Electrolysis of water is an attractive hydrogen generation method. As the most efficient catalyst for this reaction is platinum (Pt), what makes this approach expensive, many studies focus on enhancing the hydrogen producing efficiency of other inexpensive catalysts. In this study, an Au electrode and Au supported Pt/ TiO2 electrode without UV illumination were chosen as the catalyst for electrochemical hydrogen evolution reaction (HER) in acidic solution, and a Rayleigh-type surface acoustic wave (SAW) was used to promote the HER. Our results demonstrate that under the influence of SAW, both electrodes exhibit better HER activity with a higher current in the polarization curves from cyclic voltammetry. Analyzing the Tafel slope and the exchange current density with and without the effect of SAW suggests the enhancement of the HER activity especially at low overpotentials up to 100 mV. The effect strength increases with increasing power of the radio frequency (RF) signal. Various control experiments indicate that this is mainly induced by a microstreaming effect caused by the mechanical vibration of the SAW, while an off-resonance RF signal with a comparable electric field only reaches about 16.5 % of the increase of the current density at medium overpotentials. Thus, SAW-induced acoustic streaming is shown as tunable method to boost hydrogen production especially in the low and medium range of overpotential with promising potential for broader application in electrocatalysis and photocatalysis.
We quantify endocytosis-like nanoparticle uptake of model membranes as a function of temperature and therefore phase state. As model membranes, we use giant unilamellar vesicles consisting of 1,2-dipentadecanoyl-sn-glycero-3-phosphocholine (15:0 PC). Time-series micrographs of the vesicle shrinkage show uptake rates that are a highly non-linear function of temperature. A global maximum appears close to the main structural phase transition at T = T m + 3 K, and a minor peak at the pretransition T = T p = 22 °C. The quality of the kinetics linear fits reveals a deviation from the linear trend at the vesicle shrinkage peaks. To further elucidate the origin of the shrinkage peak, we performed force spectroscopy on a supported lipid bilayer. The results indicate a collapse of the adhesion energy at the structural phase transition. Further using literature results on the bending modulus as function of temperature and Helfrich’s model, this allows us to make qualitative conclusions on the membrane tension as function of temperature.
With a view on adding to their use in trace gas sensing, we perform a combined experimental and theoretical study of the change of the conductivity of a metal organic framework (iron (1,2,3)-triazolate, Fe(ta)2) with the uptake of chemically inert gases. To align our first-principles calculations with experimental measurements, we perform an ensemble average over different microscopic arrangements of the gas molecules in the pores of the metal-organic framework (MOF). Up to the experimentally reachable limit of gas uptake, we find a good agreement between both approaches. Thus, we can employ theory to further interpret our experimental results in terms of changes to the parameters of the Bardeen-Shockley band theory, electron-phonon coupling (in the form of the deformation potential), bulk modulus, and carrier effective mass. We find the first of these to be most strongly influenced through the gas uptake. Furthermore, we find the changes to the deformation potential to strongly depend on the individual microscopic arrangements of molecules in the pores of the MOF. This hints at a possible synthetic engineering of the material, e.g., by closing off certain pores, for a stronger, more interpretable electric response upon gas sorption.
Direct conversion of X-ray irradiation using a semiconductor material is an emerging technology in medical and material sciences. Existing technologies face problems, such as sensitivity or resilience. Here, we describe a novel class of X-ray sensors based on GaN thin film and GaN/AlGaN high-electron-mobility transistors (HEMTs), a promising enabling technology in the modern world of GaN devices for high power, high temperature, high frequency, optoelectronic, and military/space applications. The GaN/AlGaN HEMT-based X-ray sensors offer superior performance, as evidenced by higher sensitivity due to intensification of electrons in the two-dimensional electron gas (2DEG), by ionizing radiation. This increase in detector sensitivity, by a factor of 104 compared to GaN thin film, now offers the opportunity to reduce health risks associated with the steady increase in CT scans in today's medicine, and the associated increase in exposure to harmful ionizing radiation, by introducing GaN/AlGaN sensors into X-ray imaging devices, for the benefit of the patient.
