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1. Stabilizing Ti ₃ C ₂ T _x MXene flakes in air by removing confined water

   https://doi.org/10.1073/pnas.2400084121  

   Fang, Hui; Thakur, Anupma; Zahmatkeshsaredorahi, Amirhossein; Fang, Zhenyao; Rad, Vahid; Shamsabadi, Ahmad A; Pereyra, Claudia; Soroush, Masoud; Rappe, Andrew M; Xu, Xiaoji G; et al (July 2024, Proceedings of the National Academy of Sciences)

   MXenes have demonstrated potential for various applications owing to their tunable surface chemistry and metallic conductivity. However, high temperatures can accelerate MXene film oxidation in air. Understanding the mechanisms of MXene oxidation at elevated temperatures, which is still limited, is critical in improving their thermal stability for high-temperature applications. Here, we demonstrate that Ti ${}_3$C ${}_2$T ${}_x$MXene monoflakes have exceptional thermal stability at temperatures up to 600 ${}^{°}$C in air, while multiflakes readily oxidize in air at 300 ${}^{°}$C. Density functional theory calculations indicate that confined water between Ti ${}_3$C ${}_2$T ${}_x$flakes has higher removal energy than surface water and can thus persist to higher temperatures, leading to oxidation. We demonstrate that the amount of confined water correlates with the degree of oxidation in stacked flakes. Confined water can be fully removed by vacuum annealing Ti ${}_3$C ${}_2$T ${}_x$films at 600 ${}^{°}$C, resulting in substantial stability improvement in multiflake films (can withstand 600 ${}^{°}$C in air). These findings provide fundamental insights into the kinetics of confined water and its role in Ti ${}_3$C ${}_2$T ${}_x$oxidation. This work enables the use of stable monoflake MXenes in high-temperature applications and provides guidelines for proper vacuum annealing of multiflake films to enhance their stability. 

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2. Designing multicomponent hydrides with potential high T _c superconductivity

   https://doi.org/10.1073/pnas.2413096121  

   Denchfield, Adam; Park, Hyowon; Hemley, Russell J (November 2024, Proceedings of the National Academy of Sciences)

   While hydrogen-rich materials have been demonstrated to exhibit high T_csuperconductivity at high pressures, there is an ongoing search for ternary, quaternary, and more chemically complex hydrides that achieve such high critical temperatures at much lower pressures. First-principles searches are impeded by the computational complexity of solving the Eliashberg equations for large, complex crystal structures. Here, we adopt a simplified approach using electronic indicators previously established to be correlated with superconductivity in hydrides. This is used to study complex hydride structures, which are predicted to exhibit promisingly high critical temperatures for superconductivity. In particular, we propose three classes of hydrides inspired by the Fm $\overline{3}$m RH ${}_3$structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH ${}_{11}$X ${}_3$Y] is based on a Pm $\overline{3}$m structure showing moderately high T_c, where the T_cestimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH ${}_{11}$) ${}_2$X ${}_6$YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing T_c. The third class [(R ${}^1$H ${}_{11}$)(R ${}^2$H ${}_{11}$)X ${}_6$YZ] improves the strong hydrogen network connectivity by introducing anisotropy in the hydrogen network through a specific doping pattern. These design principles and associated model structures provide flexibility to optimize both T_cand the structural stability of complex hydrides. 

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3. ‘Golden Ratio Yoshimura’ for meta-stable and massively reconfigurable deployment

   https://doi.org/10.1098/rsta.2024.0009  

   Deshpande, Vishrut; Phalak, Yogesh; Zhou, Ziyang; Walker, Ian; Li, Suyi (October 2024, Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences)

