Periodic Distributions and Ultrafast Dynamics of Hot Electrons in Plasmonic Resonators.

Understanding and managing hot electrons in metals are of fundamental and practical interest in plasmonic studies and applications. A major challenge for the development of hot electron devices requires the efficient and controllable generation of long-lived hot electrons so that they can be harnessed effectively before relaxation. Here, we report the ultrafast spatiotemporal evolution of hot electrons in plasmonic resonators. Using femtosecond-resolution interferometric imaging, we show the unique periodic distributions of hot electrons due to standing plasmonic waves. In particular, this distribution can be flexibly tuned by the size, shape, and dimension of the resonator. We also demonstrate that the hot electron lifetimes are substantially prolonged at hot spots. This appealing effect is interpreted as a result of the locally concentrated energy density at the antinodes in standing hot electron waves. These results could be useful to control the distributions and lifetimes of hot electrons in plasmonic devices for targeted optoelectronic applications.

Sounding a New Era in Biomechanics with Acoustic Force Spectroscopy.

The acoustic force spectroscopy (AFS) tool was recently introduced as a novel tool for probing mechanical properties of biomolecules, expanding the application of sound waves to high-throughput quantification of the mechanical properties of single cells. By using controlled acoustic forces in the piconewton to nanonewton range, tens to hundreds of cells functionalized by attached microspheres can simultaneously be stretched and tracked in real-time with sub millisecond time response. Since its first application, several studies have demonstrated the potential and versatility of the AFS for high-throughput measurements of force-induced molecular mechanisms, revealing insight into cellular biomechanics and mechanobiology at the molecular level. In this chapter, we describe the operation of the AFS starting with the underlying physical principles, followed by a run-down of experimental considerations, and finally leading to applications in molecular and cellular biology.

Simulations and Experimental Analysis of a High Viscosity Inkjet Printing Device Based on Fabry-Pérot Resonator.

The study investigates the effect of changing various input parameters on the pressure responses at acoustic cavities of a droplet-based acoustic printing device consisting of a Fabry-Pérot (FP) resonator and a standing wave-source chamber. The standing wave of the acoustic radiation pressure at the FP resonator is analyzed. The behavior of the standing wave and acoustic radiation force at the FP resonator is presented and compared with the measured results by varying the position of the standing wave-generating plate. The pressure changes inside the standing wave-source chamber are investigated and discussed to determine the reason for the sudden high-pressure drop at the FP resonator. Furthermore, the effects of inserting the nozzle and droplet inside the FP resonator on the standing wave and acoustic radiation force are analyzed. Experimental analysis is performed by collecting acoustic pressure data at the outlet of the FP resonator. The simulated and measured pressure drop behaviors are compared. The presented numerical approach can be used to set optimal design guidelines for obtaining a higher acoustic pressure inside the acoustic cavities of droplet-based acoustic jetting and other acoustofluidic devices.

Observations of Bell Inequality Violations with Causal Isolation between Source and Detectors.

We report the experimental observations of Bell inequality violations (BIV) in entangled photons causally separated by a rotating mirror. A Foucault mirror gating geometry is used to causally isolate the entangled photon source and detectors. We report an observed BIV of CHSH-S=2.30±0.07>2.00. This result rules out theories that explain correlations with traveling communication between source and detectors, including super-luminal and instantaneous communication.

N-Heterocyclic Carbenes: Molecular Porters of Surface Mounted Ru-Porphyrins.

Ru-porphyrins act as convenient pedestals for the assembly of N-heterocyclic carbenes (NHCs) on solid surfaces. Upon deposition of a simple NHC ligand on a close packed Ru-porphyrin monolayer, an extraordinary phenomenon can be observed: Ru-porphyrin molecules are transferred from the silver surface to the next molecular layer. We have investigated the structural features and dynamics of this portering process and analysed the associated binding strengths and work function changes. A rearrangement of the molecular layer is induced by the NHC uptake: the NHC selective binding to the Ru causes the ejection of whole porphyrin molecules from the molecular layer on silver to the layer on top. This reorganisation can be reversed by thermally induced desorption of the NHC ligand. We anticipate that the understanding of such mass transport processes will have crucial implications for the functionalisation of surfaces with carbenes.

