High-sensitivity narrow­band T-shaped cantilever Fabry-perot acoustic sensor for photoacoustic spectroscopy.

Photoacoustic spectroscopy (PAS) has been rapidly developed and applied to different detection scenarios. The acoustic pressure detection is an important part in the PAS system. In this paper, an ultrahigh sensitivity Fabry-Perot acoustic sensor with a T-shaped cantilever was proposed. To achieve the best acoustic pressure effect, the dimension of the cantilever structure was designed and optimized by finite element analysis using COMSOL Multiphysics. Simulation results showed that the sensitivity of such T-shaped cantilever was 1.5 times higher than that based on a rectangular cantilever, and the resonance frequency of T-shaped cantilever were able to modulate from 800 Hz to 1500 Hz by adjusting the multi-parameter characteristics. Experimental sensing results showed that the resonance frequency of T-shaped Fabry-Perot acoustic sensor was 1080 Hz, yielding a high sensitivity of 1.428 µm/Pa, with a signal-to-noise ratio (SNR) of 84.8 dB and a detectable pressure limit of 1.9 µPa/Hz1/2@1 kHz. We successfully used such acoustic sensor to measure acetylene (C2H2) concentration in the PAS. The sensitivity of PAS for C2H2 gas was 3.22 pm/ppm with a concentration range of 50 ppm ∼100 ppm, and the minimum detection limit was 24.91ppb.

A nanonewton force sensor using a U-shape tapered microfiber interferometer.

Nanomechanical measurements, especially the detection of weak contact forces, play a vital role in many fields, such as material science, micromanipulation, and mechanobiology. However, it remains a challenging task to realize the measurement of ultraweak force levels as low as nanonewtons with a simple sensing configuration. In this work, an ultrasensitive all-fiber nanonewton force sensor structure based on a single-mode-tapered U-shape multimode-single-mode fiber probe is proposed and experimentally demonstrated with a limit of detection of ~5.4 nanonewtons. The use of the sensor is demonstrated by force measurement on a human hair sample to determine the spring constant of the hair. The results agree well with measurements using an atomic force microscope for the spring constant of the hair. Compared with other force sensors based on optical fiber in the literature, the proposed all-fiber force sensor provides a substantial advancement in the minimum detectable force possible, with the advantages of a simple configuration, ease of fabrication, and low cost.

Capillary wave tweezer.

Precise control of microparticle movement is crucial in high throughput processing for various applications in scalable manufacturing, such as particle monolayer assembly and 3D bio-printing. Current techniques using acoustic, electrical and optical methods offer precise manipulation advantages, but their scalability is restricted due to issues such as, high input powers and complex fabrication and operation processes. In this work, we introduce the concept of capillary wave tweezers, where mm-scale capillary wave fields are dynamically manipulated to control the position of microparticles in a liquid volume. Capillary waves are generated in an open liquid volume using low frequency vibrations (in the range of 10-100 Hz) to trap particles underneath the nodes of the capillary waves. By shifting the displacement nodes of the waves, the trapped particles are precisely displaced. Using analytical and numerical models, we identify conditions under which a stable control over particle motion is achieved. By showcasing the ability to dynamically control the movement of microparticles, our concept offers a simple and high throughput method to manipulate particles in open systems.

The novel π-d conjugated TM2B3N3S6 (TM = Mo, Ti and W) monolayers as highly active single-atom catalysts for electrocatalytic synthesis of ammonia.

