Revealing nanoscale structural phase separation in La$_{3}$Ni$_{2}$O$_{7-\delta}$ single crystal via scanning near-field optical microscopy

Abstract

The discovery of superconductivity in La3Ni2O7-${\delta}$ under high pressure,with an onset critical temperature around 80 K, has sparked significant interest in the superconducting phases of Ruddlesden-Popper nickelates, Lan+1NinO3n+1. While La4Ni3O10 exhibits nearly 100% superconductivity with Tc~30 K under high pressure, magnetic susceptibility studies on La3Ni2O7-${\delta}$, however, reveal a more complex picture, indicating either filamentary superconductivity or that approximately 50% of crystal phase becomes superconducting in polycrystalline samples. In this study, we employed scattering-type scanning near-field optical microscopy to visualize nanoscale structural phase separation in La3Ni2O7-${\delta}$, identifying enhanced optical conductivity with stripes approximately 183 nm wide. These stripes run diagonally with respect to the Ni-O-Ni bond directions in the a-b plane, ruling out the possibility that they arise from impurity phases, like the '1313', '214' or '4310' structures. The dark regions and bright stripes exhibit optical conductivities ~ 22% and 29% of gold's, respectively. Additionally, we find that the bright stripes constitute about 38% of the total field of view, while the remainder consists of dark regions and the transitional region between dark regions and bright stripes. Our results suggest that optical conductivity stripes originate from nanoscale structural phase separation. In contrast, La4Ni3O10 exhibits uniform and higher optical conductivity with no observable evidence of phase separation. Thus, our study represents a pioneering effort to directly image nanoscale phase separation in Lan+1NinO3n+1 nickelates. This observation could provide crucial insights into the factors that limit the superconducting volume fraction of La3Ni2O7-${\delta}$, highlighting SNOM as a powerful probe for exploring nanoscale low-energy physics in correlated quantum materials.