Entwined lattice of atoms and anionic electrons in layered electride LaCl

Abstract

Controlling the lattice geometry that governs electronic structure is a central theme in condensed-matter physics, yet in crystalline solids this geometry is usually fixed by the atomic framework. Electrides offer an alternative route to electronic structure design in which their excess electrons can organize into anionic electron lattice (AEL) and provide a lattice-like degree of freedom. Recent work has highlighted the standalone limit, where the AEL in YCl yields bands well described by the dice-lattice model. Here, using angle-resolved photoemission spectroscopy (ARPES), we show that LaCl, although isostructural to YCl, realizes a qualitatively different regime where the AEL is entwined with the La cation framework, producing a fully reconstructed electronic structure. Combining the ARPES result with tight-binding model analysis, we demonstrate that this radical divergence stems from the activation of direct hopping channels between the AEL and the La atomic lattice. This coupling reshapes the effective lattice geometry, reconstructs the electronic states, and modifies the associated Chern band topology, transforming the bipartite dice-lattice network in YCl into a tripartite structure in LaCl. Our findings demonstrate that the coupling between the AEL and the atomic lattice can actively shape the effective lattice geometry that governs the electronic structure. This coupling can act as a powerful tuning knob for electronic structure design that is inaccessible in conventional materials.