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Negative compressibility is a sign of thermodynamic instability of open ornon-equilibrium systems. In quantum materials consisting of multiple mutuallycoupled subsystems, the compressibility of one subsystem can be negative if itis countered by positive compressibility of the others. Manifestations of thiseffect have so far been limited to low-dimensional dilute electron systems.Here we present evidence from angle-resolved photoemission spectroscopy (ARPES)for negative electronic compressibility (NEC) in the quasi-three-dimensional(3D) spin-orbit correlated metal (Sr1-xLax)3Ir2O7. Increased electron fillingaccompanies an anomalous decrease of the chemical potential, as indicated bythe overall movement of the deep valence bands. Such anomaly, suggestive ofNEC, is shown to be primarily driven by the lowering in energy of theconduction band as the correlated bandgap reduces. Our finding points to adistinct pathway towards an uncharted territory of NEC featuring bulkcorrelated metals with unique potential for applications in low-powernanoelectronics and novel metamaterials.

Spectroscopic evidence for negative electronic compressibility in a quasi-three-dimensional spin-orbit correlated metal