Defect Engineering of Metal Halide Perovskite Nanocrystals via Spontaneous Diffusion of Ag Nanocrystals.

Perovskite nanocrystals (NCs) have emerged as a promising building block for the fabrication of optic-/optoelectronic-/electronic devices owing to their superior characteristics, such as high absorption coefficient, rapid ion mobilities, and tunable energy levels. However, their low structural stability and poor surface passivation have restricted their application to next-generation devices. Herein, a drug delivery system (DDS)-inspired post-treatment strategy is reported for improving their structural stability by doping of Ag into CsPbBr3 (CPB) perovskite NCs; delivery to damaged sites can promote their structural recovery slowly and uniformly, averting the permanent loss of their intrinsic characteristics. Ag NCs are designed through surface-chemistry tuning and structural engineering to enable their circulation in CPB NC dispersions, followed by their delivery to the CPB NC surface, defect-site recovery, and defect prevention. The perovskite-structure healing process through the DDS-type process (with Ag NCs as the drug) is analyzed by a combination of theoretical calculations (with density functional theory) and experimental analyses. The proposed DDS-inspired healing strategy significantly enhances the optical properties and stability of perovskite NCs, enabling the fabrication of white light-emitting diodes.

Highly Conductive and Sensitive Wearable Strain Sensors with Metal/Nanoparticle Double Layer for Noninterference Voice Detection.

Human voice recognition via skin-attachable devices has significant potential for gathering important physiological information from acoustic data without background noise interference. In this study, a highly sensitive and conductive wearable crack-based strain sensor was developed for voice-recognition systems. The sensor was fabricated using a double-layer structure of Ag nanoparticles (NPs) and Ag metal on a biocompatible polydimethylsiloxane substrate. The top metal layer acts as a conducting active layer, whereas the bottom Ag NP layer induces channel cracks in the upper layer, effectively hindering current flow. Subsequently, the double-layer film exhibits a low electrical resistance value (<5 × 10-5 Ω cm), ultrahigh sensitivity (gauge factor = 1870), and a fast response/recovery time (252/168 µs). A sound wave was detected at a high frequency of 15 kHz with a signal-to-noise ratio (SNR) over 40 dB. The sensor exhibited excellent anti-interference characteristics and effectively differentiated between different voice qualities (modal, pressed, and breathy), with a systematic analysis revealing successful detection of the laryngeal state and glottal source. This ultrasensitive wearable sensor has potential applications in various physiological signal measurement methods, personalized healthcare systems, and ubiquitous computing.

Ink-lithographic fabrication of silver-nanocrystal-based multiaxial strain gauge sensors through the coffee-ring effect for voice recognition applications.

Human voice recognition techniques have remarkable potential for clinical applications because information from acoustic signals can reflect human body conditions. This paper reports the fabrication of Ag nanocrystal (NC)-based multiaxial wearable strain gauge sensors by ink-lithography for voice recognition systems. Benefiting from the one-step-device-fabrication strategy of ink-lithography, which can yield Ag NC patterns with specific dimensions and endow physical properties, the Ag NC-based multiaxial strain sensors can be fabricated on an ultrathin substrate (~ 6 µm). Additionally, the coffee-ring effect can be induced onto the Ag NC patterns to realize high sensitivity and angle dependence (gauge factors [Formula: see text] = 11.7 ± 1.2 and [Formula: see text] = 105.5 ± 20.1); moreover, the voice onset time for voice recognition can be detected by the sensors. These features assist in distinguishing between voiced and voiceless plosive contrasts via measurements of contact-based voice onset time differences and can act as a cornerstone for further advancements in wearable sensors as well as voice recognition and analysis.

Stretchable and Directly Patternable Double-Layer Structure Electrodes with Complete Coverage.

Stretchable electrodes are widely used in next-generation wearable electronics. Recent studies incorporated designs that help rigid electrodes attain stretchability. However, these structures exhibited unsatisfactory charge/signal extraction efficiency because of their low areal fill factor. Additionally, they cannot be photolithographically patterned on polymer substrates because of their low adhesion, requiring additional complicated fabrication steps. We developed photolithographically patternable stretchable electrodes with complete coverage and enhanced charge-extraction efficiency. The electrodes, comprising double layers, included a chemically treated Ag nanowire mesh and Au thin film. The interfacial linker role of polyvinylpyrrolidone chemically strengthened the interfacial bonds, and the reinforced concrete structure of nanowire-embedded metal thin films enhanced the mechanical properties. Therefore, the electrodes provided superior efficiency and stability in capturing physical, electromagnetic, and electrophysiological signals while exceeding the existing stretchable electrode limits. A broad range of applications are foreseen, such as electrocardiogram sensing electrodes, strain sensors, temperature sensors, and antennas.

Ink-Lithography for Property Engineering and Patterning of Nanocrystal Thin Films.

Next-generation devices and systems require the development and integration of advanced materials, the realization of which inevitably requires two separate processes: property engineering and patterning. Here, we report a one-step, ink-lithography technique to pattern and engineer the properties of thin films of colloidal nanocrystals that exploits their chemically addressable surface. Colloidal nanocrystals are deposited by solution-based methods to form thin films and a local chemical treatment is applied using an ink-printing technique to simultaneously modify (i) the chemical nature of the nanocrystal surface to allow thin-film patterning and (ii) the physical electronic, optical, thermal, and mechanical properties of the nanocrystal thin films. The ink-lithography technique is applied to the library of colloidal nanocrystals to engineer thin films of metals, semiconductors, and insulators on both rigid and flexible substrates and demonstrate their application in high-resolution image replications, anticounterfeit devices, multicolor filters, thin-film transistors and circuits, photoconductors, and wearable multisensors.

