Crossover of high-energy spin fluctuations from collective triplons to localized magnetic excitations in Sr14−xCaxCu24O41 ladder

We studied the magnetic excitations in the quasi-one-dimensional (q-1D) ladder subsystem of Sr_14−xCa_xCu₂₄O₄₁ (SCCO) using Cu L₃-edge resonant inelastic X-ray scattering (RIXS). By comparing momentum-resolved RIXS spectra with high (x = 12.2) and without (x = 0) Ca content, we track the evolution of the magnetic excitations from collective two-triplon (2 T) excitations (x = 0) to weakly- dispersive gapped modes at an energy of 280 meV (x = 12.2). Density matrix renormalization group (DMRG) calculations of the RIXS response in the doped ladders suggest that the flat magnetic dispersion and damped excitation profile observed at x = 12.2 originates from enhanced hole localization. This interpretation is supported by polarization-dependent RIXS measurements, where we disentangle the spin-conserving ΔS = 0 scattering from the predominant ΔS = 1 spin-flip signal in the RIXS spectra. The results show that the low-energy weight in the ΔS = 0 channel is depleted when Sr is replaced by Ca, consistent with a reduced carrier mobility. Our results demonstrate that off-ladder impurities can affect both the low-energy magnetic excitations and superconducting correlations in the CuO₄ plaquettes. Finally, our study characterizes the magnetic and charge fluctuations in the phase from which superconductivity emerges in SCCO at elevated pressures.