In prototype ferromagnet-antiferromagnet interfaces we demonstrate that surface acoustic waves can be used to identify complex magnetic phases arising upon evolution of exchange springs in an applied field. Applying sub-GHz surface acoustic waves to study the domain structure of the ferromagnetic layer in exchange-biased bilayers of Ir20Mn80-Co60Fe20B20, we are able to associate the magnetoelastic resonance with the presence of the exchange spin-spirals in both the ferromagnetic and antiferromagnetic layer. Our findings offer a complementary, integrative insight into emergent magnetic materials for applications of noncollinear spin textures in view of low-energy-consumption spintronic devices.
The interaction between surface acoustic waves (SAWs) and spin waves (SWs) in a piezoelectric-magnetic thin film heterostructure yields potential for the realization of novel microwave devices and applications in magnonics. In the present work, we characterize magnetoacoustic waves in three adjacent magnetic micro-stripes made from CoFe + Ga, CoFe, and CoFe + Pt with a single pair of tapered interdigital transducers (TIDTs). The magnetic micro-stripes were deposited by focused electron beam-induced deposition and focused ion beam-induced deposition direct-writing techniques. The transmission characteristics of the TIDTs are leveraged to selectively address the individual micro-stripes. Here, the external magnetic field is continuously rotated out of the plane of the magnetic thin film and the forward volume SW geometry is probed with the external magnetic field along the film normal. Our experimental findings are well explained by an extended phenomenological model based on a modified Landau–Lifshitz–Gilbert approach that considers SWs with nonzero wave vectors. Magnetoelastic excitation of forward volume SWs is possible because of the vertical shear strain ɛxz of the Rayleigh-type SAW.
With the development of ink jet printers or spotters for biological applications, the control size and homogeneity of small fluids as well as their successful deposition on various substrates has gained significant importance. We study the impingement process of such small droplets onto a solid substrate and investigate their evaporation and drying process by means of surface acoustic wave (SAW) transmission experiments. We observe a strong fluid-SAW interaction resulting in an attenuation which toward the end of the evaporation and drying process exhibits characteristic oscillations being related to temperature, SAW amplitude, and fluid properties such as viscosity and wetting angle. It is found that oscillations can only be seen in pinned, very flat droplets, while the pinning can be roughly controlled via the SAW amplitude. The frequency of those characteristic oscillations is superlinear with respect to temperature, rather proportional to the evaporation rate and can change drastically depending on the liquid used. In our experiments, isopropanol, ethanol, and water with various glycerol concentrations were loaded onto the SAW delay line. Based on the experimental results, simulations using the finite element method were performed. We find that a standing wave pattern within the droplet is responsible for the transmission oscillations. These findings might lead to new methods, e.g., sensory systems, being able to examine droplets according to their physical or chemical properties.
A Love-wave based biosensor is introduced for analyzing a standardized wound healing assay by observing cell growth and quantifying cell detachment processes. Utilizing the piezoelectric material LiTaO3 36° XY-cut with a thin SiO2-cover layer, shear horizontal surface acoustic waves (SAW) are excited and detected by a set of Interdigital Transducers. Epithelial cells, being cultivated on the substrate and invading the sensors delay line cause a phase shift in the transmitted SAW signal. This phase shift correlates exactly with the surface coverage of the invading cells. After wound healing, emerging fluctuations in the phase shift signal provide information about the cell growth in a confluent cell layer. Additionally, the signal slope allows to quantify the cell detachment process induced by apoptosis, necrosis or cell lysis substances, respectively. Furthermore, culture conditions like temperature or osmolality can be simultaneously monitored by SAW. Based on a theoretical approach and using FEM simulations, we identified the acoustoelectric interaction as the main reason for the phase shift in various frequency- and time-dependent studies. Our model is validated by experimental data and allows predicting the phase change caused by variations in the cell-substrate distance or the volume ratio of the nucleus and the complete cell.
Membrane-associated enzymes have been found to behave differently qualitatively and quantitatively in terms of activity. These findings were highly debated in the 1970s and many general correlations and reaction specific models have been proposed, reviewed, and discarded. However, new biological applications brought up the need for clarification and elucidation. To address literature shortcomings, we chose the intrinsically water-soluble enzyme a disintegrin and metalloproteinase with a thrombospondin type 1 motif, member 13 (ADAMTS13) and large unilamellar vesicles with a relative broad phase transition. We here present activity measurements of ADAMTS13 in the freely dissolved state and the membrane associated state for phosphocholine lipids with different acyl-chain lengths (13:0, 14:0 and 15:0) and thus main phase transition temperatures. While the freely dissolved enzyme shows a simple Arrhenius behavior, the activity of membrane associated ADAMTS13 in addition shows a peak. This peak temperature correlates with the main phase transition temperature of the used lipids. These findings support an alternative theory of catalysis. This theory predicts a correlation of the membrane associated activity and the heat capacity, as both are susceptibilities of the same surface Gibb's free energy, since the enzyme is attached to the membrane.
