Magnetism, structure, and charge correlation at a pressure-induced Mott-Hubbard insulator-metal transition

We use synchrotron x-ray diffraction and electrical transport under pressure to probe both the magnetism and the structure of single crystal NiS2 across its Mott-Hubbard transition. In the insulator, the low-temperature antiferromagnetic order results from superexchange among correlated electrons and couples to a (1/2, 1/2, 1/2) superlattice distortion. Applying pressure suppresses the insulating state, but enhances the magnetism as the superexchange increases with decreasing lattice constant. By comparing our results under pressure to previous studies of doped crystals we show that this dependence of the magnetism on the lattice constant is consistent for both band broadening and band filling. In the high pressure metallic phase the lattice symmetry is reduced from cubic to monoclinic, pointing to the primary influence of charge correlations at the transition. There exists a wide regime of phase separation that may be a general characteristic of correlated quantum matter.Comment: 5 pages, 3 figure

Approaching the quantum critical point in a highly-correlated all-in-all-out antiferromagnet

Continuous quantum phase transition involving all-in–all-out (AIAO) antiferromagnetic order in strongly spin-orbit-coupled 5d compounds could give rise to various exotic electronic phases and strongly-coupled quantum critical phenomena. Here we experimentally trace the AIAO spin order in Sm₂Ir₂O₇ using direct resonant x-ray magnetic diffraction techniques under high pressure. The magnetic order is suppressed at a critical pressure P_c=6.30GPa, while the lattice symmetry remains in the cubic Fd−3m space group across the quantum critical point. Comparing pressure tuning and the chemical series R₂Ir₂O₇ reveals that the approach to the AIAO quantum phase transition is characterized by contrasting evolutions of the pyrochlore lattice constant a and the trigonal distortion surrounding individual Ir moments, which affects the 5d bandwidth and the Ising anisotropy, respectively. We posit that the opposite effects of pressure and chemical tuning lead to spin fluctuations with different Ising and Heisenberg character in the quantum critical region. Finally, the observed low pressure scale of the AIAO quantum phase transition in Sm₂Ir₂O₇ identifies a circumscribed region of P-T space for investigating the putative magnetic Weyl semimetal state

Diffraction line-shapes, Fermi surface nesting, and quantum criticality in antiferromagnetic chromium at high pressure (invited)

We explore the behavior of the nested bandstructure of chromium as a function of temperature and pressure to the point where magnetism disappears. X-ray diffraction measurements of the charge order parameter suggest that the nesting condition is maintained at high pressure, where the spin density wave ground state is destabilized by a continuous quantum phase transition. By comparing diffraction line-shapes measured throughout the temperature-pressure phase diagram we are able to identify and describe three regimes: thermal near-critical, weak coupling ground state, and quantum critical

Pressure-induced Spin-Peierls to Incommensurate Charge-Density-Wave Transition in the Ground State of TiOCl

The ground state of the spin-Peierls system TiOCl was probed using synchrotron x-ray diffraction on a single-crystal sample at T = 6 K. We tracked the evolution of the structural superlattice peaks associated with the dimerized ground state as a function of pressure. The dimerization along the b axis is rapidly suppressed in the vicinity of a first-order structural phase transition at Pc = 13.1(1) GPa. The high-pressure phase is characterized by an incommensurate charge density wave perpendicular to the original spin chain direction. These results show that the electronic ground state undergoes a fundamental change in symmetry, indicating a significant change in the principal interactions.Comment: 5 pages, 4 figure

Strongly-coupled quantum critical point in an all-in-all-out antiferromagnet

Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Using newly-developed, high-pressure resonant x-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd2Os2O7 as the all-in-all-out (AIAO) antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound

Invited Article: High-pressure techniques for condensed matter physics at low temperature

Condensed matter experiments at high pressure accentuate the need for accurate pressure scales over a broad range of temperatures, as well as placing a premium on a homogeneous pressure environment. However, challenges remain in diamond anvil cell technology, including both the quality of various pressure transmitting media and the accuracy of secondary pressure scales at low temperature. We directly calibrate the ruby fluorescence R1 line shift with pressure at T=4.5 K using high-resolution x-ray powder diffraction measurements of the silver lattice constant and its known equation of state up to P=16 GPa. Our results reveal a ruby pressure scale at low temperatures that differs by 6% from the best available ruby scale at room T. We also use ruby fluorescence to characterize the pressure inhomogeneity and anisotropy in two representative and commonly used pressure media, helium and methanol:ethanol 4:1, under the same preparation conditions for pressures up to 20 GPa at T=5 K. Contrary to the accepted wisdom, both media show equal levels of pressure inhomogeneity measured over the same area, with a consistent Delta P/P per unit area of +/- 1.8 %/(10^(4) µm^(2)) from 0 to 20 GPa. The helium medium shows an essentially constant deviatoric stress of 0.021 +/- 0.011 GPa up to 16 GPa, while the methanol:ethanol mixture shows a similar level of anisotropy up to 10 GPa, above which the anisotropy increases. The quality of both pressure media is further examined under the more stringent requirements of single crystal x-ray diffraction at cryogenic temperature. For such experiments we conclude that the ratio of sample-to-pressure chamber volume is a critical parameter in maintaining sample quality at high pressure, and may affect the choice of pressure medium