Recently, single-atom catalysts (SACs) are receiving significant attention in electrocatalysis fields due to their excellent specific activities and extremely high atomic utilization ratio. Effective loading of metal atoms and high stability of SACs increase the number of exposed active sites, thus significantly improving their catalytic efficiency. Herein, we proposed a series (29 in total) of two-dimensional (2D) conjugated structures of TM2B3N3S6 (TM means those 3d to 5d transition metals) and studied the performance as single-atom catalysts for nitrogen reduction reaction (NRR) using density functional theory (DFT). Results show that TM2B3N3S6 (TM = Mo, Ti and W) monolayers have superior performance for ammonia synthesis with low limiting potentials of -0.38, -0.53 and -0.68 V, respectively. Among them, the Mo2B3N3S6 monolayer shows the best catalytic performance of NRR. Meanwhile, the π conjugated B3N3S6 rings undergo coordinated electron transfer with the d orbitals of TM to exhibit good chargeability, and these TM2B3N3S6 monolayers activate isolated N2 according to the "acceptance-donation" mechanism. We have also verified the good stability (i.e., Ef < 0, and Udiss > 0) and high selectivity (Ud = -0.03, 0.01 and 0.10 V, respectively) of the above four types of monolayers for NRR over hydrogen evolution reaction (HER). The NRR activities have been clarified by multiple-level descriptors (ΔG*N2H, ICOHP, and Ɛd) in the terms of basic characteristics, electronic property, and energy. Moreover, the aqueous solution can promote the NRR process, leading to the reduction of ΔGPDS from 0.38 eV to 0.27 eV for the Mo2B3N3S6 monolayer. However, the TM2B3N3S6 (TM = Mo, Ti and W) also showed excellent stability in aqueous phase. This study proves that the π-d conjugated monolayers of TM2B3N3S6 (TM = Mo, Ti and W) as electrocatalysts show great potentials for the nitrogen reduction.

A phase transition model in dual-amorphous water undergoing liquid-liquid transition.

An in-depth understanding of liquid-liquid phase transition (LLPT) in condensed water will gain insight into anomalous behaviors of dual-amorphous condensed water. Despite numerous experimental, molecular simulation, and theoretical studies, it is yet to achieve a widely accepted consensus with convinced evidence in the condensed matter physics for two-state liquid-liquid transition of water. In this work, a theoretical model is proposed based on the Avrami equation, commonly used to describe first-order phase transitions, to elucidate complex homogeneous and inhomogeneous condensation from high-density liquid (HDL) water to low-density liquid (LDL) water for both pure and ionic dual-amorphous condensed water. This model unifies the coupling effects of temperature and electrolyte concentration based on the new theoretical framework. The Adam-Gibbs theory is then introduced to characterize the synergistic motion and relaxation behavior of condensed water. Variations in the configurational entropy under electrostatic forces are further explored, and an analytical 2D cloud chart is developed to visualize the synergistic effect of temperature and electrolyte concentration on the configurational entropy of ionic water. The constitutive relationships among viscosity, temperature, and electrolyte concentration are derived to analyze their synergistic effects under different condensation fractions of LDL and HDL. The Stokes-Einstein relation and free volume theory are further used to analyze diffusion coefficients and densities (or apparent density) during both pure and ionic LLPT. Finally, theoretical results obtained from these models are compared with experimental results reported in literature to validate the accuracy and applicability of the proposed models, which offer significant benefits and advancements in effectively predicting physical property changes of dual-amorphous condensed water.

Impact Dynamics of Non-Newtonian Droplets on Superhydrophobic Surfaces.

Droplet impact behavior on a solid surface is critical for many industrial applications such as spray coating, food production, printing, and agriculture. For all of these applications, a common challenge is to modify and control the impact regime and contact time of the droplets. This challenge becomes more critical for non-Newtonian liquids with complex rheology. In this research, we explored the impact dynamics of non-Newtonian liquids (by adding different concentrations of Xanthan into water) on superhydrophobic surfaces. Our experimental results show that by increasing the Xanthan concentration in water, the shapes of the bouncing droplet are dramatically altered, e.g., its shape at the separation moment is changed from a conventional vertical jetting into a "mushroom"-like one. As a result, the contact time of the non-Newtonian droplet could be reduced by up to ∼50%. We compare the impact scenarios of Xanthan liquids with those of glycerol solutions having a similar apparent viscosity, and results show that the differences in the elongation viscosity induce different impact dynamics of the droplets. Finally, we show that by increasing the Weber number for all of the liquids, the contact time is reduced, and the maximum spreading radius is increased.

Dual-Wave Acoustofluidic Centrifuge for Ultrafast Concentration of Nanoparticles and Extracellular Vesicles.

