Epitaxial strain tuning of electronic and spin excitations in La$_3$Ni$_2$O$_7$ thin films (2502.03178v2)

Abstract: The discovery of ambient-pressure superconductivity with $T_{c,\text{onset}} > 40$ K in La$3$Ni$_2$O$_7$ (LNO) thin films under in-plane biaxial compressive strain underscores the pivotal role of epitaxial strain in tuning exotic electronic states and provides a unique platform for investigating the superconducting mechanisms in nickelate superconductors. Here, we use resonant inelastic X-ray scattering (RIXS) to probe the strain-dependent electronic and spin excitations in LNO thin films with biaxial strain ranging from $\epsilon\approx-1.04\%$ to $1.91\%$. Compared with the bulk crystal, the LNO thin film grown on LaAlO$_3$ (with $\epsilon\approx-1.04\%$) exhibits similar $dd$ excitations and enhanced spin excitation bandwidth. In contrast, the 0.4 eV and 1.6 eV $dd$ excitations associated with the Ni 3$d{z^2}$ orbital, along with the spin excitations, are significantly suppressed in the film grown on SrTiO$3$ ($\varepsilon\approx1.91\%$). The $c$-axis compression and the reduced out-of-plane Ni-O-Ni bond angle, induced by in-plane tensile strain in LNO/SrTiO$_3$ broaden the Ni 3$d{z^2}$ bandwidth and decrease the Ni 3$d_{z^2}$-O 2$p_{z}$ hybridization, thereby suppressing the $dd$ excitations. The evolution of spin excitations reflects significant changes in the interlayer exchange coupling $J_z$, which can be attributed to the strain-tuned Ni-O-Ni bond angle. Since superconductivity is observed only in films with in-plane compressive strain ($\epsilon\sim-2\%$), the strain-dependent spin correlations align with the emergence of superconductivity, providing indirect evidence for spin-fluctuation-mediated unconventional superconductivity in LNO.