In this study, we present proof of concept for an x-ray detector. The hybrid device consists of a synthetic single crystal diamond in mechanical contact with a piezoelectric lithium niobate surface acoustic wave (SAW) delay line. Upon x-ray irradiation, the diamond crystal experiences a change in conductivity, which, in turn, very sensitively influences the SAW transmission on the delay line. This change in SAW attenuation is directly used to monitor the x-ray beam intensity. The SAW attenuation shows a monotonic variation with dose rate D in the studied range between 100 and 1800 μGy/s. While the response time leaves room for further improvement, the SAW detection principle offers the unique possibility for wireless remote powering and sensing.
Here, we present a novel approach for the transient permeabilization of cells. We combined laminar shear flow in a microchannel with chaotic advection employing surface acoustic waves. First, as a fundamental result on the one hand, and as a kind of reference measurement for the more complex acoustofluidic approach on the other hand, we studied the permeabilization of cells in pure shear flow in a microchannel with Y-geometry. As a proof of principle, we used fluorescent dyes as model drugs and investigated their internalization into HeLa cells. We found that drug uptake scaled non-linearly with flow rate and thus shear stress. For calcein, we obtained a maximal enhancement factor of about 12 at an optimum flow rate of Q = 500 µL/h in the geometry used here compared to static incubation. This result is discussed in the light of structural phase transitions of lipid membranes accompanied by non-linear effects, as the plasma membrane is the main barrier to overcome. Second, we demonstrated the enhanced permeabilization of acoustically trapped cells in surface acoustic wave induced vortices in a microchannel, with an enhancement factor of about 18 compared to quasi-static incubation. Moreover, we optimized the trapping conditions regarding flow rate, the power level of the surface acoustic wave, and trapping time. Finally, we showed that our method is not limited to small molecules but can also be applied to compounds with higher molecular weight.
Surface acoustic waves double the photocatalytic activity of platinum-doped titanium dioxide for water splitting with methanol as a sacrificial material.
A fluid-independent ultrasonic approach for flow determination in microchannels in the harsh environment of an ultra high pressure liquid chromatography (UHPLC) system is presented. Ultrasonic waves in the fluid are excited by separate media surface acoustic waves (SAW) of Rayleigh-Wave type. The LiNbO3 SAW chip being equipped with interdigitated transducers for SAW excitation also marks the bottom of the fluid channel and thus allows for very effective SAW coupling to the fluid. The channel ceiling acts as an acoustical mirror for longitudinal ultrasonic waves propagating through the fluid. To deduce the fluid flow from the ultrasonic transmission after reflection, we employ a combination of time differential phase and time of flight measurements with a two port vector network analyzer. To verify and assign our experimental results, we use an adapted time explicit finite element method. In the simulation, both the piezoelectric single crystal and the fluid are included and we solve the linear Navier-Stokes equation to evaluate the background flow. By changing the ultrasonic propagation direction, we are able to deduce the fluid volume flow over time with very high accuracy, independent of the actual liquid in the channel.
We study the interaction of surface acoustic waves (SAWs) with spin waves (SWs) in a Co40Fe40B20/Au/Ni81Fe19 system composed of two ferromagnetic layers separated by a nonmagnetic Au spacer layer. Because of interlayer magnetic dipolar coupling between the two ferromagnetic layers, a symmetric and an antisymmetric SW mode form, which both show a highly nondegenerate dispersion relation for oppositely propagating SWs. Due to magnetoacoustic SAW-SW interaction, we observe highly nonreciprocal SAW transmission in the piezoelectric-ferromagnetic hybrid device. We experimentally and theoretically characterize the magnetoacoustic wave propagation as a function of frequency, wave vector, and external magnetic field magnitude and orientation. Additionally, we demonstrate that the nonreciprocal SW dispersion of a coupled magnetic bilayer is highly tuneable and not limited to ultrathin magnetic films, in contrast to the nonreciprocity induced by the interfacial Dzyaloshinskii-Moriya interaction. Therefore, magnetoacoustic coupling in ferromagnetic multilayers provides a promising route towards building efficient acoustic isolators.
