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Functional thin film superlattices with stability in extreme environments can lead to transformative performance in optical and thermal applications such as thermophotovoltaics. In this work, key issues associated with defects that prevent layer-by-layer growth in epitaxial, low-miscibility oxide superlattices are investigated. Layer protrusions, approximately 8 nm wide and 3 nm thick, arise from a strain relaxation mechanism in 8 nm bilayer superlattices of Ba(Zr0.5Hf0.5)O3/MgO and propagate through the subsequent superlattice layers forming an inverted pyramid structure that is spatially phase offset from the matrix. The density and size of these defects scales with the number of interfaces in the sample, indicating that surface roughness during growth is a significant factor in the formation of these defects. In situ high temperature transmission electron microscopy (1000 °C, in vacuo) measurement reveals that phase decomposition of Ba(Zr0.5Hf0.5)O3 and decoherence of the superlattice is nucleated by these defects. This work highlights that achieving optimum growth conditions is imperative to the synthesis of single-crystalline superlattices with sharp interfaces for optimized performance in extreme environments. [ABSTRACT FROM AUTHOR]

We present a radiative cooling material capable of enhancing albedo while reducing ground surface temperatures beneath fielded bifacial solar panels. Electrospinning a layer of polyacrylonitrile nanofibers, or nanoPAN, onto a polymer-coated silver mirror yields a total solar reflectance of 99 %, an albedo of 0.96, and a thermal emittance of 0.80. The combination of high albedo and high emittance is enabled by wavelength-selective scattering induced by the hierarchical morphology of nanoPAN, which includes both thin fibers and bead-like structures. During outdoor testing, the material outperforms the radiative cooling power of a state-of-the-art control by ∼20 W/m2 and boosts the photocurrent produced by a commercial silicon cell by up to 6.4 mA/cm2 compared to sand. These experiments validate essential characteristics of a high-albedo radiative-cooling reflector with promising potential applications in thermal and light management of fielded bifacial panels. [ABSTRACT FROM AUTHOR]

Gradient epsilon-near-zero (ENZ) metamaterials offer broadband directional control over thermal emission. Implementing this approach using materials that remain stable in harsh thermo-chemical environments would allow it to be broadly deployed in thermal photonics. Our prior work showed that heterostructures of rock salt MgO and perovskite BaZr0.5Hf0.5O3 (BZHO) are stable up to 1100 °C in air, with no discernible intermixing. In this work, we design a gradient ENZ metamaterial made from three lattice-matched refractory oxides: MgO, BZHO, and NiO. The miscibility of MgO and NiO makes it possible to linearly vary the ENZ frequency of the metamaterial layers. BZHO is used as a thin, interlayer diffusion barrier. We model the emissivity of our gradient ENZ metamaterial at 25 and 1000 °C to demonstrate that the spectral bandwidth of directional emission is preserved at high temperatures despite changes in the optical properties of each material. Finally, we discuss practical fabrication challenges associated with the back reflector and offer potential solutions based on advancements in hetero-integration. Overall, this work shows a pathway toward gradient ENZ metamaterials with ultrahigh-temperature stability. [ABSTRACT FROM AUTHOR]

Although spectrally selective materials play a key role in existing and emerging solar thermal technologies, temperature‐related degradation currently limits their use to below 700 °C in vacuum and even lower temperatures in air. Here a solar‐transparent refractory aerogel that offers stable performance up to 800 °C in air is demonstrated, which is significantly greater than its silica counterpart. This improved stability is attributed to the formation of a refractory aluminum silicate phase, which is synthesized using a conformal single cycle of atomic layer deposition within the high‐aspect‐ratio pores of silica aerogels. Based on direct heat loss measurements, the transparent refractory aerogel achieves a receiver efficiency of 75% at 100 suns and an absorber temperature of 700 °C, which is a 5% improvement over the state of the art. Transparent refractory aerogels may find widespread applicability in solar thermal technologies by enabling the use of lower‐cost optical focusing systems and eliminating the need for highly evacuated receivers. In particular, a shift to higher operating temperatures while maintaining a high receiver efficiency can enable the use of advanced supercritical CO2 power cycles and ultimately translate to an ≈10% (absolute) improvement in solar‐to‐electrical conversion efficiency relative to existing linear concentrating systems. [ABSTRACT FROM AUTHOR]

Although spectrally selective materials play a key role in existing and emerging solar thermal technologies, temperature‐related degradation currently limits their use to below 700 °C in vacuum and even lower temperatures in air. Here a solar‐transparent refractory aerogel that offers stable performance up to 800 °C in air is demonstrated, which is significantly greater than its silica counterpart. This improved stability is attributed to the formation of a refractory aluminum silicate phase, which is synthesized using a conformal single cycle of atomic layer deposition within the high‐aspect‐ratio pores of silica aerogels. Based on direct heat loss measurements, the transparent refractory aerogel achieves a receiver efficiency of 75% at 100 suns and an absorber temperature of 700 °C, which is a 5% improvement over the state of the art. Transparent refractory aerogels may find widespread applicability in solar thermal technologies by enabling the use of lower‐cost optical focusing systems and eliminating the need for highly evacuated receivers. In particular, a shift to higher operating temperatures while maintaining a high receiver efficiency can enable the use of advanced supercritical CO2 power cycles and ultimately translate to an ≈10% (absolute) improvement in solar‐to‐electrical conversion efficiency relative to existing linear concentrating systems. [ABSTRACT FROM AUTHOR]

