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We report a comprehensive study of Sperrylite (PtAs2), the main platinum source in natural minerals, as a function of applied pressures up to 150 GPa. While no structural phase transition was detected from pressure-dependent X-ray measurements, the unit cell volume shrinks monotonically with pressure following the third-order Birch-Murnaghan equation of state. The mildly semiconducting behavior found in pure synthesized crystals at ambient pressures becomes more insulating upon increasing applied pressure before metalizing at higher pressures, giving way to the appearance of an abrupt decrease in resistance near 3 K at pressures above 92 GPa consistent with the onset of a superconducing phase. The pressure evolution of the calculated electronic band structure reveals the same physical trend as our transport measurements, with a non-monotonic evolution explained by a hole band that is pushed below the Fermi energy and an electron band that approaches it as a function of pressure, both reaching a touching point suggestive of an excitonic state. A topological Lifshitz transition of the electronic structure and an increase in the density of states may naturally explain the onset of superconductivity in this material, Comment: 7 pages, 7 figures

We have studied the effects of phonon-boundary scattering on the thermal transport in topological Kondo insulator, SmB$_6$. The studies have been performed by using the $3\omega$ method in the temperature range 300K - 3K. We show that the observed thermal conductivity of micro-size SmB$_6$ is of the order of magnitude smaller than for a bulk single-crystal. Using the Callaway model we analyzed the low-temperature lattice thermal conductivity of the micro crystal and show that phonon scattering by sample boundaries plays a major role in the thermal resistance in this topological material. In addition, we show that the temperature dependence of the lattice thermal conductivity shows a double peak structure that suggests complex phonon-phonon or phonon-defects interactions in SmB$_6$. These findings provide guidance for the understanding of the thermal transport of advanced materials and devices at a micro-scale., Comment: 5 pages including references, 3 figures

Density Functional Tight Binding (DFTB) is an attractive method for accelerated quantum simulations of condensed matter due to its enhanced computational efficiency over standard Density Functional Theory approaches. However, DFTB models can be challenging to determine for individual systems of interest, especially for metallic and interfacial systems where different bonding arrangements can lead to significant changes in electronic states. In this regard, we have created a rapid-screening approach for determining systematically improvable DFTB interaction potentials that can yield transferable models for a variety of conditions. Our method leverages a recent reactive molecular dynamics force field where many-body interactions are represented by linear combinations of Chebyshev polynomials. This allows for the efficient creation of multi-center representations with relative ease, requiring only a small investment in initial DFT calculations. We have focused our workflow on TiH$_2$ as a model system and show that a relatively small training set based on unit-cell sized calculations yields a model accurate for both bulk and surface properties. Our approach is easy to implement and can yield accurate DFTB models over a broad range of thermodynamic conditions, where physical and chemical properties can be difficult to interrogate directly and there is historically a significant reliance on theoretical approaches for interpretation and validation of experimental results., Comment: 45 pages, 7 tables, 7 figures. New version contains updated figures and light editorial changes. This version has been submitted as a revision to J Chem. Theory Comput

Solid state ionic approaches for modifying ion distributions in getter/oxide heterostructures offer exciting potentials to control material properties. Here we report a simple, scalable approach allowing for total control of the superconducting transition in optimally doped YBa$_{2}$Cu$_{3}$O$_{7-{\delta}}$ (YBCO) films via a chemically-driven ionic migration mechanism. Using a thin Gd capping layer of up to 20 nm deposited onto 100 nm thick epitaxial YBCO films, oxygen is found to leach from deep within the YBCO. Progressive reduction of the superconducting transition is observed, with complete suppression possible for a sufficiently thick Gd layer. These effects arise from the combined impact of redox-driven electron doping and modification of the YBCO microstructure due to oxygen migration and depletion. This work demonstrates an effective ionic control of superconductivity in oxides, an interface induced effect that goes well into the quasi-bulk regime, opening up possibilities for electric field manipulation., Comment: 26 pages, 5 figures

We report the results of high pressure x-ray diffraction, x-ray absorption, and electrical transport measurements of Kondo insulator Ce$_3$Bi$_4$Pt$_3$ up to 42 GPa, the highest pressure reached in the study of any Ce-based KI. We observe a smooth decrease in volume and movement toward intermediate Ce valence with pressure, both of which point to increased electron correlations. Despite this, temperature-dependent resistance data show the suppression of the interaction-driven ambient pressure insulating ground state. We also discuss potential ramifications of these results for the predicted topological KI state., Comment: 8 pages, 5 figures