Extracellular vesicles (EVs) are secreted nanostructures that play various roles in critical cancer processes. They operate as an intercellular communication system, transferring complex sets of biomolecules from cell to cell. The concentration of EVs is difficult to decipher, and there is an unmet technological need for improved (faster, simpler, and gentler) approaches to isolate EVs from complex matrices. Herein, an acoustofluidic concentration of extracellular vesicles (ACEV) is presented, based on a thin-film printed circuit board with interdigital electrodes mounted on a piezoelectric substrate. An angle of 120° is identified between the electrodes and the reference flat of the piezoelectric substrate for simultaneous generation of Rayleigh and shear horizontal waves. The dual waves create a complex acoustic field in a droplet, resulting in effective concentration of nanoparticles and EVs. The ACEV is able to concentrate 20 nm nanospheres within 105 s and four EV dilutions derived from the human prostate cancer (Du145) cell line in approximately 30 s. Cryo-electron microscopy confirmed the preservation of EV integrity. The ACEV device holds great potential to revolutionize investigations of EVs. Its faster, simpler, and gentler approach to EV isolation and concentration can save time and effort in phenotypic and functional studies of EVs.

Metal-organic framework-derived trimetallic oxides with dual sensing functions for ethanol.

Metal-organic framework (MOF)-derived metal oxide semiconductors have recently received extensive attention in gas sensing applications due to their high porosity and three-dimensional architecture. Still, challenges remain for MOF-derived materials, including low-cost and facile synthetic methods, rational nanostructure design, and superior gas-sensing performances. Herein, a series of Fe-MIL-88B-derived trimetallic FeCoNi oxides (FCN-MOS) with a mesoporous structure were synthesized by a one-step hydrothermal reaction followed by calcination. The FCN-MOS system consists of three main phases: α-Fe2O3 (n-type), CoFe2O4, and NiFe2O4 (p-type), and the nanostructure and pore size can be controlled by altering the content of α-Fe2O3, CoFe2O4, and NiFe2O4. The sensors based on FCN-MOS exhibit a high response of 71.9, a good selectivity towards 100 ppm ethanol at 250 °C, and long-term stability up to 60 days. Additionally, the FCN-MOS-based sensors show a p-n transition gas sensing behavior with the alteration of the Fe/Co/Ni ratio.

Integrated label-free erbium-doped fiber laser biosensing system for detection of single cell Staphylococcus aureus.

A critical challenge to realize ultra-high sensitivity with optical fiber interferometers for label free biosensing is to achieve high quality factors (Q-factor) in liquid. In this work a high Q-factor of 105, which significantly improves the detection resolution is described based on a structure of single mode -core-only -single mode fiber (SCS) with its multimode (or Mach-Zehnder) interference effect as a filter that is integrated into an erbium-doped fiber laser (EDFL) system for excitation. In the case study, the section of core-only fiber is functionalized with porcine immunoglobulin G (IgG) antibodies, which could selectively bind to bacterial pathogen of Staphylococcus aureus (S. aureus). The developed microfiber-based biosensing platform called SCS-based EDFL biosensors can effectively detect concentrations of S. aureus from 10 to 105 CFU/mL, with a responsivity of 0.426 nm wavelength shift in the measured spectrum for S. aureus concentration of 10 CFU/mL. The limit of detection (LoD) is estimated as 7.3 CFU/mL based on the measurement of S. aureus with minimum concentration of 10 CFU/mL. In addition, when a lower concentration of 1 CFU/mL is applied to the biosensor, a wavelength shift of 0.12 nm is observed in 10% of samples (1/10), indicating actual LoD of 1 CFU/mL for the proposed biosensor. Attributed to its good sensitivity, stability, reproducibility and specificity, the proposed EDFL based biosensing platform has great potentials for diagnostics.

Simulation of a Temperature-Compensated Voltage Sensor Based on Photonic Crystal Fiber Infiltrated with Liquid Crystal and Ethanol.