Noninterference Wearable Strain Sensor: Near-Zero Temperature Coefficient of Resistance Nanoparticle Arrays with Thermal Expansion and Transport Engineering.

In this study, non-temperature interference strain gauge sensors, which are only sensitive to strain but not temperature, are developed by engineering the properties and structure from a material perspective. The environmental interference from temperature fluctuations is successfully eliminated by controlling the charge transport in nanoparticles with thermally expandable polymer substrates. Notably, the negative temperature coefficient of resistance (TCR), which originates from the hopping transport in nanoparticle arrays, is compensated by the positive TCR of the effective surface thermal expansion with anchoring effects. This strategy successfully controls the TCR from negative to positive. A near-zero TCR (NZTCR), less than 1.0 × 10-6 K-1, is achieved through precisely controlled expansion. Various characterization methods and finite element and transport simulations are conducted to investigate the correlated electrical, mechanical, and thermal properties of the materials and elucidate the compensated NZTCR mechanism. With this strategy, an all-solution-processed, transparent, highly sensitive, and noninterference strain sensor is fabricated with a gauge factor higher than 5000 at 1% strain, as demonstrated by pulse and motion sensing, as well as the noninterference property under variable-temperature conditions. It is envisaged that the sensor developed herein is applicable to multifunctional wearable sensors or e-skins for artificial skin or robots.

Janus-like Jagged Structure with Nanocrystals for Self-Sorting Wearable Tactile Sensor.

In this study, a self-sorting sensor was developed with the ability to distinguish between different pressure regimes and translate the pressure to electrical signals. Specifically, the self-sorting sensor can distinguish between soft and hard pressure like the human skin, without any software assistance and complicated circuits. To achieve the self-sorting property, Janus-like jagged structures were prepared via an all-solution process of spontaneous chemical patterning; they comprised electrically semi-insulating vertices and highly conductive valleys. This unique structure facilitates the detection and determination of the intensities and types of pressure by providing a significant gap between the current levels of two types of states, similar to the function of fibers in the human tactile system. The fabricated sensors also exhibit high sensitivity and durability as well as low power consumption, as demonstrated by the electronic skin and ternary Morse signal applications. Compared with conventional wearable pressure sensors, this sensor can detect signals without additional programming; thus, it is highly suitable for delay-sensitive, energy-efficient sensor applications such as driverless vehicles, autonomous artificial intelligence technology, and prosthetic devices.

Post-synthetic oriented attachment of CsPbBr3 perovskite nanocrystal building blocks: from first principle calculation to experimental demonstration of size and dimensionality (0D/1D/2D).

Post-synthesis engineering methods that employ oriented attachment to precisely control the size and dimensionality (0D/1D/2D) of as-synthesized CsPbBr3 nanocrystals (NCs) are demonstrated. We investigated the chemical effects of the properties of polar solvents, including their immiscibility, polarity, and boiling point, on the surfaces of NCs, as well as their effect on the structural and optical properties of NCs. Appropriate exploitation of the solvent properties made it possible to use a polar solvent to mildly affect the NCs indirectly such that they discarded their ligands and became attached to proximal NCs without being destroyed. Based on our observations, we developed a method whereby a solution of the NCs in a non-polar solvent is mixed with a polar solvent to form an immiscible phase to induce epitaxial growth of CsPbBr3 NCs. The method enables the size of NCs to be easily regulated from 5 to 50 nm by controlling the engineering time. Taking advantage of the minimal effect of a mild solvent, we also developed a self-assembly method that operates at the liquid-air interface to systematically control the dimensionality. At this interface, the NCs self-assemble in the horizontal direction and grow into micron-sized, single-crystalline, defect-free nanowires (1D) and nanoplates (2D) via oriented attachment. Finally, we discuss the origin of the non-destructive oriented attachment phenomenon and the surface chemistry of a perovskite NC using density functional theory (DFT) simulations and a proposed model system.

Colloidal-annealing of ZnO nanoparticles to passivate traps and improve charge extraction in colloidal quantum dot solar cells.

The popularity of colloidal quantum dot (CQD) solar cells has increased owing to their tunable bandgap, multiple exciton generation, and low-cost solution processes. ZnO nanoparticle (NP) layers are generally employed as electron transport layers in CQD solar cells to efficiently extract the electrons. However, trap sites and the unfavorable band structure of the as-synthesized ZnO NPs have hindered their potential performance. Herein, we introduce a facile method of ZnO NP annealing in the colloidal state. Electrical, structural, and optical analyses demonstrated that the colloidal-annealing of ZnO NPs effectively passivated the defects and simultaneously shifted their band diagram; therefore, colloidal-annealing is a more favorable method as compared to conventional film-annealing. These CQD solar cells based on colloidal-annealed ZnO NPs exhibited efficient charge extraction, reduced recombination and achieved an enhanced power conversion efficiency (PCE) of 9.29%, whereas the CQD solar cells based on ZnO NPs without annealing had a PCE of 8.05%. Moreover, the CQD solar cells using colloidal-annealed ZnO NPs exhibited an improved air stability with 98% retention after 120 days, as compared to that of CQD solar cells using non-annealed ZnO NPs with 84% retention.