Direct probe of Fermi surface evolution across a pressure-induced quantum phase transition

The nature of a material's Fermi surface is crucial to understanding its electronic, magnetic, optical, and thermal characteristics. Traditional measurements such as angle-resolved photoemission spectroscopy and de Haas–van Alphen quantum oscillations can be difficult to perform in the vicinity of a pressure-driven quantum phase transition, although the evolution of the Fermi surface may be tied to the emergence of exotic phenomena. We demonstrate here that magnetic x-ray diffraction in combination with Hall effect measurements in a diamond anvil cell can provide valuable insight into the Fermi surface evolution in spin- and charge-density-wave systems near quantum phase transitions. In particular, we track the gradual evolution of the Fermi surface in elemental chromium and delineate the critical pressure and absence of Fermi surface reconstruction at the spin-flip transition

Approaching the quantum critical point in a highly-correlated all-in-all-out antiferromagnet

Continuous quantum phase transitions involving all-in-all-out (AIAO) antiferromagnetic order in strongly spin-orbit-coupled 5d compounds could give rise to various exotic electronic phases and strongly-coupled quantum critical phenomena. Here we experimentally trace the AIAO spin order in Sm2Ir2O7 using direct resonant x-ray magnetic diffraction techniques under high pressure. The magnetic order is suppressed at a critical pressure Pc=6.30 GPa, while the lattice symmetry remains in the cubic Fd-3m space group across the quantum critical point. Comparing pressure tuning and the chemical series R2Ir2O7 reveals that the suppression of the AIAO order and the approach to the spin-disordered state is characterized by contrasting evolutions of both the pyrochlore lattice constant a and the trigonal distortion x. The former affects the 5d bandwidth, the latter the Ising anisotropy, and as such we posit that the opposite effects of pressure and chemical tuning lead to spin fluctuations with different Ising and Heisenberg character in the quantum critical region. Finally, the observed low-pressure scale of the AIAO quantum phase transition in Sm2Ir2O7 identifies a circumscribed region of P-T space for investigating the putative magnetic Weyl-semimetal state

Quantum interference in superposed lattices

Charge transport in solids at low temperature reveals a material's mesoscopic properties and structure. Under a magnetic field, Shubnikov-de Haas (SdH) oscillations inform complex quantum transport phenomena that are not limited by the ground state characteristics. Here, in elemental metal Cr with two incommensurately superposed lattices of ions and a spin-density-wave ground state, we reveal that the phases of several low-frequency SdH oscillations in sigma_xx (rho_xx) and sigma_yy (rho_yy) are opposite, contrast with oscillations from normal cyclotron orbits that maintain identical phases. We trace the origin of the low frequency SdH oscillations to quantum interference effects arising from the incommensurate orbits of Cr's superposed reciprocal lattices, and explain the observed pi-phase shift by the reconnection of anisotropic joint open and closed orbits

Approaching the quantum critical point in a highly-correlated all-in-all-out antiferromagnet

Continuous quantum phase transition involving all-in–all-out (AIAO) antiferromagnetic order in strongly spin-orbit-coupled 5d compounds could give rise to various exotic electronic phases and strongly-coupled quantum critical phenomena. Here we experimentally trace the AIAO spin order in Sm₂Ir₂O₇ using direct resonant x-ray magnetic diffraction techniques under high pressure. The magnetic order is suppressed at a critical pressure P_c=6.30GPa, while the lattice symmetry remains in the cubic Fd−3m space group across the quantum critical point. Comparing pressure tuning and the chemical series R₂Ir₂O₇ reveals that the approach to the AIAO quantum phase transition is characterized by contrasting evolutions of the pyrochlore lattice constant a and the trigonal distortion surrounding individual Ir moments, which affects the 5d bandwidth and the Ising anisotropy, respectively. We posit that the opposite effects of pressure and chemical tuning lead to spin fluctuations with different Ising and Heisenberg character in the quantum critical region. Finally, the observed low pressure scale of the AIAO quantum phase transition in Sm₂Ir₂O₇ identifies a circumscribed region of P-T space for investigating the putative magnetic Weyl semimetal state