arXiv subjects

G. R. Stewart

Publications and source records attributed to G. R. Stewart.

At least 19 recordsLinked to original sources

arXiv2024

Superconductivity in WBe2

WBe2, which occurs in space group 194, with hexagonal symmetry P63/mmc, is prepared by arc-melting at temperatures above 2200 C, where Be vapor loss is significant. This study is motivated by recent work on MoB2 and WB2, both superconductors (Tc=32 and 17 K respectively) under high (~70 GPa) pressure. In order to avoid the known Be-rich superconducting phases (WBe13 and WBe22) in the complex phase diagram, both known to be superconducting at 4.1 K, the sample was prepared with a slight (~5%) excess of W. The resultant sample, prepared using high purity (99.999%) Be, is essentially single phase WBe2, with some spread in its superconducting properties due to the known homogeneity range. (WBe2 forms in space group 194 between approximately W1.02Be1.98 and W0.88Be2.12.) Characterization was carried out with x-ray diffraction, electrical resistivity, rho, in zero and applied magnetic fields, and specific heat. The resistivity in zero and applied fields and specific heat data indicate that our sample of WBe2 is a bulk superconductor at ambient pressure with a Tc(onset) in the resistivity at 1.05 K, and Tc(rho->0) at ~0.86 K. There is no signature of superconductivity in rho at 4.1 K, indicating successful avoidance of WBe13 and WBe22. The resistivity data in field indicate an upper critical field of approximately 400 gauss.

cond-mat.supr-con↗

arXiv2024

Superconductivity in pressurized Re$_{0.10}$Mo$_{0.90}$B$_2$

The recent surprising discovery of superconductivity with critical temperature $T_c$ = 32 K in MoB$_2$ above 70 GPa has led to the search for related materials that may superconduct at similarly high $T_c$ values and lower pressures. We have studied the superconducting and structural properties of Re$_{0.10}$Mo$_{0.90}$B$_2$ to 170 GPa. A structural phase transition from R3m to P6/mmm commences at 48 GPa, with the first signatures of superconductivity appearing above 44 GPa. The critical temperature is observed to increase with pressure. A complete resistive transition is observed only above 150 GPa, where the highest onset $T_c$ of 30 K is also achieved. Upon releasing pressure, the high pressure superconducting phase is found to be metastable. During unloading, a complete resistive superconducting transition is observed all the way down to 20 GPa (with onset $T_c \sim 20$ K). Our results suggest that the P6/mmm structure is responsible for the observed superconductivity.

cond-mat.supr-con↗

arXiv2024

Effect of low-temperature compression on superconductivity and crystal structure in strontium metal

The superconducting and structural properties of elemental strontium metal were investigated under pressures up to 60 GPa while maintaining cryogenic conditions during pressure application. Applying pressure at low temperatures reveals differences in superconducting and structural phases compared to previous reports obtained at room temperatures. Notably, the superconducting critical temperature exhibits a twofold increase under compression after cryogenic cooling within the pressure range of 35-42 GPa, compared to cryogenic cooling after room-temperature compression. Subsequently, the transition width becomes significantly sharper above 42 GPa. Low-temperature X-ray diffraction measurements under pressure reveal that this change corresponds to the Sr-III to Sr-IV transition, with no evidence of any metastable structure. Furthermore, the monoclinic Sr-IV structure was observed to remain stable to much higher pressures - at least up to 60 GPa, without the appearance of the incommensurate Sr-V phase present at room temperature. This implies that thermal activation energy plays an important role in overcoming the presence of a kinetic barrier to the Sr-V phase at room temperature.

cond-mat.supr-con↗

arXiv2023

Diboride compounds doped with transition metals$\unicode{x2013}$a route to superconductivity through structure stabilization as well as defects

Recent investigations into MoB$_{2}$ have unveiled a direct connection between a pressure-induced structural transition to a P6/mmm space group structure and the emergence of superconductivity, producing critical temperatures up to 32 K at 100 GPa. This pressure-induced superconducting state underscores the potential of doped MoB$_{2}$ as a possible candidate for metastable superconductivity at ambient pressure. In this work, we demonstrate that doping by Zr, Hf, or Ta stabilizes the P6/mmm structure at ambient pressure and results in the realization of a superconducting state with critical temperatures ranging from 2.4 up to 8.5 K depending on the specific doping. We estimate the electron-phonon coupling $λ$ and the density of states based on resistivity and specific heat data, finding that $λ$ ranges from 0.4 - 0.6 for these compounds. Finally, to investigate the role of possible metastable defect structures on the critical temperature, we analyze MoB$_{2}$, MoB$_{2.5}$, and Nb/Zr-doped MoB$_{2}$ using rapid cooling techniques. Notably, splat-quenching produces samples with higher critical temperatures and even retains superconductivity in MoB$_{2}$ at ambient pressure, achieving a critical temperature of 4.5 K.

