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J. W. Kolis

Publications and source records attributed to J. W. Kolis.

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Observation of Dipolar Spin-ice--like Correlations in the Quantum Spin Ice Candidate Ce$_2$Sn$_2$O$_7$

We report diffuse scattering measurements on the dipolar-octupolar pyrochlore, Ce$_2$Sn$_2$O$_7$, to elucidate its magnetic correlations within the correlated paramagnetic regime above its ordering temperature, $\mathrm{T_N}\sim 40~$mK. The magnetic transition at $\mathrm{T_N}$, observed in recent specific heat measurements, has been interpreted within the nearest-neighbor XYZ model as a transition into an all-in-all-out (AIAO) magnetic order. However, the observed diffuse scattering above $\mathrm{T_N}$ argues against an AIAO magnetic order by exhibiting $no$ short-range order at the AIAO wave-vectors, inconsistent with the nearest neighbor model. Instead, the observed diffuse scattering strongly resembles that observed in classical dipolar spin ice, Dy$_2$Ti$_2$O$_7$, and suggests the presence of short-range correlated structures such as chains, or clusters in the low energy manifold of Ce$_2$Sn$_2$O$_7$, favored by further neighbor interactions. We discuss how chain-like states qualitatively account for the observed H-T phase diagram under a [1,1,0]-field.

cond-mat.str-el

Zero-Field Long Range Order at $T \sim 40$ mK in the Proximate Quantum Spin Ice Ce$_2$Sn$_2$O$_7$ and Phase Diagram for Magnetic Fields Along [1,1,0]

The Ce$^{3+}$ pseudospin-1/2 degrees of freedom in the pyrochlore magnets Ce$_2$X$_2$O$_7$, with $X$ = Zr, Hf, or Sn, possess dipole-octupole character. The XYZ nearest-neighbor model Hamiltonians which have successfully described their properties make them attractive candidates for quantum spin ice ground states. We report new heat capacity measurements to very low temperatures on a high-quality single crystal of Ce$_2$Sn$_2$O$_7$ grown by hydrothermal techniques. Our zero-field measurements uncover a clear first order transition to long-ranged order at $T \sim 0.04$ K, well below the downturn in the broader Schottky-like anomaly that is a common feature in the zero-field heat capacity for cerium pyrochlores. This observation settles the debate as to whether Ce$_2$Sn$_2$O$_7$ possesses a QSI ground state in zero field - it does not. However, we also find compelling evidence suggesting that spin ice physics is nearby, and remains relevant to Ce$_2$Sn$_2$O$_7$. Application of a magnetic field along the $[1,1,0]$ direction leads to an evolution of this peak to a weak anomaly at higher temperature more characteristic of a continuous, mean field transition. At higher fields along $[1,1,0]$, the Schottky-like anomaly bifurcates similar to expectations for independent polarized $α$ and orthogonal $β$ chains in classical spin ice. These new experimental results demonstrate richness to the phase diagram for Ce-based pyrochlores.

cond-mat.str-el

Dipolar spin ice regime proximate to an all-in-all-out Néel ground state in the dipolar-octupolar pyrochlore Ce$_2$Sn$_2$O$_7$

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) Néel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order.

cond-mat.str-el

Understanding Reentrance in Frustrated Magnets: the Case of the Er$_2$Sn$_2$O$_7$ Pyrochlore

