Highly Reliable 3D Channel Memory and Its Application in a Neuromorphic Sensory System for Hand Gesture Recognition.

Brain-inspired neuromorphic computing systems, based on a crossbar array of two-terminal multilevel resistive random-access memory (RRAM), have attracted attention as promising technologies for processing large amounts of unstructured data. However, the low reliability and inferior conductance tunability of RRAM, caused by uncontrollable metal filament formation in the uneven switching medium, result in lower accuracy compared to the software neural network (SW-NN). In this work, we present a highly reliable CoOx-based multilevel RRAM with an optimized crystal size and density in the switching medium, providing a three-dimensional (3D) grain boundary (GB) network. This design enhances the reliability of the RRAM by improving the cycle-to-cycle endurance and device-to-device stability of the I-V characteristics with minimal variation. Furthermore, the designed 3D GB-channel RRAM (3D GB-RRAM) exhibits excellent conductance tunability, demonstrating high symmetricity (624), low nonlinearity (ßLTP/ßLTD ∼ 0.20/0.39), and a large dynamic range (Gmax/Gmin ∼ 31.1). The cyclic stability of long-term potentiation and depression also exceeds 100 cycles (105 voltage pulses), and the relative standard deviation of Gmax/Gmin is only 2.9%. Leveraging these superior reliability and performance attributes, we propose a neuromorphic sensory system for finger motion tracking and hand gesture recognition as a potential elemental technology for the metaverse. This system consists of a stretchable double-layered photoacoustic strain sensor and a crossbar array neural network. We perform training and recognition tasks on ultrasonic patterns associated with finger motion and hand gestures, attaining a recognition accuracy of 97.9% and 97.4%, comparable to that of SW-NN (99.8% and 98.7%).

Dielectric light-trapping nanostructure for enhanced light absorption in organic solar cells.

Dielectric scatterers where Mie resonances can be excited in both electric and magnetic modes have emerged as a promising candidate for efficient light trapping (LT) in thin-film solar cells. We present that light absorption in organic solar cells (OSCs) can be significantly enhanced by a front-sided incorporation of a core-shell nanostructure consisting of a high-refractive-index dielectric nanosphere array conformally coated with a low-refractive-index dielectric layer. Strong forward light scattering of the all-dielectric LT structure enables the absorption in an organic semiconductor to be remarkably boosted over a broad range of wavelengths, which is attributed to interference of a simultaneous excitation of the electric and magnetic dipole resonant modes. The OSC with the LT structure shows the short-circuit current density (Jsc) of 28.23 mA/cm2, which is 10% higher than that of a flat OSC. We also explore how the LT structure affects scattering cross-sections, spectral multipole resonances, and far-field radiation patterns. The approach described in this work could offer the possibility for the improvement of characteristic performances of various applications, such as other thin-film solar cells, photodiodes, light-emitting diodes, and absorbers.

Light-enhanced molecular polarity enabling multispectral color-cognitive memristor for neuromorphic visual system.

An optoelectronic synapse having a multispectral color-discriminating ability is an essential prerequisite to emulate the human retina for realizing a neuromorphic visual system. Several studies based on the three-terminal transistor architecture have shown its feasibility; however, its implementation with a two-terminal memristor architecture, advantageous to achieving high integration density as a simple crossbar array for an ultra-high-resolution vision chip, remains a challenge. Furthermore, regardless of the architecture, it requires specific material combinations to exhibit the photo-synaptic functionalities, and thus its integration into various systems is limited. Here, we suggest an approach that can universally introduce a color-discriminating synaptic functionality into a two-terminal memristor irrespective of the kinds of switching medium. This is possible by simply introducing the molecular interlayer with long-lasting photo-enhanced dipoles that can adjust the resistance of the memristor at the light-irradiation. We also propose the molecular design principle that can afford this feature. The optoelectronic synapse array having a color-discriminating functionality is confirmed to improve the inference accuracy of the convolutional neural network for the colorful image recognition tasks through a visual pre-processing. Additionally, the wavelength-dependent optoelectronic synapse can also be leveraged in the design of a light-programmable reservoir computing system.