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arXiv2023

Nb-substitution suppresses the superconducting critical temperature of pressurized MoB$_2$

A recent work has demonstrated that MoB$_2$, transforming to the same structure as MgB$_2$ ($P6/mmm$), superconducts at temperatures above 30 K near 100 GPa [C. Pei $et$ $al$. Natl. Sci. Rev., nwad034 (2023)], and Nb-substitution in MoB$_2$ stabilizes the $P6/mmm$ structure down to ambient pressure [A. C. Hire $et$ $al$. Phys. Rev. B 106, 174515 (2022)]. The current work explores the high pressure superconducting behavior of Nb-substituted MoB$_2$ (Nb$_{0.25}$Mo$_{0.75}$B$_2$). High pressure x-ray diffraction measurements show that the sample remains in the ambient pressure $P6/mmm$ structure to at least 160 GPa. Electrical resistivity measurements demonstrate that from an ambient pressure $T_c$ of 8 K (confirmed by specific heat to be a bulk effect), the critical temperature is suppressed to 4 K at 50 GPa, before gradually rising to 5.5 K at 170 GPa. The critical temperature at high pressure is thus significantly lower than that found in MoB$_2$ under pressure (30 K), revealing that Nb-substitution results in a strong suppression of the superconducting critical temperature. Our calculations indeed find a reduced electron-phonon coupling in Nb$_{0.25}$Mo$_{0.75}$B$_2$, but do not account fully for the observed suppression, which may also arise from inhomogeneity and enhanced spin fluctuations.

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arXiv2022

High critical field superconductivity at ambient pressure in MoB$_2$ stabilized in the P6/mmm structure via Nb substitution

Recently it was discovered that, under elevated pressures, MoB$_2$ exhibits superconductivity at a critical temperature, $T_c$, as high as 32 K. The superconductivity appears to develop following a pressure-induced structural transition from the ambient pressure R$\bar{3}$m structure to an MgB$_2$-like P6/mmm structure. This suggests that remarkably high $T_c$ values among diborides are not restricted to MgB$_2$ as previously appeared to be the case, and that similarly high $T_c$ values may occur in other diborides if they can be coerced into the MgB$_2$ structure. In this paper, we show that density functional theory calculations indicate that phonon free energy stabilizes the P6/mmm structure over the R$\bar{3}$m at high temperatures across the Nb$_{1-x}$Mo$_x$B$_2$ series. X-ray diffraction confirms that the synthesized Nb-substituted MoB$_2$ adopts the MgB$_2$ crystal structure. High magnetic field electrical resistivity measurements and specific heat measurements demonstrate that Nb$_{1-x}$Mo$_x$B$_2$ exhibits superconductivity with $T_c$ as high as 8 K and critical fields approaching 6 T.

cond-mat.supr-con↗

arXiv2022

Creating superconductivity in WB2 through pressure-induced metastable planar defects

High-pressure electrical resistivity measurements reveal that the mechanical deformation of ultra-hard WB2 during compression induces superconductivity above 50 GPa with a maximum superconducting critical temperature, Tc of 17 K at 90 GPa. Upon further compression up to 190 GPa, the Tc gradually decreases. Theoretical calculations show that electron-phonon mediated superconductivity originates from the formation of metastable stacking faults and twin boundaries that exhibit a local structure resembling MgB2} (hP3, space group 191, prototype AlB2). Synchrotron x-ray diffraction measurements up to 145 GPa} show that the ambient pressure hP12 structure (space group 194, prototype WB2) continues to persist to this pressure, consistent with the formation of the planar defects above 50 GPa. The abrupt appearance of superconductivity under pressure does not coincide with a structural transition but instead with the formation and percolation of mechanically-induced stacking faults and twin boundaries. The results identify an alternate route for designing superconducting materials.

