Comparative structural evolution under pressure of powder and single crystals of the layered antiferromagnet FePS3

FePS3 is a layered magnetic van der Waals compound that undergoes a Mott insulator-metal transition under applied pressure. The transition has an associated change in the crystal symmetry and magnetic structure. Understanding the underlying physics of these transitions requires a detailed understanding of the crystal structure as a function of pressure. Two conflicting models have previously been proposed for the evolution of the structure with pressure. To settle the disagreement, we present a study of the pressure-dependent crystal structures using both single-crystal and powder x-ray diffraction measurements. We show unambiguously that the highest-pressure transition involves a collapse of the interplanar spacing, along with an increase in symmetry from a monoclinic to a trigonal space group, to the exclusion of other models. Our collected results are crucial for understanding high-pressure behavior in these materials and demonstrate a clear and complete methodology for exploring complex two-dimensional material structures under pressure

Bulk properties of the van der Waals hard ferromagnet VI3

We present comprehensive measurements of the structural, magnetic, and electronic properties of layered van der Waals ferromagnet VI3 down to low temperatures. Despite belonging to a well-studied family of transition-metal trihalides, this material has received very little attention. We outline, from high-resolution powder x-ray diffraction measurements, a corrected room-temperature crystal structure to that previously proposed and uncover a structural transition at 79 K, also seen in the heat capacity. Magnetization measurements confirm VI3 to be a hard ferromagnet (9.1 kOe coercive field at 2 K) with a high degree of anisotropy, and the pressure dependence of the magnetic properties provide evidence for the two-dimensional nature of the magnetic order. Optical and electrical transport measurements show this material to be an insulator with an optical band gap of 0.67 eV - the previous theoretical predictions of d-band metallicity then lead us to believe VI3 to be a correlated Mott insulator. Our latest band-structure calculations support this picture and show good agreement with the experimental data. We suggest VI3 to host great potential in the thriving field of low-dimensional magnetism and functional materials, together with opportunities to study and make use of low-dimensional Mott physics

Pressure induced electronic and structural phase evolution in Van der Waals compound FePS3_3

Two-dimensional materials have proven to be a prolific breeding ground of new and unstudied forms of magnetism and unusual metallic states, particularly when tuned between their insulating and metallic phases. In this paper we present work on a new metal to insulator transition system FePS3 . This compound is a two-dimensional van-der-Waals antiferromagnetic Mott insulator. Here we report the discovery of an insulator-metal transition in FePS3, as evidenced by x-ray diffraction and electrical transport measurements, using high pressure as a tuning parameter. Two structural phase transitions are observed in the x-ray diffraction data as a function of pressure and resistivity measurements show evidence of the onset of a metallic state at high pressures. We propose models for the two new structures that can successfully explain the x-ray diffraction patterns

Dielectric Response of Quantum Critical Ferroelectric as a Function of Pressure.

In this work we report for the first time measurements of the dielectric loss of single-crystal SrTiO3 under the application of hydrostatic pressure up to 20 kbar and temperatures down to 200 mK which allow us to comment on the evolution of new fundamental material properties and their relationship with the recently discovered quantum critical phenomena in this material. The well known 18 K peak or shoulder was no longer observed after pressure was applied, even after subsequently removing it, suggesting it is associated with the twin walls formed at the 110 K cubic-tetragonal transition. The family of familiar peaks were all seen to increase in temperature linearly with pressure and the height of the 9.4 K peak was drastically suppressed by even the smallest pressures. This peak is discussed in the context of a postulated ferroelectric quantum critical point in SrTiO3 and the behaviour of its size linked to the position of this point on the recently established phase diagram