   Yoshimura origami is a classical folding pattern that has inspired many deployable structure designs. Its applications span from space exploration, kinetic architectures and soft robots to even everyday household items. However, despite its wide usage, Yoshimura has been fixated on a set of design constraints to ensure its flat foldability. Through extensive kinematic analysis and prototype tests, this study presents a new Yoshimura that intentionally defies these constraints. Remarkably, one can impart a unique meta-stability by using the Golden Ratio angle ( ${\cot }^{-1}1.618\approx {31.72}^{\circ }$) to define the triangular facets of a generalized Yoshimura (with $n=3$, where $n$is the number of rhombi shapes along its cylindrical circumference). As a result, when its facets are strategically popped out, a ‘Golden Ratio Yoshimura’ boom with $m$modules can be theoretically reconfigured into $8^m$geometrically unique and load-bearing shapes. This result not only challenges the existing design norms but also opens up a new avenue to create deployable and versatile structural systems. This article is part of the theme issue ‘Origami/Kirigami-inspired structures: from fundamentals to applications’. 

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4. The metastable Q ³ Δ ₂ state of ThO: a new resource for the ACME electron EDM search

   https://doi.org/10.1088/1367-2630/ab6a3a  

   Wu, X.; Han, Z.; Chow, J.; Ang, D. G.; Meisenhelder, C.; Panda, C. D.; West, E. P.; Gabrielse, G.; Doyle, J. M.; DeMille, D. (February 2020, New Journal of Physics)

   Abstract The best upper limit for the electron electric dipole moment was recently set by the ACME collaboration. This experiment measures an electron spin-precession in a cold beam of ThO molecules in their metastable $H{(}^3{\mathrm{\Delta }}_1)$state. Improvement in the statistical and systematic uncertainties is possible with more efficient use of molecules from the source and better magnetometry in the experiment, respectively. Here, we report measurements of several relevant properties of the long-lived $Q{(}^3{\mathrm{\Delta }}_2)$state of ThO, and show that this state is a very useful resource for both these purposes. TheQstate lifetime is long enough that its decay during the time of flight in the ACME beam experiment is negligible. The large electric dipole moment measured for theQstate, giving rise to a large linear Stark shift, is ideal for an electrostatic lens that increases the fraction of molecules detected downstream. The measured magnetic moment of theQstate is also large enough to be used as a sensitive co-magnetometer in ACME. Finally, we show that theQstate has a large transition dipole moment to the $C{(}^1{\mathrm{\Pi }}_1)$state, which allows for efficient population transfer between the ground state $X{(}^1{\mathrm{\Sigma }}^{+})$and theQstate via $X-C-Q$Stimulated Raman Adiabatic Passage (STIRAP). We demonstrate 90 % STIRAP transfer efficiency. In the course of these measurements, we also determine the magnetic moment ofCstate, the $X\to C$transition dipole moment, and branching ratios of decays from theCstate. 

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5. Structural phase purification of bulk HfO ₂ :Y through pressure cycling

   https://doi.org/10.1073/pnas.2312571121  

   Musfeldt, J. L.; Singh, Sobhit; Fan, Shiyu; Gu, Yanhong; Xu, Xianghan; Cheong, S.-W.; Liu, Z.; Vanderbilt, David; Rabe, Karin M. (January 2024, Proceedings of the National Academy of Sciences)

   We combine synchrotron-based infrared absorption and Raman scattering spectroscopies with diamond anvil cell techniques and first-principles calculations to explore the properties of hafnia under compression. We find that pressure drives HfO ${}_2$:7%Y from the mixed monoclinic ( $P{2}_1/c$) $+$antipolar orthorhombic ( $\mathit{Pbca}$) phase to pure antipolar orthorhombic ( $\mathit{Pbca}$) phase at approximately 6.3 GPa. This transformation is irreversible, meaning that upon release, the material is kinetically trapped in the $\mathit{Pbca}$metastable state at 300 K. Compression also drives polar orthorhombic ( $Pca{2}_1$) hafnia into the tetragonal ( $P{4}_2/nmc$) phase, although the latter is not metastable upon release. These results are unified by an analysis of the energy landscape. The fact that pressure allows us to stabilize targeted metastable structures with less Y stabilizer is important to preserving the flat phonon band physics of pure HfO ${}_2$. 

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