Micro-ultrasonic Assessment of Early Stage Clot Formation and Whole Blood Coagulation Using an All-Optical Ultrasound Transducer and Adaptive Signal Processing Algorithm.

Abnormal formation of solid thrombus inside a blood vessel can cause thrombotic morbidity and mortality. This necessitates early stage diagnosis, which requires quantitative assessment with a small volume, for effective therapy with low risk to unwanted development of various diseases. We propose a micro-ultrasonic diagnosis using an all-optical ultrasound-based spectral sensing (AOUSS) technique for sensitive and quantitative characterization of early stage and whole blood coagulation. The AOUSS technique detects and analyzes minute viscoelastic variations of blood at a micro-ultrasonic spot (<100 µm) defined by laser-generated focused ultrasound (LGFU). This utilizes (1) a uniquely designed optical transducer configuration for frequency-spectral matching and wideband operation (6 dB widths: 7-32 MHz and d.c. ∼ 46 MHz, respectively) and (2) an empirical mode decomposition (EMD)-based signal process particularly adapted to nonstationary LGFU signals backscattered from the spot. An EMD-derived spectral analysis enables one to assess viscoelastic variations during the initiation of fibrin formation, which occurs at a very early stage of blood coagulation (1 min) with high sensitivity (frequency transition per storage modulus increment = 8.81 MHz/MPa). Our results exhibit strong agreement with those obtained by conventional rheometry (Pearson's R > 0.95), which are also confirmed by optical microscopy. The micro-ultrasonic and high-sensitivity detection of AOUSS poses a potential clinical significance, serving as a screening modality to diagnose early stage clot formation (e.g., as an indicator for hypercoagulation of blood) and stages of blood-to-clot transition to check a potential risk for development into thrombotic diseases.

Manipulation of resonance orders and absorbing materials for structural colors in transmission with improved color purity.

We present an improved color purity of additive transmissive structural color filters by controlling a resonance order and by inserting a highly absorbing material. The proposed structure consists of a single metal sandwiched by two transparent dielectric media serving as a cavity to minimize the ohmic loss in the metal mirrors, which is distinctly different from a conventional Fabry-Perot (FP) cavity that is in general designed to have two metal mirrors. Low reflections at an air-dielectric interface cause a quality-factor of a resonance to be reduced, causing a degraded color purity, which can be improved by employing a 1st order resonance that exhibits a narrower bandwidth than a fundamental FP resonant mode (0th order). For a red color with the improved purity, introducing an ultrathin absorbing layer in the middle of a top cavity enables the 1st resonance to be trivially influenced while selectively suppressing a 2nd order resonance appearing at the shorter wavelength region. Moreover, angle-insensitive performances up to 60° are attained by utilizing a cavity material with high index of refraction. Besides, the fabrication of the structural coloring devices involves a few deposition steps, thus rendering the approach suitable for applications over the large area. The described concept could be applied to diverse applications, such as colored solar panels, sensors, imaging devices, and decorations.

Light absorption enhancement in ultrathin perovskite solar cells using light scattering of high-index dielectric nanospheres.

Arrays of high-index dielectric nanoparticles supporting both electrical and magnetic resonances have gained increasing attention for their excellent light-trapping (LT) effects, thus greatly improving the performance of ultrathin solar cells. This work explores front-located, high-index dielectric subwavelength nanosphere arrays as an efficient and broadband LT structure patterned on top of an ultrathin perovskite solar cell (PSC) for a greatly enhanced absorption. Combined strong light scattering and anti-reflection properties achieved by optimized geometrical parameters of the LT structure lead to a broadband absorption enhancement in the ultrathin thickness of a photoactive layer (100 nm) yielding the short-circuit current density (Jsc) of 18.7 mA/cm2, which is 31.7% higher than that of a planar counterpart. Moreover, effects of the LT structure on far-field radiation patterns, scattering cross-sections, multipoles' contributions, and asymmetry parameters along with the incidence angle and polarization dependence are investigated. The present strategy could be applied to diverse applications, such as other ultrathin or semitransparent solar cells, absorbers and photodetectors.

