing naphthalocyanine dye (zinc 2,11,20,29-tetra-tert-butyl-2,3-naphthalocynanine) into the solid hydrocarbon (eicosane, n-C20H42) core of liquid fluorocarbon (C5F12) drops suspended in an aqueous medium. Droplets with a uniform diameter of 11.7 ± 0.7 µm were formed using a flow-focusing microfluidic device. The solid hydrocarbon formed a crumpled spherical structure within the liquid fluorocarbon droplet. The photoactivation behavior of these dye-containing endoskeletal droplets was investigated using NIR laser irradiation. When exposed to a pulsed laser of 720 nm wavelength, the dye-containing droplets vaporized at an average laser fluence of 65 mJ/cm2, whereas blank droplets without the dye did not vaporize at any fluence up to 100 mJ/cm2. Furthermore, dye-loaded droplets with a smaller, polydisperse size distribution were prepared using a simple shaking method and studied in a flow phantom for their photoacoustic signal and ultrasound contrast imaging. These results demonstrate that dye-containing endoskeletal droplets can be made to vaporize by externally applied optical energy. Such droplets may be useful for a variety of photoacoustic applications for sensing, imaging, and therapy.

Contrast-Enhanced Sonography with Biomimetic Lung Surfactant Nanodrops.

Nanodrops comprising a perfluorocarbon liquid core can be acoustically vaporized into echogenic microbubbles for ultrasound imaging. Packaging the microbubble in its condensed liquid state provides some advantages, including in situ activation of the acoustic signal, longer circulation persistence, and the advent of expanded diagnostic and therapeutic applications in pathologies which exhibit compromised vasculature. One obstacle to clinical translation is the inability of the limited surfactant present on the nanodrop to encapsulate the greatly expanded microbubble interface, resulting in ephemeral microbubbles with limited utility. In this study, we examine a biomimetic approach to stabilize an expanding gas surface by employing the lung surfactant replacement, beractant. Lung surfactant contains a suite of lipids and proteins that provide efficient shuttling of material from bilayer folds to the monolayer surface. We hypothesized that beractant would improve stability of acoustically vaporized microbubbles. To test this hypothesis, we characterized beractant surface dilation mechanics and revealed a novel biophysical phenomenon of rapid interfacial melting, spreading, and resolidification. We then harnessed this unique functionality to increase the stability and echogenicity of microbubbles produced after acoustic droplet vaporization for in vivo ultrasound imaging. Such biomimetic lung surfactant-stabilized nanodrops may be useful for applications in ultrasound imaging and therapy.

Sub-acoustic resolution optical focusing through scattering using photoacoustic fluctuation guided wavefront shaping.

Focusing light through turbid media using wavefront shaping generally requires a noninvasive guide star to provide feedback on the focusing process. Here we report a photoacoustic guide star mechanism suitable for wavefront shaping through a scattering wall that is based on the fluctuations in the photoacoustic signals generated in a micro-vessel filled with flowing absorbers. The standard deviation of photoacoustic signals generated from random distributions of particles is dependent on the illumination volume and increases nonlinearly as the illumination volume is decreased. We harness this effect to guide wavefront shaping using the standard deviation of the photoacoustic response as the feedback signal. We further demonstrate sub-acoustic resolution optical focusing through a diffuser with a genetic algorithm optimization routine.

The effect of size range on ultrasound-induced translations in microbubble populations.

Microbubble translations driven by ultrasound-induced radiation forces can be beneficial for applications in ultrasound molecular imaging and drug delivery. Here, the effect of size range in microbubble populations on their translations is investigated experimentally and theoretically. The displacements within five distinct size-isolated microbubble populations are driven by a standard ultrasound-imaging probe at frequencies ranging from 3 to 7 MHz, and measured using the multi-gate spectral Doppler approach. Peak microbubble displacements, reaching up to 10 µm per pulse, are found to describe transient phenomena from the resonant proportion of each bubble population. The overall trend of the statistical behavior of the bubble displacements, quantified by the total number of identified displacements, reveals significant differences between the bubble populations as a function of the transmission frequency. A good agreement is found between the experiments and theory that includes a model parameter fit, which is further supported by separate measurements of individual microbubbles to characterize the viscoelasticity of their stabilizing lipid shell. These findings may help to tune the microbubble size distribution and ultrasound transmission parameters to optimize the radiation-force translations. They also demonstrate a simple technique to characterize the microbubble shell viscosity, the fitted model parameter, from freely floating microbubble populations using a standard ultrasound-imaging probe.