Quantum critical phenomena in a compressible displacive ferroelectric

The dielectric and magnetic polarizations of quantum paraelectrics and paramagnetic materials have in many cases been found to initially increase with increasing thermal disorder and hence exhibit peaks as a function of temperature. A quantitative description of these examples of 'order-by-disorder' phenomenona has remained elusive in nearly ferromagnetic metals and in dielectrics on the border of displacive ferroelectric transitions. Here we present an experimental study of the evolution of the dielectric susceptibility peak as a function of pressure in the nearly ferroelectric material, strontium titanate, which reveals that the peak position collapses towards absolute zero as the ferroelectric quantum critical point is approached. We show that this behaviour can be described in detail without the use of adjustable parameters in terms of the Larkin-Khmelnitskii-Shneerson-Rechester (LKSR) theory, first introduced nearly 50 years ago, of the hybridization of polar and acoustic modes in quantum paraelectrics, in contrast to alternative models that have been proposed. Our study allows us to construct for the first time a detailed temperature-pressure phase diagram of a material on the border of a ferroelectric quantum critical point comprising ferroelectric, quantum critical paraelectric and hybridized polar-acoustic regimes. Furthermore, at the lowest temperatures, below the susceptibility maximum, we observe a new regime characterized by a linear temperature dependence of the inverse susceptibility that differs sharply from the quartic temperature dependence predicted by the LKSR theory. We find that this non-LKSR low temperature regime cannot be accounted for in terms of any detailed model reported in the literature, and its interpretation poses a new empirical and conceptual challenge

Low temperature resistivity of the rare earth diborides (Er, Ho, Tm)B<inf>2</inf>

© Springer International Publishing Switzerland 2015. The discovery of superconductivity in MgB2 sparked much interest in the diborides and led to further discoveries in this class of materials. Attention has focussed on the transitions metal diborides and the rare-earth diborides have remained sparsely investigated. Here we present electrical transport in polycrystalline samples of ErB2, TmB2 and HoB2 as a function of temperature down to 0.1 K. Particularly interesting is the large difference in the temperature dependence of resistivity, above and below the clear magnetic ordering temperature of 13.8, 9 and 7.5 K for ErB2, HoB2 and TmB2 respectively

Modular thermal Hall effect measurement setup for fast-turnaround screening of materials over wide temperature range using capacitive thermometry

We demonstrate a simple and easy-to-build probe designed to be loaded into a widely available Quantum Design Physical Properties Measurement System (PPMS) cryostat, with a detachable shielded sample puck section and robust heat sinking of three pairs of coaxial cables. It can be in principle used with any low-temperature cryostat. Our modular puck design has a radiation shield for thermal isolation and protection of the delicate sample space while handling and allows any variety of experimental setup benefiting from shielded coaxial wiring to be constructed on a selection of sample pucks. Pucks can be quickly and easily switched, and the system makes use of the simple yet extremely stable temperature and magnetic field control of the easy-to-use PPMS system. We focus on a setup designed for measurements of the thermal Hall effect and show that this system can yield unprecedented resolution over a wide temperature range and with rapid sample mounting or changing—allowing a large collection of potential samples to be screened for this novel physics. Our design aims to make these sensitive but challenging measurements quick, reliable, cheap, and accessible, through the use of a standard, widespread base cryostat and a system of modular removable sample stage pucks to allow quick turnaround and screening of a large number of candidate samples for potential new thermal Hall physics

Modular thermal Hall effect measurement setup for fast-turnaround screening of materials over wide temperature range using capacitive thermometry

We demonstrate a simple and easy-to-build probe designed to be loaded into a widely available Quantum Design Physical Properties Measurement System (PPMS) cryostat, with a detachable shielded sample puck section and robust heat sinking of three pairs of coaxial cables. It can be in principle used with any low-temperature cryostat. Our modular puck design has a radiation shield for thermal isolation and protection of the delicate sample space while handling and allows any variety of experimental setup benefiting from shielded coaxial wiring to be constructed on a selection of sample pucks. Pucks can be quickly and easily switched, and the system makes use of the simple yet extremely stable temperature and magnetic field control of the easy-to-use PPMS system. We focus on a setup designed for measurements of the thermal Hall effect and show that this system can yield unprecedented resolution over a wide temperature range and with rapid sample mounting or changing—allowing a large collection of potential samples to be screened for this novel physics. Our design aims to make these sensitive but challenging measurements quick, reliable, cheap, and accessible, through the use of a standard, widespread base cryostat and a system of modular removable sample stage pucks to allow quick turnaround and screening of a large number of candidate samples for potential new thermal Hall physics

