Many materials systems comprise complex structures where multiple materials are integrated to achieve a desired performance. Often in these systems, it is a combination of both the materials and their structure that dictate performance. Here the authors layout an integrated computational–statistical–experimental methodology for hierarchical materials systems that takes a holistic design approach to both the material and structure. The authors used computational modeling of the physical system combined with statistical design of experiments to explore an activated carbon adsorption bed. The large parameter space makes experimental optimization impractical. Instead, a computational–statistical approach is coupled with physical experiments to validate the optimization results.

The remarkable broadband and omnidirectional anti-reflectivity observed in the glasswing butterfly arises from the random array of nanopillars present on their wings. In the present study, analogous structures have been replicated on transparent substrates using a scalable, low-cost method that exploits surface dewetting of silver thin films on silica substrates to form an etch mask. Directional etching was applied with high selectivity between Ag and SiO2 using CHF3, allowing large aspect ratios to be achieved with 20 min etches. Single-sided nanostructuring of glass by this method improved the transmission of light by 2–8% for viewing angles of 25°, 45°, and 65°.

In the current manuscript we discuss the response of dynamic metallogels that display reversion to the liquid state when exposed to phosphines. The metallogels are formed through the condensation of formaldehyde and poly(alkyloxide)amines in polar aprotic solvents. The gel formation can be catalyzed with trivalent metals (Al(III and Fe(III)) with concomitant enhanced dynamism (gelation/degelation). When various phosphines are introduced, the metallogel is irreversibly liquefied. This process adds a new vector for controlling the bulk properties of this class of materials. Here, we explore the mechanism in detail for the reaction of tris(carboxyethyl)phosphine with N,N,N-triethoxylethyl-1,3,5-hexahydro-1,3,5-triazine (HEHT, 1) a stable derivative of the active hexahydrotriazine (HT) core in dimethylformamide in the presence or absence of Al(III). Additionally, density functional theory is used on the model N,N,N-trimethyl system (MHT, 2) to estimate reaction parameters and predict nuclear magnetic resonance spectra.

Scanning thermal microscopy allows thermal characterization with nanoscale resolution. However, quantitative usage has been met with skepticism, because no standard exists for calibrating probe–sample thermal exchange. In this paper, three published strategies for calibrating probe–sample thermal exchange are directly compared, then used to measure bulk and thin-film thermal conductivity. It is shown that with an appropriately calibrated probe and film-on-substrate heat conduction model, thermal conductivity values of ultrathin-film (2.9–202 nm) Al2O3 on silicon are within 20% deviation of independently measured values, while more commonly used methods yield values that may deviate by more a factor of two.

Solid state batteries are an emerging alternative to traditional liquid electrolyte cells that provide potential for safe and high-energy density power sources. This report describes a self-forming, solid state battery based on the Li/I2 couple using an LiI-rich LiI(3-hydroxypropionitrile)2 electrolyte (LiI–LiI(HPN)2). As the negative and positive active materials are generated in situ, the solid electrolyte–current collector interfaces play a critical role in determining the electrochemical response of the battery. Herein, we report the investigation of solid electrolyte–current collector interfaces with a self-forming LiI–LiI(HPN)2 solid electrolyte and the role of varying interface design in reducing resistance during cycling.

This work is based on a recent theoretical study of how the hydrostatic pressure and core/shell sizes affect the optical properties associated with the transition from the ground state to first excited state (1s–1p), of an exciton confined in spherical core/shell quantum dots (SCSQDs). We have computed under an effective mass framework, linear, third-order nonlinear, and total absorption coefficients (AC) and refractive index (RI) as functions of photon energy for different sizes of SCSQDs with varying hydrostatic pressure. Our results show that the optical absorption is deeply dependent on the incident light intensity. Both AC and RI significantly influenced by the confinement and pressure effects.

