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We describe a novel approach for the rational design and synthesis of self-assembled periodic nanostructures using martensitic phase transformations. We demonstrate this approach in a thin film of perovskite SrSnO3 with reconfigurable periodic nanostructures consisting of regularly spaced regions of sharply contrasted dielectric properties. The films can be designed to have different periodicities and relative phase fractions via chemical doping or strain engineering. The dielectric contrast within a single film can be tuned using temperature and laser wavelength, effectively creating a variable photonic crystal. Our results show the realistic possibility of designing large-area self-assembled periodic structures using martensitic phase transformations with the potential of implementing built-to-order nanostructures for tailored optoelectronic functionalities.
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Adding thermal conductivity enhancements to increase thermal power in solid-liquid phase-change thermal energy storage modules compromises volumetric energy density and often times reduces the mass and volume of active phase change material (PCM) by well over half. In this study, a new concept of building thermal energy storage modules using high-conductivity, solid-solid, shape memory alloys is demonstrated to eliminate this trade-off and enable devices that have both high heat transfer rate and high thermal capacity. Nickel titanium, Ni50.28Ti49.36, was solution heat treated and characterized using differential scanning calorimetry and Xenon Flash to determine transformation temperature (78deg-C), latent heat (183 kJm-3), and thermal conductivity in the Austenite and Martensite phases (12.92/12.64 Wm-1K-1). Four parallel-plate thermal energy storage demonstrators were designed, fabricated, and tested in a thermofluidic test setup. These included a baseline sensible heating module (aluminum), a conventional solid-liquid PCM module (aluminum/1-octadecanol), an all-solid-solid PCM module (Ni50.28Ti49.36), and a composite solid-solid/solid-liquid PCM module (Ni50.28Ti49.36/1-octadecanol). By using high-conductivity solid-solid PCMs, and eliminating the need for encapsulants and conductivity enhancements, we are able to demonstrate a 1.73-3.38 times improvement in volumetric thermal capacity and a 2.03-3.21 times improvement in power density as compared to the conventional approaches. These experimental results are bolstered by analytical models to explain the observed heat transfer physics and reveal a 5.86 times improvement in thermal time constant. This work demonstrates the ability to build high-capacity and high-power thermal energy storage modules using multifunctional shape memory alloys and opens the door for leap ahead improvement in thermal energy storage performance.
Self-assembled, semimetallic ErSb single crystal nanostructures, grown by molecular beam epitaxy, are embedded within a semiconductor GaSb matrix. Formation, evolution and orientation of a variety of nanostructures, including spherical nanoparticles, elongated nanorods, octagonal shaped nanowires oriented along the surface normal and nanowires oriented in the growth plane, are controlled simply by the Er fraction. The plasmonic properties of the semimetal/semiconductor composites are characterized and quantified by three polarization-resolved spectroscopy techniques, spanning more than three orders of magnitude in frequency from 100 GHz up to 300 THz. The effect of the size, shape and orientation of the nanostructures is characterized by polarization-sensitive response and modeled by a Maxwell-Garnett effective medium theory.
Layered multi-ferroic materials exhibit a variety of functional properties that can be tuned by varying the temperature and pressure. As-synthesized CuInP$_2$S$_6$ is a layered material that displays ferrielectric behavior at room temperature. When synthesized with Cu deficiencies, CuInP$_2$S$_6$ spontaneously phase segregates to form ferrielectric CuInP$_2$S$_6$ (CIPS) and paraelectric In$_{4/3}$P$_2$S$_6$ (IPS) domains in a two-dimensional self-assembled heterostructure. Here, we study the effect of hydrostatic pressure on the structure of Cu-deficient CuInP$_2$S$_6$ by Raman spectroscopy measurements up to 20 GPa. Detailed analysis of the frequencies, intensities, and linewidths of the Raman peaks reveals four discontinuities in the spectra around 2, 10, 13 and 17 GPa. At ~2 GPa, we observe a structural transition initiated by the diffusion of IPS domains, which culminates in a drastic reduction of the number of peaks around 10 GPa. We attribute this to a possible monoclinic-trigonal phase transition at 10 GPa. At higher pressures (~ 13 GPa), significant increases in peak intensities and sharpening of the Raman peaks suggest a bandgap-lowering and an isostructural electronic transition, with a possible onset of metallization at pressures above 17 GPa. When the pressure is released, the structure again phase-separates into two distinct chemical domains within the same single crystalline framework -- however, these domains are much smaller in size than the as-synthesized material resulting in suppression of ferroelectricity through nanoconfinement. Hydrostatic pressure can thus be used to tune the electronic and ferrielectric properties of Cu-deficient layered CuInP$_2$S$_6$.
We propose systems with structures defined by self-assembled triply periodic minimal surfaces (STPMS) as candidates for photonic bandgap materials. To support our proposal we have calculated the photonic bands for different STPMS and we have found that, at least, the double diamond and gyroid structures present full photonic bandgaps. Given the great variety of systems which crystalize in these structures, the diversity of possible materials that form them and the range of lattice constants they present, the construction of photonic bandgap materials with gaps in the visible range may be presently within reach.
Colloidal crystals exhibit structural color without any color pigment due to the crystals periodic nanostructure, which can interfere with visible light. This crystal structure is iridescent as the resulting color changes with the viewing or illumination angle, which limits its use for printing or displays. To eliminate the iridescent property, it is important to make the packing of the colloidal nanoparticles disordered. Here, we introduce a drop-casting method where a droplet of a water- ethanol mixture containing monodisperse polymer-coated silica nanoparticles creates a relatively uniform and non-iridescent deposit after the droplet evaporates completely on a heated substrate. The uniformity is caused by a thermal Marangoni flow and fast evaporation effects due to the heated substrate, whereas non-iridescence is the outcome of short-range-ordered packing of nanoparticles by depletion attraction and friction effects produced by polymer brushes. We show that the colors of the final deposits from individual droplets remain unchanged while the viewing angle is varied under ambient light. We expect that the coating method is compatible with ink-jet printing and the uniformly coated self-assembled non-iridescent nanostructures have potential for color displays using reflection mode and other optical devices.
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