Single Microbubble Measurements of Lipid Monolayer Viscoelastic Properties for Small-Amplitude Oscillations.

Lipid monolayer rheology plays an important role in a variety of interfacial phenomena, the physics of biological membranes, and the dynamic response of acoustic bubbles and drops. We show here measurements of lipid monolayer elasticity and viscosity for very small strains at megahertz frequency. Individual plasmonic microbubbles of 2-6 µm radius were photothermally activated with a short laser pulse, and the subsequent nanometer-scale radial oscillations during ring-down were monitored by optical scatter. This method provided average dynamic response measurements of single microbubbles. Each microbubble was modeled as an underdamped linear oscillator to determine the damping ratio and eigenfrequency, and thus the lipid monolayer viscosity and elasticity. Our nonisothermal measurement technique revealed viscoelastic trends for different lipid shell compositions. We observed a significant increase in surface elasticity with the lipid acyl chain length for 16 to 20 carbons, and this effect was explained by an intermolecular forces model that accounts for the lipid composition, packing, and hydration. The surface viscosity was found to be equivalent for these lipid shells. We also observed an anomalous decrease in elasticity and an increase in viscosity when increasing the acyl chain length from 20 to 22 carbons. These results illustrate the use of a novel nondestructive optical technique to investigate lipid monolayer rheology in new regimes of frequency and strain, possibly elucidating the phase behavior, as well as how the dynamic response of a microbubble can be tuned by the lipid intermolecular forces.

Experimental and numerical study of the excitability of zero group velocity Lamb waves by laser-ultrasound.

The excitability of zero group velocity (ZGV) Lamb waves using a pulsed laser source is investigated experimentally and through numerical simulation. Experimentally, a laser based ultrasonic technique is used to find the optical spot size on the sample surface that allows an optimal coupling of the optical energy into the ZGV mode. Numerical simulations, using the time domain finite differences technique, are carried out to model the thermoelastic generation process by laser irradiation and the propagation of the generated acoustic waves. The experimental results are in good agreement with the numerical predictions. The experimentally and numerically obtained responses of the plate are investigated by a short-time Fourier transform. The responses show that the source diameter does not affect the fundamental behavior of the temporal decay of the ZGV mode.

Optically induced resonance of nanoparticle-loaded microbubbles.

We report on the optical excitation and detection of resonant microbubble oscillations. Optically absorbing nanoparticles were attached to the shell of a lipid-encapsulated microbubble, allowing for optical pulsing to photothermally drive the microbubble into resonance. A modified optical microscope was used to track the bubble wall radius as a function of time using light scattering. The microbubble response from a nanosecond laser pulse was measured, and the eigenfrequency and vibrational amplitude were determined and compared to theory. The ability to optically drive microbubble oscillations may have applications in basic studies of bubble dynamics and biomedical imaging and therapy.

High contrast three-dimensional photoacoustic imaging through scattering media by localized optical fluence enhancement.

We demonstrate enhanced three-dimensional photoacoustic imaging behind a scattering material by increasing the fluence in the ultrasound transducer focus. We enhance the optical intensity using wavefront shaping before the scatterer. The photoacoustic signal induced by an object placed behind the scattering medium serves as feedback to optimize the wavefront, enabling one order of magnitude enhancement of the photoacoustic amplitude. Using the enhanced optical intensity, we scan the object in two-dimensions before post-processing of the data to reconstruct the image. The temporal profile of the photoacoustic signal provides the information used to reconstruct the third dimension.

Real-time laser ultrasonic monitoring of laser-induced thermal processes.

Intra- and inter-layer integrity of components fabricated with advanced manufacturing techniques, such as laser powder bed fusion, is dependent upon rapid heating, melting, and solidification processes. There is a need for new techniques to provide in situ feedback of these processes. Here a laser-based ultrasonic technique to probe thermal effects induced by a high-power continuous wave laser in titanium samples is described. Numerical simulations were performed to show that, for a spatially uniform heating beam, laser-induced surface acoustic waves are strongly influenced by surface heating conditions, are dispersive in the case of rapid heating, and that an abrupt velocity reduction happens upon the onset of surface melting. Furthermore, laser-based ultrasound experimental results which monitor the transient change of surface wave travel time associated with high power laser surface heating are provided. A pulsed laser is used to generate high frequency surface acoustic waves that propagate through the laser-heated region and are detected using a photorefractive crystal-based interferometer. Qualitative agreement is observed between theory and experiment with both showing a rapid reduction in the surface wave velocity at the onset of illumination and further decrease in surface wave velocity associated with melting. It is demonstrated that changes in the surface wave velocity can be used to track local heating and detect the onset of surface melting in real time.