cond-mat.supr-con↗

arXiv2021

Machine learning of superconducting critical temperature from Eliashberg theory

The Eliashberg theory of superconductivity accounts for the fundamental physics of conventional electron-phonon superconductors, including the retardation of the interaction and the effect of the Coulomb pseudopotential, to predict the critical temperature $T_c$ and other properties. McMillan, Allen, and Dynes derived approximate closed-form expressions for the critical temperature predicted by this theory, which depends essentially on the electron-phonon spectral function $α^2F(ω)$, using $α^2F$ for low-$T_c$ superconductors. Here we show that modern machine learning techniques can substantially improve these formulae, accounting for more general shapes of the $α^2F$ function. Using symbolic regression and the sure independence screening and sparsifying operator (SISSO) framework, together with a database of artificially generated $α^2F$ functions, ranging from multimodal Einstein-like models to calculated spectra of polyhydrides, as well as numerical solutions of the Eliashberg equations, we derive a formula for $T_c$ that performs as well as Allen-Dynes for low-$T_c$ superconductors, and substantially better for higher-$T_c$ ones. The expression identified through our data-driven approach corrects the systematic underestimation of $T_c$ while reproducing the physical constraints originally outlined by Allen and Dynes. This equation should replace the Allen-Dynes formula for the prediction of higher-temperature superconductors and for the estimation of $λ$ from experimental data.

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arXiv2021

A15 Nb$_3$Si -- A "high" Tc superconductor synthesized at a pressure of one megabar and metastable at ambient conditions

A15 Nb$_3$Si is, until now, the only high temperature superconductor produced at high pressure (~110 GPa) that has been successfully brought back to room pressure conditions in a metastable condition. Based on the current great interest in trying to create metastable-at-room-pressure high temperature superconductors produced at high pressure, we have restudied explosively compressed A15 Nb$_3$Si and its production from tetragonal Nb$_3$Si. First, diamond anvil cell pressure measurements up to 88 GPa were performed on explosively compressed A15 Nb$_3$Si material to trace Tc as a function of pressure. Tc is suppressed to ~ 5.2 K at 88 GPa. Then, using these Tc (P) data for A15 Nb$_3$Si, pressures up to 92 GPa were applied at room temperature (which increased to 120 GPa at 5 K) on tetragonal Nb$_3$Si. Measurements of the resistivity gave no indication of any A15 structure production, i.e., no indications of the superconductivity characteristic of A15 Nb$_3$Si. This is in contrast to the explosive compression (up to P~110 GPa) of tetragonal Nb$_3$Si, which produced 50-70% A15 material, Tc = 18 K at ambient pressure, in a 1981 Los Alamos National Laboratory experiment. Our theoretical calculations show that A15 Nb$_3$Si has an enthalpy vs the tetragonal structure that is 0.07 eV/atom smaller at 100 GPa, implying that the accompanying high temperature (1000 deg C) caused by explosive compression is necessary to successfully drive the reaction kinetics of the tetragonal -> A15 Nb$_3$Si structural transformation. Annealing experiments on the A15 explosively compressed material reaching time scales of 39 years are consistent with this viewpoint.

cond-mat.supr-con↗

arXiv2021

Towards high-throughput superconductor discovery via machine learning

Even though superconductivity has been studied intensively for more than a century, the vast majority of superconductivity research today is carried out in nearly the same manner as decades ago. That is, each study tends to focus on only a single material or small subset of materials, and discoveries are made more or less serendipitously. Recent increases in computing power, novel machine learning algorithms, and improved experimental capabilities offer new opportunities to revolutionize superconductor discovery. These will enable the rapid prediction of structures and properties of novel materials in an automated, high-throughput fashion and the efficient experimental testing of these predictions. Here, we review efforts to use machine learning to attain this goal.

cond-mat.supr-con↗

arXiv2021

High pressure study of low-Z superconductor Be$_{22}$Re

With $T_c \sim 9.6~\mathrm{K}$, Be$_{22}$Re exhibits one of the highest critical temperatures among Be-rich compounds. We have carried out a series of high-pressure electrical resistivity measurements on this compound to 30 GPa. The data show that the critical temperature $T_c$ is suppressed gradually at a rate of $dT_c/dP = -0.05~\mathrm{K/GPa}$. Using density functional theory (DFT) calculations of the electronic and phonon density of states (DOS) and the measured critical temperature, we estimate that the rapid increase in lattice stiffening in Be$_{22}$Re overwhelms a moderate increase in the electron-ion interaction with pressure, resulting in the decrease in $T_c$. High pressure x-ray diffraction measurements show that the ambient pressure crystal structure of Be$_{22}$Re persists to at least 154 GPa. We discuss the relationship between low-Z Be-rich superconductors and the high-$T_c$ superhydrides.