Standing wave approach in the theory of X-ray magnetic reflectivity.

An extension of the exact X-ray resonant magnetic reflectivity theory has been developed, taking into account the small value of the magnetic terms in the X-ray susceptibility tensor. It is shown that squared standing waves (fourth power of the total electric field) determine the output of the magnetic addition to the total reflectivity from a magnetic multilayer. The obtained generalized kinematical approach essentially speeds up the calculation of the asymmetry ratio in the magnetic reflectivity. The developed approach easily explains the peculiarities of the angular dependence of the reflectivity with the rotated polarization (such as the peak at the critical angle of the total external reflection). The revealed dependence of the magnetic part of the total reflectivity on the squared standing waves means that the selection of the reflectivity with the rotated polarization ensures higher sensitivity to the depth profiles of magnetization than the secondary radiation at the specular reflection condition.

Controlling excitable wave behaviors through the tuning of three parameters.

Excitable systems are a class of dynamical systems that can generate self-sustaining waves of activity. These waves are known to manifest differently under diverse conditions, whereas some travel as planar or radial waves, and others evolve into rotating spirals. Excitable systems can also form stationary stable patterns through standing waves. Under certain conditions, these waves are also known to be reflected at no-flux boundaries. Here, we review the basic characteristics of these four entities: traveling, rotating, standing and reflected waves. By studying their mechanisms of formation, we show how through manipulation of three critical parameters: time-scale separation, space-scale separation and threshold, we can interchangeably control the formation of all the aforementioned wave types.

Characterization of Pd/Y multilayers with B4C barrier layers using GIXR and X-ray standing wave enhanced HAXPES.

Pd/Y multilayers are high-reflectance mirrors designed to work in the 7.5-11 nm wavelength range. Samples, prepared by magnetron sputtering, are deposited with or without B4C barrier layers located at the interfaces of the Pd and Y layers to reduce interdiffusion, which is expected from calculating the mixing enthalpy of Pd and Y. Grazing-incident X-ray reflectometry is used to characterize these multilayers. B4C barrier layers are found to be effective in reducing Pd-Y interdiffusion. Details of the composition of the multilayers are revealed by hard X-ray photoemission spectroscopy with X-ray standing wave effects. This consists of measuring the photoemission intensity from the samples by performing an angular scan in the region corresponding to the multilayer period and an incident photon energy according to Bragg's law. The experimental results indicate that Pd does not chemically react with B nor C at the Pd-B4C interface while Y does react at the Y-B4C interface. The formation of Y-B or Y-C chemical compounds could be the reason why the interfaces are stabilized. By comparing the experimentally obtained angular variation of the characteristic photoemission with theoretical calculations, the depth distribution of each component element can be interpreted.

Atomic-Scale Interface for Pt Nanoparticles on SrTiO3 (001).

The interfacial structure formed by Pt nanoparticles grown epitaxially on a SrTiO3 (001) surface by pulsed laser deposition was studied by X-ray standing-wave (XSW) excited core-level photoelectron emission. The XSW-generated 3D atomic map of the Pt and interfacial oxygens for the oxidized Pt/SrTiO3 interface differs significantly from that of the as-deposited interface. After oxidation, the Pt atoms shifted upward and their atomic occupation at fcc-like sites evolved as the oxidation temperature increased. Interfacial oxygen atoms were differentiated from bulk O atoms by the chemical shift in the binding energy of their 1s electrons. After oxidation, the interfacial oxygen atoms rearranged to form a TiO2 bilayer at the interface. These results provide a more complete description of the strong metal-support interaction process at the interface.

Harnessing Standing Sound Waves to Treat Intraocular Blood Cell Accumulation.

