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Moderate Co3ZnC efficiently boosts hydrogen evolution with a high current density of 1000 mA cm−2 at a low overpotential of 219 mV via tuning the Co 3d bands, enhancing charge transfer and thus enlarging the electrochemical active surface area.

Based on silica microsphere resonators embedded with iron oxide nanoparticles, we proposed and fabricated an all-optical and continuously tunable polarization beam splitter (PBS), and a broadband optical power sensor (OPS) with high sensitivity. The PBS is realized since the effective refractive indexes of the transverse-electric and transverse-magnetic polarization modes in the microsphere resonator are different. Due to the excellent photothermal effect of iron oxide nanoparticles, we realized the all-optical and continuously tunable PBS based on the hybrid microsphere resonator. A maximum polarization splitting ratio of 20 dB and a tuning range of 5 nm are achieved. Based on this mechanism, the hybrid microsphere resonator can also be used as a broadband OPS. The sensitivity of the OPS is 0.487 nm/mW, 0.477 nm/mW, and 0.398 nm/mW when the probe wavelength is 690 nm, 980 nm, and 1550 nm, respectively. With such good performances, the tunable PBS and the broadband OPS have great potential in applications such as optical routers, switches and filters.

An all-optical control scheme of electromagnetically induced transparency (EIT) based on two coupled silica microbottle cavities coated with iron oxide nanoparticles is proposed and experimentally demonstrated. The specially designed and fabricated silica microbottle cavity with a short and spherical end, which is coated with iron oxide nanoparticles, possesses a quality (Q) factor of 1.39×108 and large all-optical tunability in a range of 282.32 GHz (2.25 nm) arising from the strong photothermal effect of the nanoparticles. Based on two coupled silica microbottle cavities, we achieve the EIT spectrum with a transparency window bandwidth of 2.3 MHz. The transparency window can be flexibly controlled by tuning the resonant frequency of the higher-Q microcavity. Besides, by tuning the resonant frequencies of the two microcavities separately, the whole EIT spectrum can be shifted with a range of 71.52 GHz, to the best of our knowledge, for the first time. Based on this scheme, we have realized all-optical and independent control of the transparency window and the whole EIT spectrum. We believe this work has great potential in applications such as light storage, optical sensing, and quantum optics.

Surface modification with polymer grafting is a versatile tool for tuning the surface properties of a wide variety of materials. From a practical point of view, such a process should be readily scalable and transferable between different substrates and consist of as least number of steps as possible. To this end, a cross-linkable amphiphilic copolymer system that is able to bind covalently to surfaces and form permanently attached networks via a one-step procedure is reported here. This system consists of brushlike copolymers (molecular brushes) made of glycidyl methacrylate, poly(oligo(ethylene glycol) methyl ether methacrylate), and lauryl methacrylate, which provide the final product with tunable reactivity and balance between hydrophilicity and hydrophobicity. The detailed study of the copolymer synthesis and properties has been carried out to establish the most efficient pathway to design and tailor this amphiphilic molecular brush system for specific applications. As an example of the applications, we showed the ability to control the deposition of graphene oxide (GO) sheets on both hydrophilic and hydrophobic surfaces using GO modified with the molecular brushes. Also, the capability to tune the osteoblast cell adhesion with the copolymer-based coatings was demonstrated.

Naturally derived materials with hierarchical organization are attractive candidates for high-performance and functional bionanocomposites because of their renewability, biocompatibility, biodegradability, flexibility, and the availability of multiple reactive sites for introducing novel functionalities. Complementary to these inherent properties, the synergistic combination of biological and synthetic components facilitated by strong interfacial interactions, can substantially enhance the structural performance and facilitate added functionalities of these bio-enabled nanocomposites. In this review, we discuss the current progress of naturally-derived bionanocomposites that has advanced our understanding of the biological/synthetic interfaces. In these bionanocomposites, various novel synthetic nanomaterials (e.g., graphene, carbon nanotube, mineral nanoparticles and metallic nanoparticles) are efficiently integrated with biological components to achieve novel properties such as superior electrical and thermal conductivity, controlled gas barrier properties, complex actuation, and unique optical properties. Two popular biocomponents, nanocellulose and silk, are mainly discussed in this review as representatives of classes of polysaccharides and polypeptides with some other biopolymers briefly discussed as well. The structures and morphologies, processing strategies, tailored functionalities and emerging applications of these bionanocomposites are analyzed and summarized. Finally, we present an outlook on the current trends in providing structural and interfacial enhancement as well as emerging applications which will employ new optical, sensing, structural, and actuating functionalities and properties.

