Abstract
In spin-ice research, small variations in structure or interactions drive a multitude of different behaviors, yet the collection of known materials relies heavily on the "227" pyrochlore structure. Here, we present thermodynamic, structural, and inelastic-neutron-scattering data on a spin-ice material, MgEr2Se4, which contributes to the relatively underexplored family of rare-earth spinel chalcogenides. X-ray and neutron diffraction confirm a normal spinel structure and place Er3+ moments on an ideal pyrochlore sublattice. Measurement of crystal electric field excitations with inelastic neutron scattering confirms that the moments have perfect Ising character, and further identifies the ground-state Kramers doublet as having dipolar-octupolar form with a significant multipolar character. Heat capacity and magnetic neutron diffuse scattering have icelike features, but are inconsistent with Monte Carlo simulations of the nearest-neighbor and next-nearest-neighbor dipolar spin-ice (DSI) models. A significant remnant entropy is observed as T→0 K, but again falls short of the full Pauling expectation for DSI, unless significant disorder is added. We show that these observations are fully in line with what has been recently reported for CdEr2Se4, and point to the importance of quantum fluctuations in these materials.
| Original language | English |
|---|---|
| Article number | 134438 |
| Journal | Physical Review B |
| Volume | 99 |
| Issue number | 13 |
| DOIs | |
| State | Published - Apr 26 2019 |
Funding
The authors acknowledge useful discussions with P. Schiffer, G. Sala, and G. Chen. This work was sponsored by the National Science Foundation, under Grant No. DMR-1455264-CAR. D.R. further acknowledges the partial support of the U.S. D.O.E., Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for the DOE under Contract No. DE-AC05-06OR23100. Synthesis and thermodynamic measurements were carried out in the Materials Research Laboratory Central Research Facilities, University of Illinois. Scattering measurements were conducted at the Center for Nanophase Materials Sciences, at the High Flux Isotope Reactor and at the Spallation Neutron Source, each DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. This work is part of the Blue Waters sustained petascale computing project, which is supported by the National Science Foundation (Awards No. OCI-0725070 and No. ACI-1238993) and the State of Illinois.