Supplementary Material

We present the synthetic procedure for AzoEA, XRD data, a more detailed description of the fifth-order response function, four-wave mixing signals acquired with layered perovskites systems incorporating stilbene and methyl phenyl ammonium spacer cations, additional fifth-order coherent Raman data sets used to compute statistics for fitting parameters, experimental data demonstrating photostability, and further discussion of numerical Fourier transformations.