This work demonstrates a facile and versatile method for generating low scattering cross-linked quantum dot (QD)-polymer composite films and patterned highly emissive structures with ultrahigh QD loading, minimal phase separation, and tunable mechanical properties. Uniform QD-polymer films are fabricated using thiol-ene chemistry, in which cross-linked polymer networks are rapidly produced in ambient conditions via fast UV polymerization in bulk to suppress QD aggregation. UV-controlled thiol-ene chemistry limits phase separation through producing highly QD loaded cross-linked composites with loadings above majority of those reported in the literature (1%) and approaching 30%. As the QD loading is increased, the thiol and ene conversion decreases, resulting in nanocomposites with widely variable and tailorable mechanical properties as a function of UV irradiation time with an elastic modulus decreasing to 1 GPa being characteristic of reinforced elastomeric materials, in contrast to usually observed stiff and brittle materials under these loading conditions. Furthermore, we demonstrate that the thiol-ene chemistry is compatible with soft-imprint lithography, making it possible to pattern highly loaded QD films while preserving the optical properties essential for high gain and low optical loss devices. The versatility of thiol-ene chemistry to produce high-dense QD-polymer films potentially makes it an important technique for polymer-based elastomeric optical metamaterials, where efficient light propagation is critical, like peculiar waveguides, sensors, and optical gain films.

We demonstrate the rapid, large-area transformation of bioenabled graphene laminates into multidimensional geometries for pop-up and stretchable applications. Water-vapor annealing facilitates the controlled plasticization of the multilayered silk–graphene morphologies, allowing highly localized kirigami cuts by programmable drag knife with diverse type and depth of cuts. By adjusting drag-knife depth, we can generate a microscale array of full and partial cuts, enabling a purely topological approach toward the control of metastable fold–unfold states and crack fracture paths in kirigami structures. Through orthogonal control over the graphene–silk compositeʼs nanoscale morphology, cut pattern, and semimetal-like conductivity, we showcase bioenabled laminates as a platform for prospective soft and shape-transforming electronics as flexible interconnects and stretchable energy harvesters.

Despite noteworthy progress in the fabrication of large-area graphene sheetlike nanomaterials, the vapor-based processing still requires sophisticated equipment and a multistage handling of the material. An alternative approach to manufacturing functional graphene-based films includes the employment of graphene oxide (GO) micrometer-scale sheets as precursors. However, search for a scalable manufacturing technique for the production of high-quality GO nanoscale films with high uniformity and high electrical conductivity is still continuing. Here we show that conventional dip-coating technique can offer fabrication of high quality mono- and bilayered films made of GO sheets. The method is based on our recent discovery that encapsulating individual GO sheets in a nanometer thick molecular brush copolymer layer allows for the nearly perfect formation of the GO layers via dip coating from water. By thermal reduction the bilayers (cemented by a carbon-forming polymer linker) are converted into highly conductive and transparent reduced GO films with a high conductivity up to 104 S/cm and optical transparency on the level of 90%. The value is the highest electrical conductivity reported for thermally reduced nanoscale GO films and is close to the conductivity of indium tin oxide currently in use for transparent electronic devices, thus making these layers intriguing candidates for replacement of ITO films.

The interfacial shear strength between different layers in multilayered structures of layer-by-layer (LbL) microcapsules is a crucial mechanical property to ensure their robustness. In this work, we investigated the interfacial shear strength of modified silk fibroin ionomers utilized in LbL shells, an ionic-cationic pair with complementary ionic pairing, (SF)-poly-l-glutamic acid (Glu) and SF-poly-l-lysine (Lys), and a complementary pair with partially screened Coulombic interactions due to the presence of poly(ethylene glycol) (PEG) segments and SF-Glu/SF-Lys[PEG] pair. Shearing and adhesive behavior between these silk ionomer surfaces in the swollen state were probed at different spatial scales and pressure ranges by using functionalized atomic force microscopy (AFM) tips as well as functionalized colloidal probes. The results show that both approaches were consistent in analyzing the interfacial shear strength of LbL silk ionomers at different spatial scales from a nanoscale to a fraction of a micron. Surprisingly, the interfacial shear strength between SF-Glu and SF-Lys[PEG] pair with partially screened ionic pairing was greater than the interfacial shear strength of the SF-Glu and SF-Lys pair with a high density of complementary ionic groups. The difference in interfacial shear strength and adhesive strength is suggested to be predominantly facilitated by the interlayer hydrogen bonding of complementary amino acids and overlap of highly swollen PEG segments.