Stabilizing high dispersions of catalytically active metals is integral to improving the lifetime, activity, and material utilization of catalysts that are periodically exposed to high temperatures during operation or maintenance. We have found that annealing palladium-based core@shell catalysts in air at elevated temperatures (800 °C) promotes the redispersion of active metals into highly dispersed sites, which we refer to as halo sites. Here, we examine the restructuring of Pd@SiO2 and Pd@CeO2 core@shell catalysts over successive 800 °C aging cycles to understand the formation, activity, nanoscale structure, and stability of these palladium halo sites. While encapsulation generally improves metal utilization by providing a physical barrier that promotes redispersion over agglomeration, our cycled aging experiments demonstrate that halo sites are not stable in all catalysts. Halo sites continue to migrate in Pd@SiO2 due to poor metal–support bonding, which leads to palladium agglomeration. In contrast, halo sites formed in Pd@CeO2 remain stable. The dispersed palladium also synergistically stabilizes the ceria from agglomerating. We attribute this stability, in addition to an observed improvement in catalytic activity, to the coordination between palladium and reducible ceria that arises during the formation of halo sites. We probe the importance of ceria oxidation state on the stability of halo sites by aging Pd@CeO2 after it has been reduced. While some halo sites agglomerate, we find that returning to air aging mitigates the loss of these sites and catalytic activity. Our findings illustrate how nanoscale catalyst structures can be designed to promote the formation of highly stable and dispersed metal sites. [ABSTRACT FROM AUTHOR]

Thermophotovoltaic cells are similar to solar cells, but instead of converting solar radiation to electricity, they are designed to utilize locally radiated heat. Development of high-efficiency thermophotovoltaic cells has the potential to enable widespread applications in grid-scale thermal energy storage1,2, direct solar energy conversion3–8, distributed co-generation9–11 and waste heat scavenging12. To reach high efficiencies, thermophotovoltaic cells must utilize the broad spectrum of a radiative thermal source. However, most thermal radiation is in a low-energy wavelength range that cannot be used to excite electronic transitions and generate electricity. One promising way to overcome this challenge is to have low-energy photons reflected and re-absorbed by the thermal emitter, where their energy can have another chance at contributing towards photogeneration in the cell. However, current methods for photon recuperation are limited by insufficient bandwidth or parasitic absorption, resulting in large efficiency losses relative to theoretical limits. Here we demonstrate near-perfect reflection of low-energy photons by embedding a layer of air (an air bridge) within a thin-film In0.53Ga0.47As cell. This result represents a fourfold reduction in parasitic absorption relative to existing thermophotovoltaic cells. The resulting gain in absolute efficiency exceeds 6 per cent, leading to a very high power conversion efficiency of more than 30 per cent, as measured with an approximately 1,455-kelvin silicon carbide emitter. As the out-of-band reflectance approaches unity, the thermophotovoltaic efficiency becomes nearly insensitive to increasing cell bandgap or decreasing emitter temperature. Accessing this regime may unlock a range of possible materials and heat sources that were previously inaccessible to thermophotovoltaic energy conversion. An air gap embedded within the structure of a thermophotovoltaic device acts as a near-perfect reflector of low-energy photons, resulting in their recovery and recycling by the thermal source, enabling excellent power-conversion efficiency. [ABSTRACT FROM AUTHOR]

The thermoelectric properties of molecular junctions are of considerable interest due to their promise for efficient energy conversion. While the dependence of thermoelectric properties of junctions on molecular structure has been recently studied, their temperature dependence remains unexplored. Using a custom built variable temperature scanning tunneling microscope, we measured the thermopower and electrical conductance of individual benzenedithiol junctions over a range of temperatures (100K–300K). We find that while the electrical conductance is independent of temperature, the thermopower increases linearly with temperature, confirming the predictions of the Landauer theory. [ABSTRACT FROM AUTHOR]

A high-temperature stable solar absorber based on a metallic 2D photonic crystal (PhC) with high and tunable spectral selectivity is demonstrated and optimized for a range of operating temperatures and irradiances. In particular, a PhC absorber with solar absorptance [ABSTRACT FROM AUTHOR]

The most common approaches to generating power from sunlight are either photovoltaic, in which sunlight directly excites electron-hole pairs in a semiconductor, or solar-thermal, in which sunlight drives a mechanical heat engine. Photovoltaic power generation is intermittent and typically only exploits a portion of the solar spectrum efficiently, whereas the intrinsic irreversibilities of small heat engines make the solar-thermal approach best suited for utility-scale power plants. There is, therefore, an increasing need for hybrid technologies for solar power generation. By converting sunlight into thermal emission tuned to energies directly above the photovoltaic bandgap using a hot absorber-emitter, solar thermophotovoltaics promise to leverage the benefits of both approaches: high efficiency, by harnessing the entire solar spectrum; scalability and compactness, because of their solid-state nature; and dispatchablility, owing to the ability to store energy using thermal or chemical means. However, efficient collection of sunlight in the absorber and spectral control in the emitter are particularly challenging at high operating temperatures. This drawback has limited previous experimental demonstrations of this approach to conversion efficiencies around or below 1% (refs 9, 10, 11). Here, we report on a full solar thermophotovoltaic device, which, thanks to the nanophotonic properties of the absorber-emitter surface, reaches experimental efficiencies of 3.2%. The device integrates a multiwalled carbon nanotube absorber and a one-dimensional Si/SiO2 photonic-crystal emitter on the same substrate, with the absorber-emitter areas optimized to tune the energy balance of the device. Our device is planar and compact and could become a viable option for high-performance solar thermophotovoltaic energy conversion. [ABSTRACT FROM AUTHOR]

A correction to the article "A nanophotonic solar thermophotovoltaic device" that was published online in the January 19, 2014 issue is presented.