Experimental Demonstration of a Stacked Hybrid Optoacoustic-Piezoelectric Transducer for Localized Heating and Enhanced Cavitation.

Laser-generated focused ultrasound (LGFU) is an emerging modality for cavitation-based therapy. However, focal pressure amplitudes by LGFU alone to achieve pulsed cavitation are often lacking as a treatment depth increases. This requires a higher pressure from a transmitter surface and more laser energies that even approach to a damage threshold of transmitter. To mitigate the requirement for LGFU-induced cavitation, we propose LGFU configurations with a locally heated focal zone using an additional high-intensity focused ultrasound (HIFU) transmitter. After confirming heat-induced cavitation enhancement using two separate transmitters, we then developed a stacked hybrid optoacoustic-piezoelectric transmitter, which is a unique configuration made by coating an optoacoustic layer directly onto a piezoelectric substrate. This shared curvature design has great practical advantage without requiring the complex alignment of two focal zones. Moreover, this enabled the amplification of cavitation bubble density by 18.5-fold compared to the LGFU operation alone. Finally, the feasibility of tissue fragmentation was confirmed through a tissue-mimicking gel, using the combination of LGFU and HIFU (not via a stacked structure). We expect that the stacked transmitter can be effectively used for stronger and faster tissue fragmentation than the LGFU transmitter alone.

Variable-focus optoacoustic lens with wide dynamic range and long focal length by using a flexible polymer nano-composite membrane.

We demonstrate a variable-focus optoacoustic lens (VFOL) by pneumatically controlling a flexible polymer nano-composite membrane, which can produce laser-generated focused ultrasound (LGFU) with a high peak amplitude (>30 MPa) and a tight focal dimension (several hundred µm) over a wide dynamic range of focus variation (>20 mm) together with a long focal length up to 60 mm, each of which is widest and longest among optoacoustic lenses developed so far. Two different designs in lens dimension have been fabricated and characterized: VFOL-L with a 40-mm diameter and VFOL-S with 10 mm. VFOL-L exhibits a wide dynamic range of focal length variation from 38.52 to 60.39 mm with a center frequency near ~ 10 MHz, which is proper for practical long-range applications with several-cm depth. In comparison, VFOL-S covers a focal variation range from 6.75 to 11.1 mm with ~ 14 MHz, producing a relatively higher-pressure amplitude, which allows the inception of acoustic cavitation at an impedance-mismatched boundary. The nano-composite membrane of VFOL is actuated from a planar to deeply curved shape by externally injecting liquid into the VFOL, resulting in a focal gain up to 255 and a positive peak pressure of > 30 MPa in the VFOL-L case. The minimum-geometrical f-number as low as 0.963 is achieved at the shortest focal length (38.52 mm) with 6-dB lateral and axial spot dimensions of 304 µm and 2.86 mm, respectively. We expect that the proposed VFOL-based LGFU with a high peak pressure, a wide dynamic axial range, and a tight focal dimension are suitably applied for depth-dependent characterization of tissues and shockwave treatment, taking advantages of optoacoustic pulses as input with inherent broadband high-frequency characteristics.

Angular selection of transmitted light and enhanced spontaneous emission in grating-coupled hyperbolic metamaterials.

We propose dielectric grating-coupled hyperbolic metamaterials as a functional device that shows angular selection of transmitted light and enhanced radiative emission rate. We numerically demonstrate that the surface plasmon polaritons in the hyperbolic metamaterials can be effectively outcoupled to the surrounding space by using gratings and facilitate control of the light transmission in the visible frequency. We confirm that the high density of states and the effect of outcoupled plasmonic modes of the proposed structure lead to the increase of Purcell factor and radiative emission. This work will provide multifunctionalities in sensing and imaging systems that use hyperbolic metamaterials.

