More Like this

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. 

   more » « less
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. 

   more » « less
3. Rapid shear zone weakening during subduction initiation

   https://doi.org/10.1073/pnas.2404939121  

   Li, Yida; Gurnis, Michael (October 2024, Proceedings of the National Academy of Sciences)

   Subduction zones play a pivotal role in the mechanics of plate tectonics by providing the driving force through slab pull and weak megathrusts that facilitate the relative motion between tectonic plates. The initiation of subduction zones is intricately linked to the accumulation of slab pull and development of weakness at plate boundaries and, by consequence, the largest changes in the energetics of mantle convection. However, the transient nature of subduction initiation accompanied by intense subsequent tectonic activity, leaves critical evidence poorly preserved and making subduction initiation difficult to constrain. We overcome these limitations through a comprehensive analysis focused on Puysegur, a well-constrained extant example of subduction initiation offshore South Island, New Zealand. Through time-dependent, three-dimensional thermo-mechanical computations and quantitative comparison to new geophysical and geological observations, including topography, stratigraphy, and seismicity, we demonstrate that subduction initiation develops with a fast strain weakening described with a small characteristic displacement ( ${\mathrm{\Delta }}_s\approx$4 to 8 km). Potential physical mechanisms contributing to the strain weakening are explored and we find that the observed fast weakening may arise through a combination of grain-size reduction within the lower lithosphere and fluid pressurization at shallower depths. With the shared commonality in the underlying physics of tectonic processes, the rapid strain weakening constrained at Puysegur offers insights into the formation of the first subduction during early Earth and the onset of plate tectonics. 

   more » « less
4. Three-dimensional 0–10 Hz physics-based simulations of the 2020 Magna, Utah, earthquake sequence

   https://doi.org/10.1177/87552930241307797  

   Xu, Ke; Olsen, Kim Bak; Yeh, Te-Yang (May 2025, Earthquake Spectra)

   Earthquakes on the Salt Lake City Segment of the Wasatch fault (WFSLC) represent the most significant seismic hazard to the Salt Lake Valley, populated by 1 million+ people. The 2020 Magna, UT, earthquake, which likely occurred on the WFSLC, generated peak ground accelerations (PGAs) as large as 0.55 gin the Salt Lake Valley. Here, we present three-dimensional (3D) physics-based wave propagation simulations of the Magna earthquake sequence in the Wasatch Front Community Velocity Model (WFCVM) up to 10 Hz to better constrain both linear and nonlinear parameters in the soils of the Salt Lake Valley. We first calibrate the WFCVM via linear simulations of a $M_w$4.59 Magna aftershock, obtaining the best fit between the recordings and synthetics, including a statistical distribution of small-scale heterogeneities with 10% standard deviation and $Q_S=0.05V_S$for frequencies $<1$ Hz and $Q_S=0.05V_S{f}^{0.4}$for frequencies $>1$ Hz ( $V_s$in m/s). Spectral ratios from our simulations of the 2020 Magna mainshock using a finite-fault source model generally overestimate those for the recordings in the linear regime at higher frequencies, in particular at stations with the largest PGAs, suggesting the presence of nonlinear soil effects. Using a fully hysteretic multi-yield-surface 3D nonlinear modeling approach, we find that damping from the reference strain–depth relations proposed by Darendeli significantly reduces the bias in terms of spectral amplification ratios at stations with the shortest epicentral distances. We find an optimal fit between the recordings and nonlinear synthetics for reference strains at about 2 standard deviations below Darendeli’s relations, with reduction of the spectral amplification bias by more than a factor of two. Our findings suggest significant nonlinear soil effects in the Salt Lake Valley and provide a basis for improved seismic hazard analysis of the greater Salt Lake City region. 

   more » « less
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 ${}_2$. 

   more » « less