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Charles R. S. Haines

Publications and source records attributed to Charles R. S. Haines.

3 recordsLinked to original sources

Emergent Polar Metal Phase in a Van der Waals Mott Magnet

We report the emergence of a two-dimensional (2D) polar metal phase in van der Waals compound FePSe$_3$ under moderate pressures. This layered material is a Mott insulator with antiferromagnetic order under ambient conditions. We show that FePSe$_3$ uniquely allows tuning a 2D correlated insulator into an exotic metal state where a loss of inversion symmetry leads to periodic polar displacements of ions, within a conducting phase - a polar metal. Our combined synchrotron and neutron diffraction data allow us to present a long-sought, unambiguous high-pressure structural model and show the polar displacements of this new phase. We also observe the suppression of magnetic ordering at the insulator-to-metal transition correspondent with this structural change. Our work outlines a comprehensive temperature-pressure phase diagram of FePSe$_3$, combining detailed structural, magnetic and transport data. The high-pressure phase exhibits activated semiconductor behavior at high temperatures, a $T^2$-dependence in its resistivity at lower temperatures - despite the conditions required for a `good metal' Fermi-Liquid description not being met in this case - and a low-temperature resistivity upturn which is suppressed as the system is tuned away from the concomitant transitions. The realisation of a tunable 2D polar metal state in FePSe$_3$ due to the loss of its inversion symmetry combined with pressure-induced metallicity offers a promising new platform to investigate this exotic phase at accessible pressures.

cond-mat.str-el↗

Comparative structural evolution under pressure of powder and single crystals of the layered antiferromagnet FePS$_3$

The layered antiferromagnet FePS$_3$ has been shown to undergo a structural transition under pressure linked to an insulator-metal transition, with two incompatible models previously proposed for the highest-pressure structure. We present a study of the high-pressure crystal structures of FePS$_3$ using both single-crystal and powder x-ray diffraction. We show that the highest pressure transition involves a collapse of the inter-planar spacing of this material, along with an increase in symmetry from a monoclinic to a trigonal structure, to the exclusion of other models. The extent of this volume collapse is shown to be sensitive to the presence of a helium pressure medium in the sample environment, indicating that consideration of such experimental factors is important for understanding high-pressure behaviours in this material.

cond-mat.str-el↗

Evolution of magnetic order in van-der-Waals antiferromagnet FePS$_3$ through insulator-metal transition

Layered van-der-Waals 2D magnetic materials are of great interest in fundamental condensed-matter physics research, as well as for potential applications in spintronics and device physics. We present neutron powder diffraction data using new ultra-high-pressure techniques to measure the magnetic structure of Mott-insulating 2D honeycomb antiferromagnet FePS$_3$ at pressures up to 183 kbar and temperatures down to 80 K. These data are complemented by high-pressure magnetometry and reverse Monte Carlo modeling of the spin configurations. As pressure is applied, the previously-measured ambient-pressure magnetic order switches from an antiferromagnetic to a ferromagnetic interplanar interaction, and from 2D-like to 3D-like character. The overall antiferromagnetic structure within the $ab$ planes, ferromagnetic chains antiferromagnetically coupled, is preserved, but the magnetic propagation vector is altered from $(0\:1\:\frac{1}{2})$ to $(0\:1\:0)$, a halving of the magnetic unit cell size. At higher pressures, coincident with the second structural transition and the insulator-metal transition in this compound, we observe a suppression of this long-range-order and emergence of a form of magnetic short-range order which survives above room temperature. Reverse Monte Carlo fitting suggests this phase to be a short-ranged version of the original ambient pressure structure - with a return to antiferromagnetic interplanar correlations. The persistence of magnetism well into the HP-II metallic state is an observation in seeming contradiction with previous x-ray spectroscopy results which suggest a spin-crossover transition.

cond-mat.str-el↗