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arXiv2020

Remarkable low-energy properties of the pseudogapped semimetal Be$_5$Pt

We report measurements and calculations on the properties of the intermetallic compound Be$_5$Pt. High-quality polycrystalline samples show a nearly constant temperature dependence of the electrical resistivity over a wide temperature range. On the other hand, relativistic electronic structure calculations indicate the existence of a narrow pseudogap in the density of states arising from accidental approximate Dirac cones extremely close to the Fermi level. A small true gap of order 3 meV is present at the Fermi level, yet the measured resistivity is nearly constant from low to room temperature. We argue that this unexpected behavior can be understood by a cancellation of the energy dependence of density of states and relaxation time due to disorder, and discuss a model for electronic transport. With applied pressure, the resistivity becomes semiconducting, consistent with theoretical calculations that show that the band gap increases with applied pressure. We further discuss the role of Be inclusions in the samples.

cond-mat.mtrl-sci↗

arXiv2020

Stabilization of antiferromagnetism in 1T-Fe$_{0.05}$TaS$_2$

1T-TaS$_2$ is a prototypical charge-density-wave (CDW) system with a Mott insulating ground state. Usually, a Mott insulator is accompanied by an antiferromagnetic state. However, the antiferromagnetic order had never been observed in 1T-TaS$_2$. Here, we report the stabilization of the antiferromagnetic order by the intercalation of a small amount of Fe into the van der Waals gap of 1T-TaS$_2$, i.e. forming 1T-Fe$_{0.05}$TaS$_2$. Upon cooling from 300~K, the electrical resistivity increases with a decreasing temperature before reaching a maximum value at around 15~K, which is close to the Neel temperature determined from our magnetic susceptibility measurement. The antiferromagnetic state can be fully suppressed when the sample thickness is reduced, indicating that the antiferromagnetic order in Fe$_{0.05}$TaS$_2$ has a non-negligible three-dimensional character. For the bulk Fe$_{0.05}$TaS$_2$, a comparison of our high pressure electrical transport data with that of 1T-TaS$_2$ indicates that, at ambient pressure, Fe$_{0.05}$TaS$_2$ is in the nearly commensurate charge-density-wave (NCCDW) phase near the border of the Mott insulating state. The temperature-pressure phase diagram thus reveals an interesting decoupling of the antiferromagnetism from the Mott insulating state.

cond-mat.str-el↗

arXiv2019

A Class of Compounds Featuring Frustrated Triangular Magnetic Lattice CsRESe$_2$ (RE=La-Lu): Quantum Spin-Liquid Candidates

A triangular lattice selenide series of rare earth (RE), CsRESe2, were synthesized as large single crystals using a flux growth method. This series stabilized in either trigonal (R-3m) or hexagonal (P63/mmc) crystal systems. Physical properties of CsRESe2 were explored by magnetic susceptibility and heat capacity measurements down to 0.4 K. Antiferromagnetic interaction was observed in all magnetic compounds, while no long-range magnetic order was found, indicating the frustrated magnetism. CsDySe2 presents spin freezing at 0.7 K, revealing a spin-glass state. CsCeSe2 and CsYbSe2 present broad peaks at 0.7 K and 1.5 K in the magnetization, respectively, suggesting the short-range interactions between magnetic rare earth ions. The lack of signature for long-range magnetic order and spin freezing down to 0.4 K in these compounds (RE = Ce, Yb) implies their candidacy for quantum spin liquid state.

cond-mat.mtrl-sci↗

arXiv2019

Field-induced magnetic transition and spin fluctuation in quantum spin liquid candidate CsYbSe$_2$

Two-dimensional triangular-lattice materials with spin-1/2 are perfect platforms for investigating quantum frustrated physics with spin fluctuations. Here we report the structure, magnetization, heat capacity and inelastic neutron scattering (INS) results on cesium ytterbium diselenide, CsYbSe$_2$. There is no long-range magnetic order down to 0.4 K at zero field. The temperature dependent magnetization, $M(T)$, reveals an easy-plane magnetic anisotropy. A maximum is found in $M(T)$ around \emph{T}$\sim$1.5 K when magnetic field $H$ is applied in the $ab$ plane, indicating the short-range interaction. The low-temperature isothermal magnetization $M(H)$ shows a one-third plateau of the estimated saturation moment, that is characteristic of a two-dimensional frustrated triangular lattice. Heat capacity shows field-induced long-range magnetic order for both $H||c$ and $H||ab$ directions. The broad peak in heat capacity and highly damped INS magnetic excitation at $T$=2 K suggests strong spin fluctuations. The dispersive in-plane INS, centered at the (1/3 1/3 0) point, and the absence of dispersion along $c$ direction suggests 120$^{\circ}$ non-collinear 2D-like spin correlations. All these results indicate that the two-dimensional frustrated material CsYbSe$_2$ can be in proximity to the triangular-lattice quantum spin liquid. We propose an experimental low-temperature $H$-$T$ phase diagram for CsYbSe$_2$.