We report the observation of the pressure-induced, fully-collapsed tetragonal phase of CaRbFe4As4 for P~ 22 GPa via high-pressure x-ray diffraction and magnetotransport measurements. The x-ray measurements, along with resistivity measurements, show that there is an initial half-collapsed tetragonal phase for 6 < P < 22 GPa, in which superconductivity is continuously suppressed from Tc= 35K at P= 3.1 GPa to Tc <2K for P >17.2 GPa, as well as signs of the fully-collapsed tetragonal phase near P=22 GPa. Density functional calculations suggest that both of these transitions are driven by increased As-As bonding, first across the Ca layer, and then at the second transition, across the Rb layer. Although electrical resistivity measurements in the fully-collapsed tetragonal phase do not show superconductivity, there is a change in the slope of both the Hall coefficient and the longitudinal resistance near 22 GPa, suggesting a strong correlation between the electronic and lattice degrees of freedom in this new iron-based superconductor., Comment: 21 pages, 6 figures

In pulsed magnetic fields up to 65T and at temperatures below the N\'eel transition, our magnetization and magnetostriction measurements reveal a field-induced metamagnetic-like transition that is suggestive of an antiferromagnetic to polarized paramagnetic or ferrimagnetic ordering. Our data also suggests a change in the nature of this metamagnetic-like transition from second- to first-order-like near a tricritical point at T_{tc} ~145K and H_{c}~52T. At high fields for H>H_{c} we found a decreased magnetic moment roughly half of the moment reported in low field measurements. We propose that \mathit{f-p} hybridization effects and magnetoelastic interactions drive the decreased moment, lack of saturation at high fields, and the decreased phase boundary., Comment: 19 pages, 10 figures

Resonant x-ray emission spectroscopy (RXES) was used to determine the pressure dependence of the f-electron occupancy in the Kondo insulator SmB6. Applied pressure reduces the f-occupancy, but surprisingly, the material maintains a significant divalent character up to a pressure of at least 35 GPa. Thus, the closure of the resistive activation energy gap and onset of magnetic order are not driven by stabilization of an integer valent state. Over the entire pressure range, the material maintains a remarkably stable intermediate valence that can in principle support a nontrivial band structure.

We have performed the first high-pressure magnetotransport and x-ray diffraction measurements on ferromagnetic LaCo5, confirming the theoretically predicted electronic topological transition driving the magneto-elastic collapse seen in the related compound YCo5. Our x-ray diffraction results show an anisotropic lattice collapse of the c-axis near 10 GPa that is also commensurate with a change in the majority charge carriers evident from high-pressure Hall effect measurements. The coupling of the electronic, magnetic and lattice degrees of freedom is further substantiated by the evolution of the anomalous Hall effect, which couples to the magnetization of the ordered state of LaCo5., Comment: 11 pages, 3 figures in main text with appendix of 5 pages and 3 figures. Submitted to PRB

Using high-pressure magnetotransport techniques we have discovered superconductivity in Bi2Te, a member of the infinitely adaptive (Bi2)m(Bi2Te3)n series, whose end members, Bi and Bi2Te3, can be tuned to display topological surface states or superconductivity. Bi2Te has a maximum Tc= 8.6 K at P= 14.5 GPa and goes through multiple high pressure phase transitions, ultimately collapsing into a bcc structure that suggests a universal behavior across the series. High-pressure magnetoresistance and Hall measurements suggest a semi-metal to metal transition near 5.4 GPa, which accompanies the hexagonal to intermediate phase transition seen via x-ray diffraction measurements. In addition, the linearity of Hc2(T) exceeds the Werthamer-Helfand-Hohenberg limit, even in the extreme spin-orbit scattering limit, yet is consistent with other strong spin-orbit materials. Considering these results in combination with similar reports on strong spin-orbit scattering materials seen in the literature, we suggest the need for a new theory that can address the unconventional nature of their superconducting states., Comment: 23 pages, 8 figures

We report a high-pressure study of simultaneous low-temperature electrical resistivity and Hall effect measurements on high quality single-crystalline KFe2As2 using designer diamond anvil cell techniques with applied pressures up to 33 GPa. In the low pressure regime, we show that the superconducting transition temperature T_c finds a maximum onset value of 7 K near 2 GPa, in contrast to previous reports that find a minimum T_c and reversal of pressure dependence at this pressure. Upon applying higher pressures, this T_c is diminished until a sudden drastic enhancement occurs coincident with a first-order structural phase transition into a collapsed tetragonal phase. The appearance of a distinct superconducting phase above 13 GPa is also accompanied by a sudden reversal of dominant charge carrier sign, from hole- to electron-like, which agrees with our band calculations predicting the emergence of an electron pocket and diminishment of hole pockets upon Fermi surface reconstruction. Our results suggest the high-temperature superconducting phase in KFe2As2 is substantially enhanced by the presence of nested electron and hole pockets, providing the key ingredient of high-T_c superconductivity in iron pnictide superconductors., Comment: 5 pages, 4 figures; Phys. Rev. B - Rapid Communications (in press)

