Laboratory for Neutron Scattering and Imaging, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland.
Department of Quantum Matter Physics, University of Geneva, CH-1211 Geneva, Switzerland.
Phys Rev Lett. 2018 Mar 30;120(13):137201. doi: 10.1103/PhysRevLett.120.137201.
Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr_{2}Se_{4} is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three orders of magnitude faster than the canonical spin ice Dy_{2}Ti_{2}O_{7}. In this Letter we use diffuse neutron scattering to show that both CdEr_{2}Se_{4} and CdEr_{2}S_{4} support a dipolar spin ice state-the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to those in Dy_{2}Ti_{2}O_{7}, i.e., dilute and uncorrelated, and so cannot provide three orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er^{3+} ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr_{2}X_{4} (X=Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr_{2}X_{4} offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples.
自旋冰中的激发表现为磁单极子,其数量和迁移率控制着自旋冰在低温下的动力学。CdEr2Se4被报道具有自旋冰的鲍林熵特征,但它的动力学比典型的自旋冰 Dy2Ti2O7快三个数量级。在这封信中,我们使用漫散射中子散射来表明 CdEr2Se4和 CdEr2S4都支持偶极自旋冰态——这是Emergent 磁单极子库仑气体的宿主相。这些库仑气体与 Dy2Ti2O7中的库仑气体具有相似的参数,即稀松和非相关,因此不能仅通过更大的单极子数量来提供三个数量级更快的动力学。我们使用交流磁化率和中子自旋回波光谱来研究单极子动力学,并使用非弹性中子散射来验证 Er3+离子的晶体电场哈密顿量。使用我们的库仑气体和晶体电场参数对单极子跳跃率进行定量计算表明,CdEr2X4(X=Se、S)中快速的动力学主要是由于单极子跳跃更快。我们的工作表明,CdEr2X4提供了研究替代自旋冰基态和动力学的可能性,与稀土 pyrochlore 相比,平衡可能在低得多的温度下实现。