Enhanced visibility through microbubble-induced photoacoustic fluctuation imaging.

A photoacoustic contrast mechanism is presented based on the photoacoustic fluctuations induced by microbubbles flowing inside a micro-vessel filled with a continuous absorber. It is demonstrated that the standard deviation of a homogeneous absorber mixed with microbubbles increases non-linearly as the microbubble concentration and microbubble size is increased. This effect is then utilized to perform photoacoustic fluctuation imaging with increased visibility and contrast of a blood flow phantom.

Optical nucleation of bubble clouds in a high pressure spherical resonator.

An experimental setup for nucleating clouds of bubbles in a high-pressure spherical resonator is described. Using nanosecond laser pulses and multiple phase gratings, bubble clouds are optically nucleated in an acoustic field. Dynamics of the clouds are captured using a high-speed CCD camera. The images reveal cloud nucleation, growth, and collapse and the resulting emission of radially expanding shockwaves. These shockwaves are reflected at the interior surface of the resonator and then reconverge to the center of the resonator. As the shocks reconverge upon the center of the resonator, they renucleate and grow the bubble cloud. This process is repeated over many acoustic cycles and with each successive shock reconvergence, the bubble cloud becomes more organized and centralized so that subsequent collapses give rise to stronger, better defined shockwaves. After many acoustic cycles individual bubbles cannot be distinguished and the cloud is then referred to as a cluster. Sustainability of the process is ultimately limited by the detuning of the acoustic field inside the resonator. The nucleation parameter space is studied in terms of laser firing phase, laser energy, and acoustic power used.

Photoacoustic Impulse Response of Lipid-Coated Ultrasound Contrast Agents.

The utility of ultrasound imaging and therapy with microbubbles may be greatly enhanced by determining their impulse-response dynamics as a function of size and composition. Prior methods for microbubble characterization utilizing high-speed cameras, acoustic transducers and laser-based techniques typically scan a limited frequency range. Here, we report on the use of a novel photoacoustic technique to measure the impulse response of single microbubbles. Individual microbubbles are driven with a broadband photoacoustic wave generated by a nanosecond-pulse laser illuminating an optical absorber. The resulting microbubble oscillations were detected by following transmission of a second laser as it passes twice through the microbubble. The system could even resolve oscillations resulting from a single-shot. As a proof-of-concept study, the size-dependent, linear impulse response of lipid-coated microbubbles was characterized using this technique. This unique method of microbubble characterization with exceptional spatiotemporal resolution opens new avenues for capturing and analyzing microbubble system dynamics.

Hydrophobically Modified Silica-Coated Gold Nanorods for Generating Nonlinear Photoacoustic Signals.

In this work, we report that gold nanorods coated with hydrophobically-modified mesoporous silica shells not only enhance photoacoustic (PA) signal over unmodified mesoporous silica coated gold nanorods, but that the relationship between PA amplitude and input laser fluence is strongly nonlinear. Mesoporous silica shells of ~14 nm thickness and with ~3 nm pores were grown on gold nanorods showing near infrared absorption. The silica was rendered hydrophobic with addition of dodecyltrichlorosilane, then re-suspended in aqueous media with a lipid monolayer. Analysis of the PA signal revealed not only an enhancement of PA signal compared to mesoporous silica coated gold nanorods at lower laser fluences, but also a nonlinear relationship between PA signal and laser fluence. We attribute each effect to the entrapment of solvent vapor in the mesopores: the vapor has both a larger expansion coefficient and thermal resistance than silica that enhances conversion to acoustic energy, and the hydrophobic porous surface is able to promote phase transition at the surface, leading to a nonlinear PA response even at fluences as low as 5 mJ cm-2. At 21 mJ cm-2, the highest laser fluence tested, the PA enhancement was >12-fold over mesoporous silica coated gold nanorods.

Ultrasonic enhancement of photoacoustic emissions by nanoparticle-targeted cavitation.

A technique to enhance the photoacoustic emissions from laser-heated nanoparticles is presented. Gold nanoparticle-doped phantoms are subjected to pulsed optical and ultrasound fields, resulting in bubble formation and collapse and producing strong acoustic emissions. The applied ultrasound field allows for cavitation at lower laser fluences than using light alone. The acoustic emission associated with bubble collapse well exceeds the direct photoacoustic response and is used to image a nanoparticle-doped region in a tissue phantom. The strong acoustic emission and low-threshold fluence associated with ultrasound-assisted cavitation make the technique well suited for nanoparticle-targeted biological imaging and tissue therapy.