We experimentally investigate the symmetry in the Hidden Order (HO) phase of intermetallic URu2Si2 by mapping the lattice and magnetic excitations via inelastic neutron and x-ray scattering measurements in the HO and high-temperature paramagnetic phases. At all temperatures the excitations respect the zone edges of the body-centered tetragonal paramagnetic phase, showing no signs of reduced spatial symmetry, even in the HO phase. The magnetic excitations originate from transitions between hybridized bands and track the Fermi surface, whose feature are corroborated by the phonon measurements. Due to a large hybridization energy scale, a full uranium moment persists in the HO phase, consistent with a lack of observed crystal-field-split states. Our results are inconsistent with local order parameter models and the behavior of typical density waves. We suggest that an order parameter that does not break spatial symmetry would naturally explain these characteristics., Comment: 16 pages, 13 figures The scope of this work was expanded to include much more magnetic neutron scattering as well as inelastic x-ray scattering. The modes originally identified as soft phonons are magnetic. Many of the figures had their quality reduced in order to fit the arxiv file size limits. Please see the PRB article for higher quality images

We have synthesized two iron-pnictide/chalcogenide materials, CuFeTe2 and Fe2As, which share crystallographic features with known iron-based superconductors, and carried out high-pressure electrical resistivity measurements on these materials to pressures in excess of 30 GPa. Both compounds crystallize in the Cu2Sb-type crystal structure that is characteristic of LiFeAs (with CuFeTe2 exhibiting a disordered variant). At ambient pressure, CuFeTe2 is a semiconductor and has been suggested to exhibit a spin-density-wave transition, while Fe2As is a metallic antiferromagnet. The electrical resistivity of CuFeTe2, measured at 4 K, decreases by almost two orders of magnitude between ambient pressure and 2.4 GPa. At 34 GPa, the electrical resistivity decreases upon cooling the sample below 150 K, suggesting the proximity of the compound to a metal-insulator transition. Neither CuFeTe2 nor Fe2As superconduct above 1.1 K throughout the measured pressure range., Comment: 6 pages, 7 figures

The CeFeAsO and CeFePO iron pnictide compounds were studied via electrical transport measurements under high-pressure. In CeFeAsO polycrystals, the magnetic phases involving the Fe and Ce ions coexist up to 15 GPa, with no signs of pressure-induced superconductivity up to 50 GPa. For the CeFePO single crystals, pressure stabilizes the Kondo screening of the Ce 4f-electron magnetic moments., Comment: 5 pages, 4 figures. Figure 1 is now separated into Fig. 1 and Fig. 2 to separate piston-cylinder and anvil pressure techniques. Updated reference list. Modified Fig. 4

The onset of antiferromagnetic order in URu2Si2 has been studied via neutron diffraction in a helium pressure medium, which most closely approximates hydrostatic conditions. The antiferromagnetic critical pressure is 0.80 GPa, considerably higher than values previously reported. Complementary electrical resistivity measurements imply that the hidden order-antiferromagnetic bicritical point far exceeds 1.02 GPa. Moreover, the redefined pressure-temperature phase diagram suggests that the superconducting and antiferromagnetic phase boundaries actually meet at a common critical pressure at zero temperature., Comment: 5 pgs, 4 figs; AFM ordered moment revised to 0.5 muB, added and corrected citations and references

The pressure-dependence of the hidden order phase transition of URu2Si2 is shown to depend sensitively upon the quality of hydrostatic pressure conditions during electrical resistivity measurements. Hysteresis in pressure is demonstrated for two choices of pressure medium: the commonly-used mixture of 1:1 Fluorinert FC70/FC77 and pure FC75. In contrast, no hysteresis is observed when the pressure medium is a 1:1 mixture of n-pentane/isoamyl alcohol, as it remains hydrostatic over the entire studied pressure range. Possible ramifications for the interpretation of the temperature-pressure phase diagram of URu2Si2 are discussed., Comment: 9 pgs, 2 figs, accepted by High Pressure Research