Certain ocular conditions result from the non-physiological presence of intraocular particles, leading to visual impairment and potential long-term damage. This happens when the normally clear aqueous humor becomes less transparent, thus blocking the visual axis and by intraocular pressure elevation due to blockage of the trabecular meshwork, as seen in secondary open-angle glaucoma (SOAG). Some of these "particle-related pathologies" acquire ocular conditions like pigment dispersion syndrome, pseodoexfoliation and uveitis. Others are trauma-related, such as blood cell accumulation in hyphema. While medical and surgical treatments exist for SOAG, there is a notable absence of effective preventive measures. Consequently, the prevailing clinical approach predominantly adopts a "wait and see" strategy, wherein the focus lies on managing secondary complications and offers no treatment options for particulate matter disposal. We developed a new technique utilizing standing acoustic waves to trap and direct intraocular particles. By employing acoustic trapping at nodal regions and controlled movement of the acoustic transducer, we successfully directed these particles to specific locations within the angle. Here, we demonstrate control and movement of polystyrene (PS) particles to specific locations within an in vitro eye model, as well as blood cells in porcine eyes (ex vivo). The removal of particles from certain areas can facilitate the outflow of aqueous humor (AH) and help maintain optimal intraocular pressure (IOP) levels, resulting in a non-invasive tool for preventing secondary glaucoma. Furthermore, by controlling the location of trapped particles we can hasten the clearance of the AH and improve visual acuity and quality more effectively. This study represents a significant step towards the practical application of our technique in clinical use.

The resonant behavior of airborne standing-wave acoustic levitators based on arrays of ultrasonic transducers.

Recently airborne standing-wave acoustic levitation has seen great advances, and its applicability has been broadened due to the development of cavities constructed with arrays of compact ultrasonic sources. Yet, the numerical methods employed to study and predict the pressure distributions inside these cavities do not consider the effect of multiple reflections on the boundaries, hiding their resonant effects. This work presents an analytical, numerical, and experimental study of the effect of multiple reflections inside ultrasonic cavities based on arrays of transducers exhibiting their influence on the pressure amplitudes of focused standing waves. Our numerical results come from a modified version of the Matrix Method to numerically compute the multiple wave reflections of cavities constructed by two opposite arrays of multiple compact sources as boundaries. The correlation between numerical and experimental results reveals that intra-cavity reflections are relevant in focused axisymmetric cavities based on two arrays of multiple ultrasonic sources having a considerable impact on the amplitude of the standing waves and consequently, on the acoustic levitation performance. Thus, intra-cavity reflections must be considered for optimal cavity designs.

Enhanced standing-wave acoustic levitation using high-order transverse modes in phased array ultrasonic cavities.

Airborne acoustic trapping by ultrasonic phased arrays has seen great advances in recent years, and yet the manipulation of objects with different shapes and sizes or heavy particles remains challenging. Here, we demonstrate that the manipulation capabilities of a standing-wave acoustic levitator can be extended by introducing intracavity high-order transverse (HOT) modes in the azimuthal direction, enabling the simultaneous trapping of several objects within a wide range of shapes and sizes with positional and rotational stability, including objects with sizes larger than one wavelength and weights in the scale of millinewtons. The conditions to generate different HOT modes are theoretically analyzed and experimentally implemented. We numerically calculate the pressure distributions, exhibiting good qualitative agreement with the experimental pressure distributions obtained with schlieren images. In addition, we calculate the acoustic force field for several examples of HOT modes and different particle sizes, which leads to a qualitative understanding of the experimental observations.

Laboratory-based 3D X-ray standing-wave analysis of nanometre-scale gratings.

The increasing structural complexity and downscaling of modern nanodevices require continuous development of structural characterization techniques that support R&D and manufacturing processes. This work explores the capability of laboratory characterization of periodic planar nanostructures using 3D X-ray standing waves as a promising method for reconstructing atomic profiles of planar nanostructures. The non-destructive nature of this metrology technique makes it highly versatile and particularly suitable for studying various types of samples. Moreover, it eliminates the need for additional sample preparation before use and can achieve sub-nanometre reconstruction resolution using widely available laboratory setups, as demonstrated on a diffractometer equipped with a microfocus X-ray tube with a copper anode.

Nonlinear standing waves for assessing material nonlinearity in thin samples.

