Electronic Reconstruction across the Tilt-Free Transition in La${}_3$Ni${}_2$O${}_7$

Abstract

The emergence of high-$T_c$ superconductivity in pressurized La${}_3$Ni${}_2$O${}_7$ is intimately linked to a structural transition that suppresses the tilts of the NiO${}_6$ octahedra, yet its impact on the electronic structure remains poorly understood. Here, we probe the electronic response across this tilt-free transition at $T_{st}\simeq 544$ K using broadband infrared-to-visible reflectivity at ambient pressure, covering photon energies from 15 meV to 3.2 eV. We observe a pronounced redistribution of spectral weight over an exceptionally broad energy range, with spectral weight transferred from excitations between 1 and 3 eV toward low-energy excitations below 1 eV. Most strikingly, two low-energy interband excitations progressively converge and merge upon entering the tilt-free phase, revealing a substantial reconstruction of the finite-energy electronic structure. These changes point to a reconstruction of the bilayer Ni $3d_{z^2}$-derived electronic states, whose interlayer coupling is central to proposed mechanisms of superconductivity in La${}_3$Ni${}_2$O${}_7$. Our results establish the tilt-free transition as a direct route to reorganizing the electronic degrees of freedom implicated in high-$T_c$ superconductivity and provide an ambient-pressure reference for the electronic structure of the superconducting state.