A simulated design for a temperature-compensated voltage sensor based on photonic crystal fiber (PCF) infiltrated with liquid crystal and ethanol is presented in this paper. The holes distributed across the transverse section of the PCF provide two channels for mode coupling between the liquid crystal or ethanol and the fiber core. The couplings are both calculated accurately and explored theoretically using the finite element method (FEM). The influence of voltage on the alignment of the liquid crystal molecules and confinement loss of the fiber mode are studied. Liquid crystal molecules rotate which changes its properties as the voltage changes. As the characteristics of the liquid crystal will be affected by temperature, therefore, we further fill using ethanol, which is merely sensitive to temperature, into one hole of the PCF to realize temperature compensation. The simulated results show that the sensitivity is up to 1.29977 nm/V with the temperature of 25 °C when the voltage ranges from 365 to 565 V. The standard deviation of the wavelength difference is less than 2 nm within the temperature adjustment from 25 to 50 °C for temperature compensation. The impacts of the construction parameters of the PCF on sensing performances of this voltage sensor are also analyzed in this paper.

An extended Stokes-Einstein model for condensed ionic water structures with topological complexity.

'What is the structure of water?' This has been a perplexing question for a long time and water structure with various phases is a great topic of research interest. Topological complexity generally occurs because hydrophilic ions strongly influence the size and shape of condensed water structures owing to their kosmotropic and chaotropic transitions. In this study, an extended Stokes-Einstein model incorporating Flory-Huggins free energy equation is proposed to describe the constitutive relationship between dynamic diffusion and condensed water structure with a topological complexity. The newly developed model provides a geometrical strategy of end-to-end distance and explores the constitutive relationship between condensed ionic water structures and their dynamic diffusion behaviors. A free-energy function is then formulated to study thermodynamics in electrolyte aqueous solution, in which the condensed ionic water structures undergo topologically complex changes. Finally, effectiveness of the proposed model is verified using both molecular dynamics simulations and experimental results reported in literature.

Cobalt-molybdenum selenide double-shelled hollow nanocages derived from metal-organic frameworks as high performance electrodes for hybrid supercapacitor.

In this paper, we developed a sequential chemical etching and selenization processes to synthesize Co-MoSex double-shelled hollow nanocages (CMS-DSHNCs) as high performance electrode materials for supercapacitor applications. Co-MoOx yolk-shelled hollow nanocages were firstly synthesized using a solvothermal process through facile ion-exchange reactions between zeolitic imidazolate framework-67 (ZIF-67) and MoO42- ions. By applying a solvothermal temperature of 160 °C in the presence of SeO32- and subsequently annealing strategy, CMS-DSHNCs were successfully synthesized with a yolk-shell hierarchically hollow and porous morphology of mixed metal selenides. The CMS-DSHNCs exhibit superior electrochemical properties as electrode materials for supercapacitor: e.g., a specific capacity of 1029.8C g-1 at 2 A g-1 (3.089C cm-2 at 6 mA cm-2), a rate capability of âˆ¼ 76.14%, a capacity retention at 50 A g-1, and a good cycle stability (95.2% capacity retention over 8000 cycles). A hybrid supercapacitor was constructed using the CMS-DSHNCs as the cathode and activated carbon (AC) as the anode in a solution of 3 M KOH, and achieved a high specific energy of 45 Wh kg-1, and a specific power up to 2222 W kg-1 with a good cycling stability of 94% after 8000 cycles.

Phase transition of supercooled water confined in cooperative two-state domain.

The question of 'what is the structure of water?' has been regarded as one of the major scientific conundrums in condensed-matter physics due to the complex phase behavior and condensed structure of supercooled water. Great effort has been made so far using both theoretical analysis based on various mathematical models and computer simulations such as molecular dynamics and first-principle. However, these theoretical and simulation studies often do not have strong evidences of condensed-matter physics to support. In this study, a cooperative domain model is formulated to describe the dynamic phase transition of supercooled water between supercooled water and amorphous ice, both of which are composed of low- and high-density liquid water. Free volume theory is initially employed to identify the working principle of dynamic phase transition and its connection to glass transition in the supercooled water. Then a cooperative two-state model is developed to characterize the dynamic anomalies of supercooled water, including density, viscosity and self-diffusion coefficient. Finally, the proposed model is verified using the experimental results reported in literature.

Untangling the mechanics of entanglements in slide-ring gels towards both super-deformability and toughness.

