Bulk superconductivity up to 96 K in pressurized nickelate single crystals

Recently, the Ruddlesden-Popper bilayer nickelate $La_3Ni_2O_7$ has emerged as a superconductor with a transition temperature ($T_c$) of approximately 80 K above 14 GPa (Refs. 1-3). Achieving higher $T_c$ in nickelate superconductors, along with the synthesis of reproducible high-quality single crystals without relying on high-oxygen-pressure growth conditions, remains a significant challenge$^{[4-7]}$. Here we report superconductivity up to 96 K under high pressure in bilayer nickelate single crystals synthesized at ambient pressure. Energy-dispersive spectroscopy, single-crystal X-ray diffraction, nuclear quadrupole resonance and scanning transmission electron microscopy evidenced high crystal quality of the flux-grown $La_2SmNi_2O_{7-{\delta}}$ single crystals. $La_2SmNi_2O_7$ exhibits clear bulk superconductivity, including zero resistivity ($T_{c,max}^{onset}$ = 92 K and $T_{c,max}^{zero}$ = 73 K at 21.6 GPa) and the Meissner effect ($T_c$= 60 K at 20.6 GPa). A low-temperature high-pressure structural study indicates that both monoclinic and tetragonal structures can support superconductivity in this bilayer nickelate. Furthermore, we established a correlation between higher $T_c$ under high pressures and larger in-plane lattice distortion under ambient conditions, corroborated by observing even higher $T_c^{onset}$ of 96 K in $La_{1.57}Sm_{1.43}Ni_2O_{7-{\delta}}$. This study overcomes key limitations in growing nickelate superconductor crystals, resolves the crystal structure in the superconducting state and demonstrates an effective pathway towards achieving higher $T_c$.