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            A new series of 20-component fluorite-based compositionally complex oxides (20CCFBOxNb/Ta) with the general chemical formula (15RE1/15)2x+1(Ce1/3Zr1/3Hf1/3)3-3x(Nb1/2Ta1/2)xO8-delta (0 <= x <= 1, where 15RE1/15 = La1/15Pr1/15Nd1/15Sm1/15Eu1/15Gd1/15Tb1/15Dy1/15Y1/15Ho1/15Er1/15Tm1/15Yb1/15Lu1/15Sc1/15) are synthesized. Despite that the Gibbs phase rule allows for the existence of up to 20 phases at the thermodynamic equilibrium, 17 of the 20CCFBOxNb/Ta compositions synthesized in this study all possess single ultrahigh-entropy phases in fluorite, pyrochlore, or weberite structure, as shown by X-ray diffraction (XRD). Only < 1 vol.% of secondary phases are observed in two compositions near the phase-transition points. With changing compositional variable x, this series of 20CCFBOxNb/Ta undergoes an abrupt fluorite-pyrochlore transition at x = ~0.27 and an abrupt pyrochlore-weberite transition at x = ~0.87. Careful characterization reveals abrupt changes of order parameters at both phase transitions. In addition, weberite short-range ordering can persist into the long-range pyrochlore phase, which leads to the lowest thermal conductivities.more » « less
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            Abstract Heat conduction in solids is typically governed by the Fourier’s law describing a diffusion process due to the short wavelength and mean free path for phonons and electrons. Surface phonon polaritons couple thermal photons and optical phonons at the surface of polar dielectrics, possessing much longer wavelength and propagation length, representing an excellent candidate to support extraordinary heat transfer. Here, we realize clear observation of thermal conductivity mediated by surface phonon polaritons in SiO2nanoribbon waveguides of 20-50 nm thick and 1-10 μm wide and also show non-Fourier behavior in over 50-100 μm distance at room and high temperature. This is enabled by rational design of the waveguide to control the mode size of the surface phonon polaritons and its efficient coupling to thermal reservoirs. Our work laid the foundation for manipulating heat conduction beyond the traditional limit via surface phonon polaritons waves in solids.more » « less
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            Abstract Two new high-entropy ceramics (HECs) in the weberite and fergusonite structures, along with the unexpected formation of ordered pyrochlore phases with ultrahigh-entropy compositions and an abrupt pyrochlore-weberite transition, are discovered in a 21-component oxide system. While the Gibbs phase rule allows 21 equilibrium phases, 9 out of the 13 compositions examined possess single HEC phases (with ultrahigh ideal configurational entropies: ∼2.7 k B per cation or higher on one sublattice in most cases). Notably, (15RE 1/15 )(Nb 1/2 Ta 1/2 )O 4 possess a single monoclinic fergusonite (C2/ c ) phase, and (15RE 1/15 ) 3 (Nb 1/2 Ta 1/2 ) 1 O 7 form a single orthorhombic (C222 1 ) weberite phase, where 15RE 1/15 represents Sc 1/15 Y 1/15 La 1/15 Pr 1/15 Nd 1/15 Sm 1/15 Eu 1/15 Gd 1/15 Tb 1/15 Dy 1/15 Ho 1/15 Er 1/15 Tm 1/15 Yb 1/15 Lu 1/15 . Moreover, a series of eight (15RE 1/15 ) 2+ x (Ti 1/4 Zr 1/4 Ce 1/4 H 1/4 ) 2−2 x (Nb 1/2 Ta 1/2 ) x O 7 specimens all exhibit single phases, where a pyrochlore-weberite transition occurs within 0.75 < x < 0.8125. This cubic-to-orthorhombic transition does not change the temperature-dependent thermal conductivity appreciably, as the amorphous limit may have already been achieved in the ultrahigh-entropy 21-component oxides. These discoveries expand the diversity and complexity of HECs, towards many-component compositionally complex ceramics (CCCs) and ultrahigh-entropy ceramics.more » « less
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            Abstract Radiative cooling has been recently intensively explored for thermal management and enhancing energy efficiency. Yet, traditional materials with singular emissivity fall short in dynamic thermal management, highlighting the need for materials that can adjust their thermal radiation in real time. Active modulation methods, requiring external stimuli such as mechanical stretch, electric potential, or humidity change, offer adaptability but can increase energy use and complexity. Passive approaches, using materials' inherent thermal‐responsive properties, face manufacturing and scalability challenges. Here, a scalable yet effective passive approach is introduced for adaptive thermal modulation based on gold (Au) and liquid crystal elastomer (LCE) with a reversible response to environmental temperature changes. This modulator enables a “low thermal resistance” state through actuation‐induced microcracks that expose a high‐emissivity polymer substrate, and a “high thermal resistance” state by closing these microcracks and forming a high thermal resistance air gap between the modulator and the target object. The flexible design and fixed external dimensions of the Au‐LCE thermal modulator make it adaptable to various surface geometries. Furthermore, by adjusting the LCE's chemical composition, the modulator's transition temperature can be tailored, broadening its applications from enhancing building energy efficiency to improving clothing thermal comfort.more » « less
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