Entanglement plays a critical role in determining the dynamic properties of polymer systems, e.g., resulting in slip links and pulley effects for achieving large deformation and high strength. Although it has been studied for decades, the mechanics of entanglements for stiffness-toughness conflict is not well understood. In this study, topological knot theory incorporating an extended tube model is proposed to understand the entanglements in a slide-ring (SR) gel, which slips over a long distance to achieve large deformation and high toughness via the pulley effect. Based on topological knot theory, the sliding behavior and pulley effect of entanglements among molecular chains and cross-linked rings are thoroughly investigated. Based on rubber elasticity theory, a free-energy function is formulated to describe mechanical toughening and slipping of topological knots, while the SR gel retains the same binding energy. Finally, the effectiveness of the proposed model is verified using both finite element analysis and experimental results reported in the literature.

Node formation mechanisms in acoustofluidic capillary bridges.

Using acoustofluidic channels formed by capillary bridges two models are developed to describe nodes formed by leaky and by evanescent waves. The liquid channel held between a microscope slide (waveguide) and a strip of polystyrene film (fluid guide) avoids solid-sidewall interactions. With this simplification, our experimental and numerical study showed that waves emitted from a single plane surface, interfere and form the nodes without any resonance in the fluid. Both models pay particular attention to tensor elements normal to the solid-liquid interfaces they find that; initially nodes form in the solid and the node pattern is replicated by waves emitted into the fluid from antinodes in the stress. At fluids depths near half an acoustic wavelength, most nodes are formed by leaky waves. In the glass, water-loading reduces node-node separation and forms an overlay type waveguide which aligns the nodes predominantly along the channel. One new practical insight is that node separation can be controlled by water depth. At 0.2 mm water depths (which are smaller than a » wavelength) nodes form from evanescent waves. Here a suspension of yeast cells formed a pattern of small dot-like clumps of cells on the surface of the polystyrene film. We found the same pattern in sound intensity normal, and close, to the water-polystyrene interface. The capillary bridge channel developed for this study is simple, low-cost, and could be developed for filtration, separation, or patterning of biological species in rapid immuno-sensing applications.

Acousto-Pi: An Opto-Acoustofluidic System Using Surface Acoustic Waves Controlled With Open-Source Electronics for Integrated In-Field Diagnostics.

Surface acoustic wave (SAW) devices are increasingly applied in life sciences, biology, and point-of-care applications due to their combined acoustofluidic sensing and actuating properties. Despite the advances in this field, there remain significant gaps in interfacing hardware and control strategies to facilitate system integration with high performance and low cost. In this work, we present a versatile and digitally controlled acoustofluidic platform by demonstrating key functions for biological assays such as droplet transportation and mixing using a closed-loop feedback control with image recognition. Moreover, we integrate optical detection by demonstrating in situ fluorescence sensing capabilities with a standard camera and digital filters, bypassing the need for expensive and complex optical setups. The Acousto-Pi setup is based on open-source Raspberry Pi hardware and 3-D printed housing, and the SAW devices are fabricated with piezoelectric thin films on a metallic substrate. The platform enables the control of droplet position and speed for sample processing (mixing and dilution of samples), as well as the control of temperature based on acousto-heating, offering embedded processing capability. It can be operated remotely while recording the measurements in cloud databases toward integrated in-field diagnostic applications such as disease outbreak control, mass healthcare screening, and food safety.

Simulations of surface acoustic wave interactions on a sessile droplet using a three-dimensional multiphase lattice Boltzmann model.

This study reports the development of a three-dimensional numerical model for acoustic interactions with a microscale sessile droplet under surface acoustic wave (SAW) excitation using the lattice Boltzmann method (LBM). We first validate the model before SAW interactions are added. The results demonstrate good agreement with the analytical results for thermodynamic consistency, Laplace law, static contact angle on a flat surface, and droplet oscillation. We then investigate SAW interactions on the droplet, with resonant frequencies ranging 61.7-250.1 MHz. According to our findings, an increase in wave amplitude elicits an increase in streaming velocity inside the droplet, causing internal mixing, and further increase in wave amplitude leads to pumping and jetting. The boundaries of wave amplitude at various resonant frequencies are predicted for mixing, pumping, and jetting modes. The modeling predictions on the roles of forces (SAW, interfacial tension, inertia, and viscosity) on the dynamics of mixing, pumping, and jetting of a droplet are in good agreement with observations and experimental data. The model is further applied to investigate the effects of SAW substrate surface wettability, viscosity ratio, and interfacial tension on SAW actuation onto the droplet. This work demonstrates the capability of the LBM in the investigation of acoustic wave interactions between SAW and a liquid medium.