We have successfully employed a charge transfer mechanism to convert carbon nanotube (CNT) powder into CNT flexible membrane with no binder. We have demonstrated the use of the CNT membranes as electrode in a stacked bipolar solid-state capacitor using grafoil as current collector that showed 80% capacitance retention over 10,000 cycles at 70 °C. The CNT membranes could have potential application in catalysis, photovoltaic, thermoelectric, and many others.

One of the critical components of energy savings in buildings is thermal insulation, especially for windows in cold climates. The conventional approach mainly relies on a double-pane design. In this study, a new concept of “Green Window” has been designed for single-pane applications that lower the U-factor. The “Green Window” is structurally and simply composed of a thin film window coating of chlorophyll that exhibits pronounced photothermal effect, while remaining highly transparent. We demonstrate a new concept in “thermal insulation” via optical means instead of solely through thermal insulators or spectral selectivity. This concept lifts the dependence on insulating materials making single-pane window highly possible.

Powering autonomous electronic devices is a key challenge toward the development of smart sensor networks. In this work, a state-of-the-art triboelectric nanogenerator is devised to enhance the output performance with an effective surface charge density of 70.2 µC/m2, which is 140 times higher than the initial results. Thin film Parylene-C material is deposited to increase charge accumulation by allowing the acceptance of more charges and enhance output performance by a factor of 10. By considering the merit of simple fabrication, we believe the effective charge inclusion layer will be an ideal energy source for low-power portable electronics.

A facile and low-cost method based for tension gradient self-assembly was developed to prepare polytetrafluoroethylene (PTFE) nanofiber coatings on stainless-steel fiber felts. The PTFE particles were used as building blocks and the self-assembly process was analyzed thoroughly. After being sintered, the PTFE particles were transformed into PTFE nanofibers. The felts coated with the PTFE nanofibers exhibited superhydrophobicity and superoleophilicity, and could separate a series of oil–water mixtures with high efficiency and good reusability. The coated felts also presented excellent chemical and thermal stabilities. Over all, this approach could easily fabricate ultra-robust oil–water separation materials suitable for industrial applications.

Aluminum-doped zinc oxide (AZO) is one of the most promising transparent conductive oxide materials for a front electrode in solar cells. In this work, we roughened substrate surface and sputtered AZO films, where the effect of roughness on various AZO properties was investigated. The haze values were largely enhanced, retaining other important properties such as conductivity and transparency. The optical band gap exhibits a clear blue shift because of the roughness. The possible cause of this shift may be variation in the Al content due to the different deposition and post-annealing mechanisms of AZO films on the roughened surface.

Quantum dots (QDs) are increasingly employed in biologic imaging applications; however, anecdotal reports suggest difficulties in QD bioconjugation. Further, the stability of commercial QDs during bioconjugation has not been systematically evaluated. Thus, we examined fluorescence losses resulting from aggregation and declining photoluminescence quantum yield (QY) for commercial CdSe/ZnS QD products from four different vendors. QDs were most stable in the aqueous media in which they were supplied. The largest QY declines were observed during centrifugal filtration, whereas the largest declines in colloidal stability occurred in 2-(N-morpholino)ethanesulfonic acid (MES) buffer. These results enable optimization of bioconjugation protocols.

Due to the lack of the stability of amine films, a promising transducer, quartz-tuning fork (QTF) prongs were modified by a bi-layer film of plasma-polymerized n-heptane (hep) and then by ethylenediamine (EDA), respectively. For this purpose, the authors investigate the stability of amine-rich thin films both in air and aqueous medium. EDA films were deposited on QTF substrates by using an RF plasma system. The final amine-rich thin film was used to immobilize biologic recognition element. Model protein studies were showed that selected thin films could be adapted to QTF transducers to be used as a biosensor template.