Changes in microbubble dynamics upon adhesion to a solid surface.

The interaction between an acoustically driven microbubble and a surface is of interest for a variety of applications, such as ultrasound imaging and therapy. Prior investigations have mainly focused on acoustic effects of a rigid boundary, where it was generally observed that the wall increases inertia and reduces the microbubble resonance frequency. Here we investigate the response of a lipid-coated microbubble adherent to a rigid wall. Firm adhesion between the microbubble and a glass surface was achieved through either specific (biotin/avidin) or nonspecific (lipid/glass) interactions. Total internal reflection fluorescence microscopy was used to verify conditions leading to either adhesion or non-adhesion of the bubble to a glass or rigid polymer surface. Individual microbubbles were driven acoustically to sub-nanometer-scale radial oscillations using a photoacoustic technique. Remarkably, adherent microbubbles were shown to have a higher resonance frequency than non-adherent microbubbles resting against the wall. Analysis of the resonance curves indicates that adhesion stiffens the bubble by an apparent increase in the shell elasticity term and decrease in the shell viscosity. Based on these results, we conclude that surface adhesion is dominant over acoustic effects for low-amplitude microbubble oscillations.

Quantitative characterization of turbid media using pressure contrast acousto-optic imaging.

An acousto-optic imaging technique suitable for the local and quantitative determination of subsurface optical properties in turbid media is presented. Acousto-optic signals elicited by ultrasound pulses at two different peak pressures in turbid media are detected by using photorefractive-crystal-based interferometry. The ratio of the measured signals, once calibrated for a particular set of pressure pulses, is found to give a direct measure of the reduced scattering coefficient of the interaction region between the light and sound. Measurements of the reduced scattering coefficient of inclusions buried in diffuse tissue phantoms are demonstrated.

Influence of the anisotropy on zero-group velocity Lamb modes.

Guided waves in a free isotropic plate (symmetric S(n) and antisymmetric A(n) Lamb modes) exhibit a resonant behavior at frequencies where their group velocity vanishes while their phase velocity remains finite. Previous studies of this phenomenon were limited to isotropic materials. In this paper, the optical generation and detection of these zero-group velocity (ZGV) Lamb modes in an anisotropic plate is investigated. With a circular laser source, multiple local resonances were observed on a silicon wafer. Experiments performed with a line source demonstrated that the frequency and the amplitude of these resonances depend on the line orientation. A comparison between experimental and theoretical dispersion curves for waves propagating along the [100] and [110] directions of the silicon crystal verified that these resonances occur at the minimum frequency of the S(1) and A(2) Lamb modes. Simulations indicated that it is possible to deduce the three elastic constants of the plate material with good accuracy from these measurements.

Propagation and Scattering of Lamb Waves at Conical Points in Plates.

Lamb waves exhibit conical dispersion at zero wave number when an accidental degeneracy occurs between thickness mode longitudinal and shear resonances of the same symmetry. Here we investigate the propagation of Lamb waves generated at the conical point frequency and the interaction of these waves with defects and interfaces. The group velocity and mode shapes of Lamb waves at the conical point are found, and it is shown that as the wavenumber gets close to zero, considerable group velocity is seen only for material properties supporting a degeneracy or near-degeneracy. The unusual wave propagation and mode conversion of Lamb waves generated at the conical point are elucidated through numerical simulations. Experimental measurements of near conical point Lamb wave interaction with holes in a plate demonstrate that these waves flow around defects while maintaining a constant phase of oscillation across that plate surface.

Photoacoustic technique to measure temperature effects on microbubble viscoelastic properties.

Phospholipid-coated microbubbles are being developed for several biomedical applications, but little is known about the effect of temperature on the viscoelastic properties of the shell. Here, we report on the use of a photoacoustic technique to study the shell properties of individual microbubbles as a function of temperature. The microbubbles were driven into small-amplitude oscillations by ultrasound waves generated from the absorption of an intensity-modulated infrared laser, and these oscillations were detected by forward-light scattering of a second blue laser. The drive laser modulation frequency was swept to determine the resonant response of 2-4 µm radius microbubbles. Lipid shell elasticity and viscosity were determined by modeling the microbubble response as a linear harmonic oscillator. The results from slow heating showed a linear decrease in elasticity and viscosity between 21 and 53 °C and a corresponding increase in the maximum oscillation amplitude. Rapid heating to 38 °C, on the other hand, showed a transient response in the viscoelastic properties, suggesting shell rupture and reformation during microbubble growth and subsequent dissolution. These effects are important for biomedical applications, which require warming of the microbubbles to body temperature.