Microscopic Evidence of Charge- and Spin-Density Waves in La₃Ni₂O_7–δ Revealed by ¹³⁹La-NQR

Abstract The recent discovery of superconductivity in La 3 Ni 2 O 7– δ with a transition temperature T c close to 80 K at high pressures has attracted significant attention, due particularly to a possible density wave (DW) transition occurring near the superconducting dome. Identifying the type of DW order is crucial for understanding the origin of superconductivity in this system. However, owing to the presence of La 4 Ni 3 O 10 and other intergrowth phases in La 3 Ni 2 O 7– δ samples, extracting the intrinsic information from the La 3 Ni 2 O 7 phase is challenging. In this study, we employed 139 La nuclear quadrupole resonance (NQR) measurements to eliminate the influence of other structural phases in the sample and obtain microscopic insights into the DW transition in La 3 Ni 2 O 7– δ . Below the DW transition temperature T DW ∼ 153 K, we observe a distinct splitting in the ±5/2 ↔ ±7/2 transition of the NQR resonance peak at the La(2) site, while only a line broadening is seen in the ±3/2 ↔ ±5/2 transition peak. Through further analysis of the spectra, we show that the line splitting is due to a unidirectional charge modulation. A magnetic line broadening is also observed below T DW , accompanied by a large enhancement of the spin-lattice relaxation rate, indicating the formation of magnetically ordered moments in the DW state. Our results suggest a simultaneous formation of charge- and spin-density wave orders in La 3 Ni 2 O 7– δ , thereby offering critical insights into the electronic correlations in Ni-based superconductors.