Reentrance, the return of a system from an ordered phase to a previously encountered less-ordered one as a controlled parameter is continuously varied, is a recurring theme found in disparate physical systems, from condensed matter to black holes. While diverse in its many incarnations and generally unsuspected, the cause of reentrance at the microscopic level is often not investigated thoroughly. Here, through detailed characterization and theoretical modeling, we uncover the microscopic mechanism behind reentrance in the strongly frustrated pyrochlore antiferromagnet Er$_2$Sn$_2$O$_7$. Taking advantage of the recent advance in rare earth stannate single crystal synthesis, we use heat capacity measurements to expose that Er$_2$Sn$_2$O$_7$ exhibits multiple instances of reentrance in its magnetic field $B$ vs. temperature $T$ phase diagram for magnetic fields along three cubic high symmetry directions. Through classical Monte Carlo simulations, mean field theory and classical linear spin-wave expansions, we argue that the origins of the multiple occurrences of reentrance observed in Er$_2$Sn$_2$O$_7$ are linked to soft modes. Depending on the field direction, these arise either from a direct $T=0$ competition between the field-evolved ground states, or from a field-induced enhancement of the competition with a distinct zero-field antiferromagnetic phase. In both scenarios, the phase competition enhances thermal fluctuations which entropically stabilize a specific ordered phase. This results in an increased transition temperature for certain field values and thus the reentrant behavior. Our work represents a detailed examination into the mechanisms responsible for reentrance in a frustrated magnet and may serve as a template for the interpretation of reentrant phenomena in other physical systems.

cond-mat.str-el

Local-Ising type magnetic order and metamagnetism in the rare-earth pyrogermanate Er$_2$Ge$_2$O$_7$

The recent discoveries of proximate quantum spin-liquid compounds and their potential application in quantum computing informs the search for new candidate materials for quantum spin-ice and spin-liquid physics. While the majority of such work has centered on members of the pyrochlore family due to their inherently frustrated linked tetrahedral structure, the rare-earth pyrogermanates also show promise for possible frustrated magnetic behavior. With the familiar stoichiometry $RE_2$Ge$_2$O$_7$, these compounds generally have tetragonal symmetry with a rare-earth sublattice built of a spiral of alternating edge and corner sharing rare-earth site triangles. Studies on Dy$_2$Ge$_2$O$_7$ and Ho$_2$Ge$_2$O$_7$ have shown tunable low temperature antiferromagnetic order, a high frustration index and spin-ice like dynamics. Here we use neutron diffraction to study magnetic order in Er$_2$Ge$_2$O$_7$ (space group $P4_{1}2_{1}2$ ) and find the lowest yet Neél temperature in the pyrogermanates of 1.15 K. Using neutron powder diffraction we find the magnetic structure to order with $k = (0,0,0)$ ordering vector, magnetic space group symmetry $P4_{1}^{'}2_{1}2^{'}$ and a refined Er moment of $m = 8.1 μ_B$ - near the expected value for the Er$^{3+}$ free ion. Provocatively, the magnetic structure exhibits similar 'local-Ising' behavior to that seen in the pyrocholres where the Er moment points up or down along the short Er-Er bond. Upon applying a magnetic field we find a first order metamagnetic transition at $\sim$ 0.35 T to a lower symmetry $P2_{1}^{'}2_{1}^{'}2$ structure. This magnetic transition involves an inversion of Er moments aligned antiparallel to the applied field describing a class I spin-flip type transition, indicating a strong local anisotropy at the Er site - reminiscent of that seen in the spin-ice pyrochlores.

cond-mat.str-el

The magnetic order of a manganese vanadate system with two-dimensional striped triangular lattice

Results of magnetization and neutron diffraction measurements of the manganese vanadate system Mn$_5$(VO$_4$)$_2$(OH)$_4$ are reported. The crystal structure of this compound contains triangular [Mn$_3$O$_{13}$] building blocks that produce two-dimensional Mn$^{2+}$ magnetic networks with striped triangular topologies. The Mn sheets are connected through the nonmagnetic vanadate tetrahedra extending along the $a$-axis. Magnetization measurements performed on single crystals reveal the onset of a long-range antiferromagnetic order below approximately 45 K. The magnetic structure is Néel-type with nearest-neighbor Mn atoms coupled via three or four antiferromagnetic bonds. The magnetic moments are confined within the layers and are oriented parallel to the $b$ direction. The magnitudes of ordered moments are reduced, presumably by geometrical frustration and the low-dimensionality of the lattice structure.

cond-mat.str-el