Superconductivity and phase diagram in Sr-doped La$_{3-x}$Sr$_{x}$Ni$_2$O$_7$ thin films

Abstract: Recent studies have demonstrated ambient pressure superconductivity in compressively strained La${3}$Ni${2}$O${7}$ thin films, yet the phase diagram of heterovalent doping$-$critical for advancing the field$-$remains unexplored. Here, we report superconductivity in Sr$^{2+}$-doped La${3-x}$Sr${x}$Ni$_2$O$_7$ films synthesized via molecular beam epitaxy with ozone-assisted post-annealing. The superconducting transition temperature ($T{\mathrm{c}}$) follows an asymmetric dome-like profile, persisting across a wide doping range ($0 \leq x \leq 0.21$) before diminishing at $x \approx 0.38$. Optimally doped films ($x = 0.09$) achieve $T_{\mathrm{c}}$ of $\sim$ 42 K, with high critical current ($J_{\mathrm{c}} > 1.4$ $\mathrm{kA/cm^{2}}$ at 2 K) and upper critical fields ($\mu_{0}H_{\mathrm{c,\parallel}}(0)= 83.7$ $\mathrm{T}$, $\mu_{0}H_{\mathrm{c,\perp}}(0)= 110.3$ $\mathrm{T}$), comparable to reported La${3-x}$Pr${x}$Ni$2$O$_7$ films. Scanning transmission electron microscopy reveals oxygen vacancies predominantly occupy at planar NiO${2}$ sites$-$unlike apical-site vacancies in bulk samples$-$due to Coulomb repulsion destabilizing planar oxygen under compressive strain. Additionally, the elongated out-of-plane Ni-O bonds, exceeding those in pressurized bulk samples by $4\%$, likely weaken the interlayer $d_{z^2}$ coupling, thus contributing to the reduced $T_{\mathrm{c}}$ in strained films. This work establishes heterovalent Sr$^{2+}$ doping as a robust tuning parameter for nickelate superconductivity, unveiling a unique phase diagram topology.