Multiorbital systems away from global half-filling host intriguing physical properties promoted by Hund’s coupling. Despite increasing awareness of this regime dubbed Hund’s metal, effect of nonlocal interaction is still elusive. Here we study a three-orbital model with 1/3 filling (two electrons per site) including the intersite Coulomb interaction (V). Using the GW plus extended dynamical mean-field theory, the valence-skipping charge order transition is shown to be driven by V. Most interestingly, the instability to this transition is significantly enhanced in the spin-freezing crossover regime, thereby lowering the critical V to the formation of charge order. This behavior is found to be closely related to the population profile of the atomic multiplet states in the spin-freezing regime. In this regime, maximum spin states are dominant in each total charge subspace with substantial amount of one- and three-electron occupations, which leads to almost equal population of one- and the maximum spin three-electron state. Our finding unveils another feature of the Hund’s metal and has potential implications for the broad range of multiorbital systems as well as the recently discovered charge order in iron pnictides.

远离全球半充实主机的多轨道系统吸引了由洪德耦合促进的物理特性。尽管人们越来越意识到这种被称为洪德金属的制度，但非局部相互作用的影响仍然难以捉摸。在这里，我们研究了一个具有1/3填充（每个位点两个电子）的三轨道模型，其中包括位间库仑相互作用（V）。使用G W加上扩展的动态平均场理论，表明价态跳跃电荷阶跃由V驱动。最有趣的是，这种转变的不稳定性在自旋冻结交叉状态下得到了显着增强，从而降低了临界V来形成收费单。发现这种行为与自旋冻结状态下原子多重态的总体分布密切相关。在这种情况下，最大的自旋态在每个总电荷子空间中占主导地位，大量的一电子和三电子占据，这导致一键和最大自旋三电子态几乎相等。我们的发现揭示了洪德金属的另一个特征，并且对广泛的多轨道系统以及最近发现的铁离子电荷顺序具有潜在的影响。