Laser-generated focused ultrasound transducer using a perforated photoacoustic lens for tissue characterization.

We demonstrate a laser-generated focused ultrasound (LGFU) transducer using a perforated-photoacoustic (PA) lens and a piezoelectric probe hydrophone suitable for high-frequency ultrasound tissue characterization. The perforated-PA lens employed a centrally located hydrophone to achieve a maximum directional response at 0° from the axial direction of the lens. Under pulsed laser irradiation, the lens produced LGFU pulses with a frequency bandwidth of 6-30 MHz and high-peak pressure amplitudes of up to 46.5 MPa at a 70-µm lateral focal width. Since the hydrophone capable of covering the transmitter frequency range (∼20 MHz) was integrated with the lens, this hybrid transducer differentiated tissue elasticity by generating and detecting high-frequency ultrasound signals. Backscattered (BS) waves from excised tissues (bone, skin, muscle, and fat) were measured and also confirmed by laser-flash shadowgraphy. We characterized the LGFU-BS signals in terms of mean frequency and spectral energy in the frequency domain, enabling to clearly differentiate tissue types. Tissue characterization was also performed with respect to the LGFU penetration depth (from the surface, 1-, and 2-mm depth). Despite acoustic attenuation over the penetration depth, LGFU-BS characterization shows consistent results that can differentiate the elastic properties of tissues. We expect that the proposed transducer can be utilized for other tissue types and also for non-destructive evaluation based on the elasticity of unknown materials.

Defect-Passivating Organic/Inorganic Bicomponent Hole-Transport Layer for High Efficiency Metal-Halide Perovskite Device.

In this work, we introduce a bicomponent hole-transport layer, composed of inorganic NiOx and a donor-acceptor-donor (D-A-D)-structured organic small molecule, for p-i-n planar perovskite photovoltaic (PV) cells. The newly designed D-A-D organic hole-transporting material (HTM), (4',4‴-(1,3,4-oxadiazole-2,5-diyl)bis(N,N-bis(4-methoxyphenyl)-[1,1'-biphenyl]-4-amine)), is shown to be an efficient HTM without a dopant, and methoxy functional units, further introduced to the molecules, are confirmed to be beneficial to passivate the defects in the perovskite, which improves the crystallinity of perovskite and suppresses the nonradiative recombination in the devices, consequently enhancing the performances of PV cells (over 20% efficiency from p-i-n architecture). Furthermore, the decreased defect sites along with the UV-blocking property of the HTM in p-i-n architecture are advantageous in improving the stability of the PV devices.

Author Correction: Light Intensity-dependent Variation in Defect Contributions to Charge Transport and Recombination in a Planar MAPbI3 Perovskite Solar Cell.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Light Intensity-dependent Variation in Defect Contributions to Charge Transport and Recombination in a Planar MAPbI3 Perovskite Solar Cell.

We investigated operation of a planar MAPbI3 solar cell with respect to intensity variation ranging from 0.01 to 1 sun. Measured J-V curves consisted of space-charge-limited currents (SCLC) in a drift-dominant range and diode-like currents in a diffusion-dominant range. The variation of power-law exponent of SCLC showed that charge trapping by defects diminished as intensity increased, and that drift currents became eventually almost ohmic. Diode-like currents were analysed using a modified Shockley-equation model, the validity of which was confirmed by comparing measured and estimated open-circuit voltages. Intensity dependence of ideality factor led us to the conclusion that there were two other types of defects that contributed mostly as recombination centers. At low intensities, monomolecular recombination occurred due to one of these defects in addition to bimolecular recombination to result in the ideality factor of ~1.7. However, at high intensities, another type of defect not only took over monomolecular recombination, but also dominated bimolecular recombination to result in the ideality factor of ~2.0. These ideality-factor values were consistent with those representing the intensity dependence of loss-current ratio estimated by using a constant internal-quantum-efficiency approximation. The presence of multiple types of defects was corroborated by findings from equivalent-circuit analysis of impedance spectra.