cond-mat.str-el↗

arXiv2019

Synthesis, magnetization and heat capacity of triangular lattice materials NaErSe$_2$ and KErSe$_2$

In this paper we report the synthesis, magnetization and heat capacity of the frustrated magnets \emph{A}ErSe$_2$(\emph{A}=Na,K) which contain perfect triangular lattices of Er$^{3+}$. The magnetization data suggests no long-range magnetic order exists in \emph{A}ErSe$_2$(\emph{A}=Na,K), which is consistent with the heat capacity measurements. Large anisotropy is observed between the magnetization within the \emph{ab} plane and along the \emph{c} axis of both compounds. When the magnetic field is applied along \emph{ab} plane, anomalies are observed at 1.8 $μ_B$ in NaErSe$_2$ at 0.2 T and 2.1 $μ_B$ in KErSe$_2$ at 0.18 T. Unlike NaErSe$_2$, a plateau-like field-induced metamagnetic transition is observed for H$\|$\emph{c} below 1 K in KErSe$_2$. Two broad peaks are observed in the heat capacity below 10 K indicating possible crystal electric field(CEF) effects and magnetic entropy released under different magnetic fields. All results indicate that \emph{A}ErSe$_2$ are strongly anisotropic, frustrated magnets with field-induced transition at low temperature. The lack of signatures for long-range magnetic order implies that these materials are candidates for hosting a quantum spin liquid ground state.

cond-mat.mtrl-sci↗

arXiv2019

Unconventional critical behavior in quasi-one-dimensional $S$ = 1 chain NiTe$_{2}$O$_{5}$

Here we report a new quasi-one-dimensional $S$ = 1 chain compound NiTe$_{2}$O$_{5}$. From the comprehensive study of the structure and magnetic properties on high quality single crystalline NiTe$_{2}$O$_{5}$, it's revealed that NiTe$_{2}$O$_{5}$ undergoes a transition into an intriguing long-range antiferromagnetic order at $T_{\rm N}=30.5 {\rm K}$, in which longitudinal magnetic moments along the chain direction are ferromagnetically ordered, while their transverse components have an alternating ferromagnetic-antiferromagnetic coupling. Even though the temperature dependence of magnetic susceptibility represents an archetypal anisotropic antiferromagnetic order, we found that critical behavior of unconventional nature with $α'\sim0.25$ and $β\sim0.18$ is accompanied by the temperature evolution of the antiferromagnetic order parameter.

cond-mat.str-el↗

arXiv2019

Superconductivity in a unique type of copper oxide

The mechanism of superconductivity in cuprates remains one of the big challenges of condensed matter physics.High Tc cuprates crystallize into layered perovskite structure featuring copper oxygen octahedral coordination. Due to the Jahn Teller effect in combination with the strong static Coulomb interaction, the octahedra in high Tc cuprates are elongated along the c axis, leading to a 3dx2-y2 orbital at the top of the band structure wherein the doped holes reside.This scenario gives rise to two dimensional characteristics in high Tc cuprates that favor d wave pairing symmetry. Here we report superconductivity in a cuprate Ba2CuO4-y wherein the local octahedron is in a very exceptional compressed version.The Ba2CuO4-y compound was synthesized at high pressure at high temperatures, and shows bulk superconductivity with critical temperature Tc above 70 K at ambient conditions. This superconducting transition temperature is more than 30 K higher than the Tc for the isostructural counterparts based on classical La2CuO4. X-ray absorption measurements indicate the heavily doped nature of the Ba2CuO4-y superconductor. In compressed octahedron the 3d3z2-r2 orbital will be lifted above the 3dx2-y2 orbital, leading to significant three dimensional nature in addition to the conventional 3dx2-y2 orbital. This work sheds important new light on advancing our comprehensive understanding of the superconducting mechanism of high Tc in cuprate materials.

cond-mat.supr-con↗