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Mechanochromic smart membranes capable of optical modulation have great potential in smart windows, artificial skins, and camouflage. However, the realization of high-contrast optical modulation based on light scattering activated at a low strain remains challenging. Here, we present a strategy for designing mechanochromic scattering membranes by introducing a Young's modulus mismatch between the two interdigitated polydimethylsiloxane phases with weak interfaces in a periodic three-dimensional (3D) structure. The refractive index-matched interfaces of the nanocomposite provide a high optical transparency of 93%. Experimental and computational studies reveal that the 3D heterogeneity facilitates the generation of numerous nanoscale debonds or "nanogaps"at the modulus-mismatching interfaces, enabling incident light scattering under tension. The heterogeneous scatterer delivers both a high transmittance contrast of >50% achieved at 15% strain and a maximum contrast of 82%. When used as a smart window, the membrane demonstrates effective diffusion of transmitting sunlight, leading to moderate indoor illumination by eliminating extremely bright or dark spots. At the other extreme, such a 3D heterogeneous design with strongly bonded interfaces can enhance the coloration sensitivity of mechanophore-dyed nanocomposites. This work presents insights into the design principles of advanced mechanochromic smart membranes. © 2021 American Chemical Society.

A rational approach is proposed to design soft multifunctional sensors capable of detection and discrimination of different physical stimuli. Herein, a flexible multifunctional sensor concurrently detecting and distinguishing minute temperature and pressure stimuli in real time is developed using electrospun carbon nanofiber (CNF) films as the sole sensing material and electrical resistance as the only output signal. The stimuli sensitivity and discriminability are coordinated by tailoring the atomic- and device-level structures of CNF films to deliver outstanding pressure and temperature sensitivities of −0.96 kPa−1 and −2.44% °C−1, respectively, enabling mutually exclusive sensing performance without signal cross-interference. The CNF multifunctional sensor is considered the first of its kind to accomplish the stimulus discriminability using only the electrical resistance as the output signal, which is most convenient to monitor and process for device applications. As such, it has distinct advantages over other reported sensors in its simple, cost-effective fabrication and readout system. It also possesses other invaluable traits, including good bending stability, fast response time, and long-term durability. Importantly, the ability to simultaneously detect and decouple temperature and pressure stimuli is demonstrated through novel applications as a skin-mountable device and a flexible game controller. © 2021 Wiley-VCH GmbH

In this era of the Internet of Things, the development of innovative sensors has rapidly accelerated with that of nanotechnology to accommodate various demands for smart applications. The practical use of three-dimensional (3D) nanostructured materials breaks several limitations of conventional sensors, including the large surface-to-volume ratio, precisely tunable pore size and porosity, and efficient signal transduction of 3D geometries. This review provides an in-depth discussion on recent advances in chemical and mechanical sensors based on 3D nanostructures, which are rationally designed and manufactured by advanced 3D nanofabrication techniques that consider structural factors (e.g., porosity, periodicity, and connectivity). In particular, we focus on a proximity-field nanopatterning technique that specializes in the production of periodic porous 3D nanostructures that satisfy the structural properties universally required to improve the performance of various sensor systems. State-of-the-art demonstrations of high-performance sensor devices such as supersensitive gas sensors and wearable strain sensors realized through designed 3D nanostructures are summarized. Finally, challenges and outlooks related to nanostructures and nanofabrication for the practical application of 3D nanostructure-based sensor systems are proposed.

Smart chromatic materials with optical transmittances that can be modified by light scattering upon external stimuli are attracting extensive interest because of their appealing applications in smart windows, privacy protection, electronic displays, etc. However, the development of these scatterers, which are mostly activated by electric fields, is hindered by their intrinsic energy consumption, slow responses, and poor stability. Recently, mechanoresponsive scatterers based on a strain-driven reconfiguration of the surface or internal structure have emerged, featuring fast responses and a simple composition/fabrication. Because there is no energy consumption to maintain the transparency/opacity, this novel scheme for scatterers holds great promise to break the existing bottleneck. This article presents recent advances in the development of mechanoresponsive scatterers and compares different structural design strategies. The scatterers are categorized into 2D, 3D, and other types according to the dimensions of their functioning structures. The fabrication methods, mechanisms, and relationships between the structural parameters and optical modulating performances are discussed for each category. Next, the potential applications of these scatterers are outlined. Finally, the advantages and disadvantages of the mainstream 2D and 3D categories are summarized, followed by a perspective on future research directions.