Tailored Nanopatterning by Controlled Continuous Nanoinscribing with Tunable Shape, Depth, and Dimension.

We present that the tailored nanopatterning with tunable shape, depth, and dimension for diverse application-specific designs can be realized by utilizing controlled dynamic nanoinscribing (DNI), which can generate bur-free plastic deformation on various flexible substrates via continuous mechanical inscription of a small sliced edge of a nanopatterned mold in a compact and vacuum-free system. Systematic controlling of prime DNI processing parameters including inscribing force, temperature, and substrate feed rate can determine the nanopattern depths and their specific profiles from rounded to angular shapes as a summation of the force-driven plastic deformation and heat-driven thermal deformation. More complex nanopatterns with gradient depths and/or multidimensional profiles can also be readily created by modulating the horizontal mold edge alignment and/or combining sequential DNI strokes, which otherwise demand laborious and costly procedures. Many practical user-specific applications may benefit from this study by tailor-making the desired nanopattern structures within desired areas, including precision machine and optics components, transparent electronics and photonics, flexible sensors, and reattachable and wearable devices. We demonstrate one vivid example in which the light diffusion direction of a light-emitting diode can be tuned by application of specifically designed DNI nanopatterns.

Flexible High-Color-Purity Structural Color Filters Based on a Higher-Order Optical Resonance Suppression.

We present flexible transmissive structural color filters with high-color-purity based on a higher-order resonance suppression by inserting an ultrathin absorbing layer in the middle of a cavity. A 3rd order Fabry-Pérot (F-P) resonance, which exhibits a narrower bandwidth than a fundamental F-P resonance, is used to produce transmissive colors with an improved color purity. The thin absorbing layer is properly placed at a center of the cavity to highly suppress only a 5th order F-P resonance appearing at a short wavelength range while not affecting the 3rd order F-P resonance for color generation, thus being able to attain the high-color-purity transmissive colors without reducing a transmission efficiency. In addition, angle-insensitive properties are achieved by compensating a net phase shift with a dielectric overlay and using a material with a high refractive index for the cavity medium. Moreover, the transmissive colors on a flexible substrate are demonstrated, presenting that changes in both the resonance wavelength and the transmission efficiency are nearly negligible when the color filters are bent with a bending radius of 5 mm and over 3000 times bending tests. The described approach could pave the way for various applications, such as colored displays, decorative solar panels, and image sensors.

Bifacial Passivation of Organic Hole Transport Interlayer for NiO x -Based p-i-n Perovskite Solar Cells.

Methoxy-functionalized triphenylamine-imidazole derivatives that can simultaneously work as hole transport materials (HTMs) and interface-modifiers are designed for high-performance and stable perovskite solar cells (PSCs). Satisfying the fundamental electrical and optical properties as HTMs of p-i-n planar PSCs, their energy levels can be further tuned by the number of methoxy units for better alignment with those of perovskite, leading to efficient hole extraction. Moreover, when they are introduced between perovskite photoabsorber and low-temperature solution-processed NiO x interlayer, widely featured as an inorganic HTM but known to be vulnerable to interfacial defect generation and poor contact formation with perovskite, nitrogen and oxygen atoms in those organic molecules are found to work as Lewis bases that can passivate undercoordinated ion-induced defects in the perovskite and NiO x layers inducing carrier recombination, and the improved interfaces are also beneficial to enhance the crystallinity of perovskite. The formation of Lewis adducts is directly observed by IR, Raman, and X-ray photoelectron spectroscopy, and improved charge extraction and reduced recombination kinetics are confirmed by time-resolved photoluminescence and transient photovoltage experiments. Moreover, UV-blocking ability of the organic HTMs, the ameliorated interfacial property, and the improved crystallinity of perovskite significantly enhance the stability of PSCs under constant UV illumination in air without encapsulation.

