Charge order through crystallization of Frenkel excitons: realization in kagome metals

Abstract: Charge order is a widely observed and representative example of spontaneous broken symmetries in quantum states of matter. Owing to the large intra-atomic Coulomb energy, the charge redistribution in such an order typically implies significant alteration of the electronic and lattice properties of materials. While the standard description of charge order, namely a "charge density wave" instability of the Fermi surface, has been broadly and successfully applied to good metals, its applicability to correlated ionic materials has been rather limited. Here, we propose an alternative general scenario of charge order - crystallization of long-lived Frenkel excitons - suitable for these ionic materials. We demonstrate this scenario on the recently discovered kagome superconductors and successfully reproduce all the characteristics of experimental observations on both local charge correlations and long-range ordering. The proposed generic scenario offers a long-sought understanding of charge order applicable to modern correlated functional materials.