Isostructural Mott transition in 2D honeycomb antiferromagnet V<inf>0.9</inf>PS<inf>3</inf>

We present the observation of an isostructural Mott insulator-metal transition in van-der-Waals honeycomb antiferromagnet V$_{0.9}$PS$_3$ through high-pressure x-ray diffraction and transport measurements. The MPX$_3$ family of magnetic van-der-Waals materials (M denotes a first row transition metal and X either S or Se) are currently the subject of broad and intense attention, but the vanadium compounds have until this point not been studied beyond their basic properties. We observe insulating variable-range-hopping type resistivity in V$_{0.9}$PS$_3$, with a gradual increase in effective dimensionality with increasing pressure, followed by a transition to a metallic resistivity temperature dependence between 112 and 124 kbar. The metallic state additionally shows a low-temperature upturn we tentatively attribute to the Kondo Effect. A gradual structural distortion is seen between 26-80 kbar, but no structural change at higher pressures corresponding to the insulator-metal transition. We conclude that the insulator-metal transition occurs in the absence of any distortions to the lattice - an isostructural Mott transition in a new class of two-dimensional material, and in strong contrast to the behavior of the other MPX$_3$ compounds

Magnetotransport of Sm2Ir2O7 across the pressure-induced quantum-critical phase boundary

Acknowledgements: We thank T. Orton and P. Ruddy at the University of Warwick for technical assistance. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No. 681260). We acknowledge the Engineering and Physical Sciences Research Council (EPSRC), UK and the Oxford-ShanghaiTech collaboration project for financial support. This work was supported by EPSRC grants No. EP/P034616/1, No. EP/V062654/1 and No. EP/N034872/1. A portion of this work was performed at the National High Magnetic Field Laboratory (NHMFL), which is supported by National Science Foundation Cooperative Agreement No. DMR-1644779 and the Department of Energy (DOE). J.S. acknowledges support from the DOE BES program “Science at 100 T”, which permitted the design and construction of the specialized equipment used in the high-field studies.AbstractRare-earth pyrochlore iridates host two interlocking magnetic sublattices of corner-sharing tetrahedra and can harbour a unique combination of frustrated moments, exotic excitations and highly correlated electrons. They are also the first systems predicted to display both topological Weyl semimetal and axion insulator phases. We have measured the transport and magnetotransport properties of single-crystal Sm2Ir2O7 up to and beyond the pressure-induced quantum critical point for all-in-all-out (AIAO) Ir order at pc = 63 kbar previously identified by resonant X-ray scattering and close to which Weyl semimetallic behavior has been previously predicted. Our findings overturn the accepted expectation that the suppression of AIAO order should lead to metallic conduction persisting down to zero temperature. Instead, the resistivity-minimum temperature, which tracks the decrease in the AIAO ordering temperature for pressures up to 30 kbar, begins to increase under further application of pressure, pointing to the presence of a second as-yet unidentified mechanism leading to non-metallic behavior. The magnetotransport does track the suppression of Ir magnetism, however, with a strong hysteresis observed only within the AIAO phase boundary, similar to that found for Ho2Ir2O7 and attributed to plastic deformation of Ir domains. Around pc we find the emergence of a new type of electronic phase, characterized by a negative magnetoresistance with small hysteresis at the lowest temperatures, and hysteresis-free positive magnetoresistance above approximately 5 K. The temperature dependence of our low-temperature transport data are found to be best described by a model consistent with a Weyl semimetal across the entire pressure range.</jats:p