Design of Polarization-Independent and Wide-Angle Broadband Absorbers for Highly Efficient Reflective Structural Color Filters.

We propose a design of angle-insensitive and polarization-independent reflective color filters with high efficiency (>80%) based on broad resonance in a Fabry⁻Pérot cavity where asymmetric metal-dielectric-metal planar structures are employed. Broadband absorption properties allow the resonance in the visible range to remain nearly constant over a broad range of incident angles of up to 40° for both s- and p-polarizations. Effects of the angles of incidence and polarization state of incident light on the purity of the resulting colors are examined on the CIE 1931 chromaticity diagram. In addition, higher-order resonances of the proposed color filters and their electric field distributions are investigated for improved color purity. Lastly, the spectral properties of the proposed structures with different metallic layers are studied. The simple strategy described in this work could be adopted in a variety of research areas, such as color decoration devices, microscopy, and colorimetric sensors.

Management of transition dipoles in organic hole-transporting materials under solar irradiation for perovskite solar cells.

In organic hole-transporting material (HTM)-based p-i-n planar perovskite solar cells, which have simple and low-temperature processibility feasible to flexible devices, the incident light has to pass through the HTM before reaching the perovskite layer. Therefore, photo-excited state of organic HTM could become important during the solar cell operation, but this feature has not usually been considered for the HTM design. Here, we prove that enhancing their property at their photo-excited states, especially their transition dipole moments, can be a methodology to develop high efficiency p-i-n perovskite solar cells. The organic HTMs are designed to have high transition dipole moments at the excited states and simultaneously to preserve those property during the solar cell operation by their extended lifetimes through the excited-state intramolecular proton transfer process, consequently reducing the charge recombination and improving extraction properties of devices. Their UV-filtering ability is also beneficial to enhance the photostability of devices.

Photoacoustic Energy Sensor for Nanosecond Optical Pulse Measurement.

We demonstrate a photoacoustic sensor capable of measuring high-energy nanosecond optical pulses in terms of temporal width and energy fluence per pulse. This was achieved by using a hybrid combination of a carbon nanotube-polydimethylsiloxane (CNT-PDMS)-based photoacoustic transmitter (i.e., light-to-sound converter) and a piezoelectric receiver (i.e., sound detector). In this photoacoustic energy sensor (PES), input pulsed optical energy is heavily absorbed by the CNT-PDMS composite film and then efficiently converted into an ultrasonic output. The output ultrasonic pulse is then measured and analyzed to retrieve the input optical characteristics. We quantitatively compared the PES performance with that of a commercial thermal energy meter. Due to the efficient energy transduction and sensing mechanism of the hybrid structure, the minimum-measurable pulsed optical energy was significantly lowered, ~157 nJ/cm², corresponding to 1/760 of the reference pyroelectric detector. Moreover, despite the limited acoustic frequency bandwidth of the piezoelectric receiver, laser pulse widths over a range of 6⁻130 ns could be measured with a linear relationship to the ultrasound pulse width of 22⁻153 ns. As CNT has a wide electromagnetic absorption spectrum, the proposed pulsed sensor system can be extensively applied to high-energy pulse measurement over visible through terahertz spectral ranges.

Polarization-sensitive tunable absorber in visible and near-infrared regimes.

A broadband tunable absorber is designed and fabricated. The tunable absorber is comprised of a dielectric-metal-dielectric multilayer and plasmonic grating. A large size of tunable absorber device is fabricated by nano-imprinting method. The experimental results show that over 90% absorption can be achieved within visible and near-infrared regimes. Moreover, the high absorption can be controlled by changing the polarization of incident light. This polarization-sensitive tunable absorber can have practical applications such as high-efficiency polarization detectors and transmissive polarizer.