We demonstrate that stronger and more robust nacre-like laminated GO (graphene oxide)/SF (silk fibroin) nanocomposite membranes can be obtained by selectively tailoring the interfacial interactions between "bricks"-GO sheets and "mortar"-silk interlayers via controlled water vapor annealing. This facial annealing process relaxes the secondary structure of silk backbones confined between flexible GO sheets. The increased mobility leads to a significant increase in ultimate strength (by up to 41%), Young's modulus (up to 75%) and toughness (up to 45%). We suggest that local silk recrystallization is initiated in the proximity to GO surface by the hydrophobic surface regions serving as nucleation sites for β-sheet domains formation and followed by SF assembly into nanofibrils. Strong hydrophobic-hydrophobic interactions between GO layers with SF nanofibrils result in enhanced shear strength of layered packing. This work presented here not only gives a better understanding of SF and GO interfacial interactions, but also provides insight on how to enhance the mechanical properties for the nacre-mimic nanocomposites by focusing on adjusting the delicate interactions between heterogeneous "brick" and adaptive "mortar" components with water/temperature annealing routines.

Power-generating flexible thin films for facile detection of biotactile events are fabricated from patterned metal-graphene oxide biopaper. These tactile materials are mechanically robust with a consistent output of 1 V and high response rate of 20 Hz. It is demonstrated that the simple quadruple electronic skin sensitively and selectively recognizes nine spatial biotactile positions and can readily be expanded.

We experimentally demonstrated an all-optical tunable sub-kHz single-mode fiber laser based on an ultrahigh-quality (Q)-factor hybrid microbottle resonator. The wavelength tunability is a very important function for fiber lasers, and the all-optical tuning method has rarely been proposed. Here, we use the iron-oxide-nanoparticle-coated silica microbottle resonator with a Q factor of 1.8×108 as the feedback element of the fiber ring laser and suppress the higher-order modes of the microresonator to achieve single-mode lasing with a linewidth of ∼500 Hz and a signal-to-noise ratio of 49 dB. Iron oxide nanoparticles are coated on the tapered area of the microbottle resonator and the control light is fed through the axial direction of the microbottle. The lasing wavelength of the fiber laser can be all-optically and linearly tuned with a range of 2.7 nm due to the strong photothermal effect of iron oxide nanoparticles. With such an excellent tunability and a narrow linewidth, this single-mode fiber laser has great potential in applications, such as optical spectroscopy, sensing, and signal processing.

Ultra-robust nanomembranes possessing high mechanical strength combined with excellent stiffness and toughness rarely achieved in nanocomposite materials are presented. These are fabricated by alternately depositing 1D cellulose nanocrystals and 2D graphene oxide nanosheets by using a spin assisted layer-by-layer assembly technique. Such a unique combination of 1D and 2D reinforcing nanostructures results in layered nanomaterials.

Novel nacre-mimic bio-nanocomposites, such as graphene-based laminates, are pushing the boundaries of strength and toughness as flexible engineering materials. Translating these material advances to functional flexible electronics requires methods for generating print-scalable microcircuits (conductive elements surrounded by dielectric) into these strong, tough, lightweight bio-nanocomposites. Here, a new paradigm for printing flexible electronics by employing facile, eco-friendly seriography to confine the reduction of graphene oxide biopapers reinforced by silk interlayers is presented. Well-defined, micropatterned regions on the biopaper are chemically reduced, generating a 106 increase in conductivity (up to 104 S m−1). Flexible, robust graphene-silk circuits are showcased in diverse applications such as resistive moisture sensors and capacitive proximity sensors. Unlike conductive (i.e., graphene- or Ag nanoparticle-loaded) inks printed onto substrates, seriography-guided reduction does not create mechanically weak interfaces between dissimilar materials and does not require the judicious formation of ink. The unimpaired functionality of printed-in graphene-silk microcircuits after thousands of punitive folding cycles and chemical attack by harsh solvents is demonstrated. This novel approach provides a low-cost, portable solution for printing micrometer-scale conductive features uniformly across large areas (>hundreds of cm2) in layered composites for applications including wearable health monitors, electronic skin, rollable antennas, and conformable displays.