The coexistence of correlated electron and hole crystals enables the realization of quantum excitonic states, capable of hosting counterflow superfluidity and topological orders with long-range quantum entanglement. Here we report evidence for imbalanced electron–hole crystals in a doped Mott insulator, namely, α-RuCl₃, through gate-tunable non-invasive van der Waals doping from graphene. Real-space imaging via scanning tunnelling microscopy reveals two distinct charge orderings at the lower and upper Hubbard band energies, whose origin is attributed to the correlation-driven honeycomb hole crystal composed of hole-rich Ru sites and rotational-symmetry-breaking paired electron crystal composed of electron-rich Ru–Ru bonds, respectively. Moreover, a gate-induced transition of electron–hole crystals is directly visualized, further corroborating their nature as correlation-driven charge crystals. The realization and atom-resolved visualization of imbalanced electron–hole crystals in a doped Mott insulator opens new doors in the search for correlated bosonic states within strongly correlated materials.

相关电子和空穴晶体的共存使得能够实现量子激子态，能够实现逆流超流性和具有长程量子纠缠的拓扑序。在这里，我们报告了掺杂莫特绝缘体（即 α-RuCl ₃ ）中通过栅极可调的非侵入性范德华掺杂石墨烯产生不平衡电子空穴晶体的证据。通过扫描隧道显微镜进行的真实空间成像揭示了哈伯德能带下部和上部的两种不同的电荷排序，其起源归因于由富含空穴的Ru位点和旋转对称破缺的配对电子晶体组成的相关驱动的蜂窝状空穴晶体分别由富电子Ru-Ru键组成。此外，电子空穴晶体的栅极诱导跃迁被直接可视化，进一步证实了它们作为相关驱动电荷晶体的性质。掺杂莫特绝缘体中不平衡电子空穴晶体的实现和原子分辨可视化为在强相关材料中寻找相关玻色子态打开了新的大门。