We study the interaction of Rayleigh and shear horizontal surface acoustic waves (SAWs) with spin waves in thin Ni films on a piezoelectric LiTaO$_3$ substrate, which supports both SAW modes simultaneously. Because Rayleigh and shear horizontal modes induce different strain components in the Ni thin films, the symmetries of the magnetoelastic driving fields, of the magnetoelastic response, and of the transmission nonreciprocity differ for both SAW modes. Our experimental findings are well explained by a theoretical model based on a modified Landau-Lifshitz-Gilbert approach. We show that the symmetries of the magnetoelastic response driven by Rayleigh- and shear horizontal SAWs complement each other, which makes it possible to excite spin waves for any relative orientation of magnetization and SAW propagation direction and, moreover, can be utilized to characterize surface strain components of unknown acoustic wave modes.
We study the interaction of surface acoustic waves with spin waves in ultrathin CoFeB/Pt bilayers. Because of the interfacial Dzyaloshinskii-Moriya interaction (DMI), the spin wave dispersion is nondegenerate for oppositely propagating spin waves in CoFeB/Pt. In combination with the additional nonreciprocity of the magnetoacoustic coupling itself, which is independent of the DMI, highly nonreciprocal acoustic wave transmission through the magnetic film is observed. We systematically characterize the magnetoacoustic wave propagation in a thickness series of CoFeB(d)/Pt samples as a function of magnetic field magnitude and direction, and at frequencies up to 7 GHz. We quantitatively model our results to extract the strength of the DMI and magnetoacoustic driving fields.
For Plasmodium falciparum related malaria (B50), one of the outstanding host factors for the development of severe disease is the ABO blood group of malaria patients, where blood group O reduces the probability of severe disease as compared to individuals of groups A, B, or AB. In this report, we investigate the stability of rosette aggregates in malaria caused by Plasmodium falciparum in microflows. These flows are created in microfluidic channels with stenosis-like constrictions of different widths down to ones narrower as the rosette's diameter. High speed videos were recorded and analyzed by a MATLAB© based tracking software (SURF: SUrvival of Rosettes in Flow). We find a correlation of rosette size, channel diameter, and blood group regarding the mobility of the rosettes. Following the concept of a thermodynamic model, we find a critical width of the stenosis for rosette rupture during their passage. Our data reveal that under physiologically relevant conditions, rosettes in blood group A have a higher rosette frequency and stability as compared to blood group O (BG O), which constitutes a crucial factor promoting the observed protection in BG O individuals against severe malaria in non-O individuals.
Significance Ultrasonic pressure fields have been proven to be beneficial for cell growth in vitro and in patients. However, conventional therapeutic-ultrasound treatment is subjected to limitations such as time restriction, external application, or energy loss. The application of surface acoustic waves (SAWs) can help to overcome some drawbacks. To understand the underlying mechanism, the adjusting parameters of SAWs and the intracellular response to the stimulation are evaluated. We identified a dependence of cell growth on SAW intensity and the presence of a vertical substrate deflection. While the cellular stress (reactive oxygen species) remains in the normal range, both cell migration and proliferation are increased. Due to the experimental design, the effect of enhanced cell growth is dominated by increased cell migration.
Unilamellar lipid vesicles can serve as model for protocells. We present a vesicle fission mechanism in a thermal gradient under flow in a convection chamber, where vesicles cycle cold and hot regions periodically. Crucial to obtain fission of the vesicles in this scenario is a temperature-induced membrane phase transition that vesicles experience multiple times. We model the temperature gradient of the chamber with a capillary to study single vesicles on their way through the temperature gradient in an external field of shear forces. Starting in the gel-like phase the spherical vesicles are heated above their main melting temperature resulting in a dumbbell-deformation. Further downstream a temperature drop below the transition temperature induces splitting of the vesicles without further physical or chemical intervention. This mechanism also holds for less cooperative systems, as shown here for a lipid alloy with a broad transition temperature width of 8 K. We find a critical tether length that can be understood from the transition width and the locally applied temperature gradient. This combination of a temperature-induced membrane phase transition and realistic flow scenarios as given e.g. in a white smoker enable a fission mechanism that can contribute to the understanding of more advanced protocell cycles.