The second harmonic generation (SHG) technique offers a quantitative damage parameter known as the acoustic nonlinearity parameter (ß) capable of detecting the change in the inherent material nonlinearity. However, current SHG methods, in particular, those used for measuring ß in construction materials, have an unresolved issue in their application due to limited sample sizes. The restricted sample dimensions lead to the generation of boundary-reflected waves, which hinder the selective detection of propagating waves and thus the precise evaluation of material nonlinearity through ß. Furthermore, the use of large samples limits the compatibility of the SHG method with other characterization modalities, such as mechanical tests, X-ray diffraction, and computerized tomography. To address this issue, this paper introduces a new SHG method that is based on the use of nonlinear standing waves - the dominant longitudinal standing waves in a forced-free configuration. The corrections for phase delay and attenuation effect of each reflected wave are made, enabling accurate measurements of ß in thin samples with no requirement in the thickness-wavelength ratio. The measured ß is then employed to quantify the microstructural modification in cement paste induced by thermal damage, validating the proposed method as a promising tool for quantifying microstructural changes in materials.

X-ray standing wave characterization of the strong metal-support interaction in Co/TiOx model catalysts.

The strong metal-support interaction (SMSI) is a phenomenon observed in supported metal catalyst systems in which reducible metal oxide supports can form overlayers over the surface of active metal nanoparticles (NPs) under a hydrogen (H2) environment at elevated temperatures. SMSI has been shown to affect catalyst performance in many reactions by changing the type and number of active sites on the catalyst surface. Laboratory methods for the analysis of SMSI at the nanoparticle-ensemble level are lacking and mostly based on indirect evidence, such as gas chemisorption. Here, we demonstrate the possibility to detect and characterize SMSIs in Co/TiOx model catalysts using the laboratory X-ray standing wave (XSW) technique for a large ensemble of NPs at the bulk scale. We designed a thermally stable MoNx/SiNx periodic multilayer to retain XSW generation after reduction with H2 gas at 600°C. The model catalyst system was synthesized here by deposition of a thin TiOx layer on top of the periodic multilayer, followed by Co NP deposition via spare ablation. A partial encapsulation of Co NPs by TiOx was identified by analyzing the change in Ti atomic distribution. This novel methodological approach can be extended to observe surface restructuring of model catalysts in situ at high temperature (up to 1000°C) and pressure (≤3 mbar), and can also be relevant for fundamental studies in the thermal stability of membranes, as well as metallurgy.

Spatiotemporal resonance in mouse primary visual cortex.

Human primary visual cortex (V1) responds more strongly, or resonates, when exposed to ∼10, ∼15-20, and ∼40-50 Hz rhythmic flickering light. Full-field flicker also evokes the perception of hallucinatory geometric patterns, which mathematical models explain as standing-wave formations emerging from periodic forcing at resonant frequencies of the simulated neural network. However, empirical evidence for such flicker-induced standing waves in the visual cortex was missing. We recorded cortical responses to flicker in awake mice using high-spatial-resolution widefield imaging in combination with high-temporal-resolution glutamate-sensing fluorescent reporter (iGluSnFR). The temporal frequency tuning curves in the mouse V1 were similar to those observed in humans, showing a banded structure with multiple resonance peaks (8, 15, and 33 Hz). Spatially, all flicker frequencies evoked responses in V1 corresponding to retinotopic stimulus location, but some evoked additional peaks. These flicker-induced cortical patterns displayed standing-wave characteristics and matched linear wave equation solutions in an area restricted to the visual cortex. Taken together, the interaction of periodic traveling waves with cortical area boundaries leads to spatiotemporal activity patterns that may affect perception.

Numerical Analysis of Standing Waves Phenomenon of Aircraft Tires.

In this paper, the generation mechanisms of standing waves on aircraft tires are discussed by comparing the time-domain model and FEA model. Unlike passenger car tires, aircraft tires accelerate to landing speed sharply when the airplane lands. According to the tire structure, the detailed finite element model of the aircraft tires is established in ABAQUS. The tire model runs on a 1.7 m spinning drum and accelerates to 300 km/h in 0.3 s. The proposed finite element model is verified by comparing the simulation results under inflation and static load with the experimental results. Similarly, by analyzing and comparing the calculated values of the time-domain model and FEA model, the variation of standing wave wavelength at different speeds is studied. In addition, the stress and strain field of the aircraft tires standing wave is analyzed. According to the definition of tire standing wave, a method for determining critical speed is proposed. Finally, the effects of tire inflation pressure and vertical load on the occurrence of standing waves were studied.