Anchoring-mediated topology signature of self-assembled elastomers undergoing mechanochromic coupling/decoupling.

Soft elastomers with their ability to integrate strain-adaptive stiffening and coloration have recently received significant research attention for application in artificial muscle and active camouflage. However, there is a lack of theoretical understanding of their complex molecular dynamics and mechanochromic coupling/decoupling. In this study, a topological dynamics model is proposed to understand the anchoring-mediated topology signature of self-assembled elastomers. Based on the constrained molecular junction model, a free-energy function is firstly formulated to describe the working principles of strain-adaptive stiffening and coloration in the self-assembled elastomer. A coupled ternary "rock-paper-scissors" model is proposed to describe the topological dynamics of self-assembly, mechanochromic coupling and mechanoresponsive stiffening of the self-assembled elastomers, in which there are three fractal geometry components in the topology network. Finally, the proposed models are verified using the experimental results reported in the literature. This study provides a fundamental approach to understand the working mechanism and topological dynamics in the self-assembled elastomers, with molecularly encoded stiffening and coloration.

Engineering inclined orientations of piezoelectric films for integrated acoustofluidics and lab-on-a-chip operated in liquid environments.

Different acoustic wave modes are required for effective implementation of biosensing and liquid actuation functions in an acoustic wave-based lab-on-a-chip. For efficient sensing in liquids, shear waves (either a thickness-shear bulk wave or a shear-horizontal surface acoustic wave) can achieve a high sensitivity, without significant loss of acoustic wave energy. On the other hand, longitudinal bulk waves or out-of-plane displacement waves (such as Rayleigh waves) enable efficient sampling functions and liquid manipulation. However, there are significant challenges in developing a lab-on-a-chip to efficiently generate multiple wave modes and perform both these functions on a single piezoelectric substrate, especially when a single crystalline orientation is available. This paper highlights the latest progress in the theories and techniques to deliver both sensing and microfluidic manipulation functions using engineered inclined-angled piezoelectric films, allowing for the simultaneous generation of longitudinal (or Rayleigh) and thickness-shear bulk (or shear-horizontal surface acoustic) waves. Challenges and theoretical constraints for generating various wave modes in the inclined films and techniques to efficiently produce inclined columnar and inclined crystalline piezoelectric films using sputtering deposition methods are presented. Applications of different wave modes in the inclined film-based lab-on-chips with multiple sensing and acoustofluidic functions are also discussed.

Flexible and Integrated Sensing Platform of Acoustic Waves and Metamaterials based on Polyimide-Coated Woven Carbon Fibers.

Versatile, in situ sensing and continuous monitoring capabilities are critically needed, but challenging, for components made of solid woven carbon fibers in aerospace, electronics, and medical applications. In this work, we proposed a unique concept of integrated sensing technology on woven carbon fibers through integration of thin-film surface acoustic wave (SAW) technology and electromagnetic metamaterials, with capabilities of noninvasive, in situ, and continuous monitoring of environmental parameters and biomolecules wirelessly. First, we fabricated composite materials using a three-layer composite design, in which the woven carbon fiber cloth was first coated with a polyimide (PI) layer followed by a layer of ZnO film. Integrated SAW and metamaterials devices were then fabricated on this composite structure. The temperature of the functional area of the device could be controlled precisely using the SAW devices, which could provide a proper incubation environment for biosampling processes. As an ultraviolet light sensor, the SAW device could achieve a good sensitivity of 56.86 ppm/(mW/cm2). On the same integrated platform, an electromagnetic resonator based on the metamaterials was demonstrated to work as a glucose concentration monitor with a sensitivity of 0.34 MHz/(mg/dL).