AgNPs@g-C3N4 composite was synthesized from Ag-containing sol and g-C3N4 powder by the ultrasonic-assisted self-assembly method. The composite has hierarchical pore size distributions, which will be beneficial to the ion transport with different size. Ag nanoparticles with the size of 5 nm successfully adhere on the surface of g-C3N4. The AgNPs@g-C3N4 composite has excellent specific capacitance and specific power performance for the supercapacitors as an electrode material. The specific capacitance of composite is 4 times greater than that of g-C3N4. It can be ascribed to the introduction of Ag nanoparticles that the internal resistance of the composite is significantly decreased.

Improvement of the performance of renewable electronic devices is a crucial point for the consolidation of this emerging technology. Herein, we develop a supercapacitor based on cellulose, carbon nanotubes, and ionic liquids. A conductive paper prepared by simple acid hydrolysis of cellulose and carboxylated carbon nanotubes was used as an electrode. A cellulose sponge impregnated with 1-n-butyl-3-methylimidazolium bis(trifluoromethane sulfonyl)imide was used as a separator/electrolyte. Electrochemical tests were performed in a two-electrode cell that presented a specific capacitance of 34.37 F/g when considered the active mass and 97.9% of capacitance retention after 5000 charge/discharge cycles.

Unlike other data intensive domains, understanding distributions, trends, correlations, and relationships in materials data sets typically involves navigating high-dimensional spaces with only a limited number of observations. Under these conditions extracting structure/property relationships is not straightforward and considerable attention must be given to the reduction of feature space before predictions can be made. Here we have used Kohonen networks (self-organizing maps) to identify hidden structure/property relationships in computational sets of twinned and single-crystal diamond nanoparticles based on structural similarity in multiple dimensions, and confirmed the importance of a limited number of surface chemical features using regression.

Luminescent oxygen sensor composed of platinum-porphyrin and a gas-permeable polymer binder was applied as an optical crack sensor paint for infrastructure. The sensor paints were designed as a three-layered structure in which the luminescent oxygen sensor layer was sandwiched between oxygen barrier layers. The sensor paints emitted intense luminescence under UV light irradiation, and the luminescence was efficiently quenched when a new crack formed on the concrete surface. Microcracks, which were <0.1 mm width and hardly visible to the naked eye, were clearly visualized under UV light irradiation due to the luminescent quenching caused by oxygen diffusion.

Hollow mesoporous polydopamine (HMPDA) microcapsules were prepared by a template method using silica nanoparticles as the templates. The template method was also used for the formation of mesoporous polydopamine (PDA), which is driven by π–π interactions of trimethylbenzene and PDA, in which the PDA wall with mesoporous structure can be obtained after template removal by extraction. Because of its surface mesoporous structure and large central cavity structure, HMPDA microcapsules have unique adsorption properties. Compared with other porous materials, PDA has better biosafety because dopamine itself is a bionic material. The above properties are of great significance for the application of HMPDA microcapsules in the field of biologic medicine, especially in drug carriers.

To identify new face centered cubic high entropy alloys (HEAs), MnFeCoNiCu thin film samples were prepared by simultaneous magnetron sputtering of elements onto Si wafers. This sputtering arrangement yielded compositional gradients in the samples. The films exhibited regions with different phases, some of which were single-phase and non-equiatomic. To screen the crystal structure and composition across film samples, multiple characterization techniques were used: scanning electron microscopy, focused ion beam, energy-dispersive x-ray spectroscopy, x-ray diffraction, and electron backscattered diffraction analysis. Using this combinatorial method, candidate single-phase HEAs were identified and then successfully arc-melted in bulk form, followed by thermomechanical processing.

Indentation and scratch models are proposed to numerically investigate effects of compressive prestress on film's mechanical responses. In indentation, normal stress distributions are strongly dependent on film thickness; the applied force and the maximum normal stresses with a prestress are much larger than without prestress. For various film thicknesses the change in the normal force in scratch between the non-prestressed and prestressed films is 4%–23%. The scratch friction coefficient is larger with prestress than without prestress. With biaxial or uniaxial prestress the material becomes more difficult to deform or to slide at the contact surface compared with cases without prestress.