Achieving abundant active sites in catalysts by fabricating three-dimensional (3D) microstructures is an efficient approach for improving their oxygen evolution reaction (OER) activities. However, the generated oxygen bubbles in the electrodes are confined in the complex 3D structure, diminishing the catalytic activities and mechanical stability of the electrodes. Therefore, it is essential to rationally design an electrocatalytically active 3D electrode with an optimal microstructure to efficiently remove generated bubbles. Here, we report the fabrication of copper oxide nanoparticles embedded in nonoxidized graphene aerogels (CuONP-NOGAs). The microstructure of CuONP-NOGAs is finely tuned by optimizing the processing parameters of bidirectional freeze casting and its influence on bubble removal behavior efficiency is elucidated. Among electrodes with different degrees of alignment and pore densities, the vertically aligned NOGA with dense porosity exhibits the best efficiency by forming direct open paths for facile bubble movements. The high electrical conductivity combined with a low transfer resistance and uniformly dispersed active particles in CuONP-NOGAs offers excellent OER activities. They deliver a remarkable potential of 1.39 V at 10 mA/cm2, which is lower than those of the state-of-the-art RuO2 and other copper oxide-based catalysts, as well as ultralong stability of more than 120 h, proving the significance of the effective design of the 3D catalyst microstructure. The present study may provide insights into the design of new 3D microstructures useful for practical application in next-generation energy conversion devices. © 2021 American Chemical Society.

Continuous real-time measurement of body temperature using a wearable sensor is an essential part of human health monitoring. Electrospun aligned carbon nanofiber (ACNF) films are employed to assemble flexible temperature sensors. The temperature sensor prepared at a low carbonization temperature of 650 °C yields an outstanding sensitivity of 1.52% °C−1, high accuracy, good linearity, fast response time and excellent long-term durability. Moreover, it exhibits high discriminability towards temperature amidst other unwanted stimuli and maintains its original performance even after repeated stretch/release cycles because of highly-aligned structures. The correlation between the atomic structure and the temperature sensing performance of ACNF sensors is established. Contrary to conventional highly conductive temperature sensors, the ACNF sensor with a low electrical conductivity prepared at a low carbonization temperature ameliorates the temperature sensing performance. This anomaly is explained by (i) the smaller and more disordered sp2 carbon crystallites yielding a high negative temperature coefficient, (ii) a larger number of defects, and (iii) a higher pyridinic-N content generating abundant entrapped and localized electrons which are activated once sufficient thermal energy is available. Flexible ACNF sensor's overall performance is among the best-known carbon material-based flexible temperature sensors, demonstrating potential applications in emerging healthcare and flexible electronics technologies.

Three-dimensional (3D) nanoarchitectures have offered unprecedented material performances in diverse applications like energy storages, catalysts, electronic, mechanical, and photonic devices. These outstanding performances are attributed to unusual material properties at the nanoscale, enormous surface areas, a geometrical uniqueness, and comparable feature sizes with optical wavelengths. For the practical use of the unusual nanoscale properties, there have been developments for macroscale fabrications of the 3D nanoarchitectures with process areas over centimeter scales. Among the many fabrication methods for 3D structures at the nanoscale, proximity-field nanopatterning (PnP) is one of the promising techniques that generates 3D optical holographic images and transforms them into material structures through a lithographic process. Using conformal and transparent phase masks as a key factor, the PnP process has advantages in terms of stability, uniformity, and reproducibility for 3D nanostructures with periods from 300 nm to several micrometers. Other merits of realizing precise 3D features with sub-100 nm and rapid processes are attributed to the interference of coherent light diffracted by phase masks. In this review, to report the overall progress of PnP from 2003, we present a comprehensive understanding of PnP, including its brief history, the fundamental principles, symmetry control of 3D nanoarchitectures, material issues for the phase masks, and the process area expansion to the wafer-scale for the target applications. Finally, technical challenges and prospects are discussed for further development and practical applications of the PnP technique. [Figure not available: see fulltext.] © 2021, Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature.

Smart chromatic materials with optical transmittances that can be modified by light scattering upon external stimuli are attracting extensive interest because of their appealing applications in smart windows, privacy protection, electronic displays, etc. However, the development of these scatterers, which are mostly activated by electric fields, is hindered by their intrinsic energy consumption, slow responses, and poor stability. Recently, mechanoresponsive scatterers based on a strain-driven reconfiguration of the surface or internal structure have emerged, featuring fast responses and a simple composition/fabrication. Because there is no energy consumption to maintain the transparency/opacity, this novel scheme for scatterers holds great promise to break the existing bottleneck. This article presents recent advances in the development of mechanoresponsive scatterers and compares different structural design strategies. The scatterers are categorized into 2D, 3D, and other types according to the dimensions of their functioning structures. The fabrication methods, mechanisms, and relationships between the structural parameters and optical modulating performances are discussed for each category. Next, the potential applications of these scatterers are outlined. Finally, the advantages and disadvantages of the mainstream 2D and 3D categories are summarized, followed by a perspective on future research directions.