Spin-state crossover beyond a conventional ligand-field theory has been a fundamental issue in condensed matter physics. Here, we report microscopic observations of spin states and low-energy dynamics through orbital-resolved NMR spectroscopy in the prototype compound LaCoO$_3$. The $^{59}$Co NMR spectrum shows the preserved crystal symmetry across the crossover, inconsistent with $d$ orbital ordering due to the Jahn-Teller distortion. The orbital degeneracy results in a pseudospin ($\tilde{J} = 1$) excited state with an orbital moment observed as $^{59}$Co hyperfine coupling tensors. We found that the population of the excited state evolves above the heart crossover temperature. The crossover involves critical spin-state fluctuations emerging under the magnetic field. These results suggest that the spin-state crossover can be mapped into a statistical problem, analogous to the supercritical liquid in liquid-gas transition.
翻译:常规离心场理论之外, 旋转交叉是浓缩物质物理学中的一个基本问题。 在这里, 我们报告在原型化合物LaCoO$3美元中, 通过轨道解解解NMR光谱仪对旋转状态和低能动态进行微镜观测。 $*59美元NMR频谱显示交叉交叉处保存的晶体对称, 与Jahn- Teller扭曲的轨道订单不一致。 轨道脱基因导致假晶($\tilde{J}=1美元) 兴奋状态, 其轨道时段观察值为$*59美元- o superfine multors。 我们发现, 兴奋状态的人口在心脏交叉温度之上会变化。 交叉点涉及到磁场下出现的关键旋转状态波动。 这些结果显示, 旋转交叉可被映射成一个统计问题, 类似于液气转换中的超临界液体。