Acoustic Manipulation of Intraocular Particles.

Various conditions cause dispersions of particulate matter to circulate inside the anterior chamber of a human eye. These dispersed particles might reduce visual acuity or promote elevation of intraocular pressure (IOP), causing secondary complications such as particle related glaucoma, which is a major cause of blindness. Medical and surgical treatment options are available to manage these complications, yet preventive measures are not currently available. Conceptually, manipulating these dispersed particles in a way that reduces their negative impact could prevent these complications. However, as the eye is a closed system, manipulating dispersed particles in it is challenging. Standing acoustic waves have been previously shown to be a versatile tool for manipulation of bioparticles from nano-sized extracellular vesicles up to millimeter-sized organisms. Here we introduce for the first time a novel method utilizing standing acoustic waves to noninvasively manipulate intraocular particles inside the anterior chamber. Using a cylindrical acoustic resonator, we show ex vivo manipulation of pigmentary particles inside porcine eyes. We study the effect of wave intensity over time and rule out temperature changes that could damage tissues. Optical coherence tomography and histologic evaluations show no signs of damage or any other side effect that could be attributed to acoustic manipulation. Finally, we lay out a clear pathway to how this technique can be used as a non-invasive tool for preventing secondary glaucoma. This concept has the potential to control and arrange intraocular particles in specific locations without causing any damage to ocular tissue and allow aqueous humor normal outflow which is crucial for maintaining proper IOP levels.

Traditional Multiwell Plates and Petri Dishes Limit the Evaluation of the Effects of Ultrasound on Cells In Vitro.

Ultrasound accelerates healing in fractured bone; however, the mechanisms responsible are poorly understood. Experimental setups and ultrasound exposures vary or are not adequately characterized across studies, resulting in inter-study variation and difficulty in concluding biological effects. This study investigated experimental variability introduced through the cell culture platform used. Continuous wave ultrasound (45 kHz; 10, 25 or 75 mW/cm2, 5 min/d) was applied, using a Duoson device, to Saos-2 cells seeded in multiwell plates or Petri dishes. Pressure field and vibration quantification and finite-element modelling suggested formation of complex interference patterns, resulting in localized displacement and velocity gradients, more pronounced in multiwell plates. Cell experiments revealed lower metabolic activities in both culture platforms at higher ultrasound intensities and absence of mineralization in certain regions of multiwell plates but not in Petri dishes. Thus, the same transducer produced variable results in different cell culture platforms. Analysis on Petri dishes further revealed that higher intensities reduced vinculin expression and distorted cell morphology, while causing mitochondrial and endoplasmic reticulum damage and accumulation of cells in sub-G1 phase, leading to cell death. More defined experimental setups and reproducible ultrasound exposure systems are required to study the real effect of ultrasound on cells for development of effective ultrasound-based therapies not just limited to bone repair and regeneration.

Practical scale modification of oleogels by ultrasonic standing waves.

Lipid-based materials, such as substitutes for saturated fats (oleogels) structurally modified with ultrasonic standing waves (USW), have been developed by our group. To enable their potential application in food products, pharmaceuticals, and cosmetics, practical and economical production methods are needed. Here, we report scale-up of our procedure of structurally modifying oleogels via the use of USW by a factor of 200 compared to our previous microfluidic chamber. To this end, we compared three different USW chamber prototypes through finite element simulations (FEM) and experimental work. Imaging of the internal structure of USW-treated oleogels was used as feedback for successful development of chambers, i.e., the formation of band-like structures was the guiding factor in chamber development. We then studied the bulk mechanical properties by a uniaxial compression test of the sonicated oleogels obtained with the most promising USW chamber, and sampled local mechanical properties using scanning acoustic microscopy. The results were interpreted using a hyperelastic foam model. The stability of the sonicated oleogels was compared to control samples using automated image analysis oil-release tests. This work enabled the effective mechanical-structural manipulation of oleogels in volumes of 10-100 mL, thus paving the way for USW treatments of large-scale lipid-based materials.