Fig. 3: Experimental evidence of sulphur oxidation and disulphide bond formation.

a, b XANES spectra at the Mn K-edge (a) and S K-edge (b) measured for pristine Sr2MnO2Cu1.5S2 (black), Sr2MnO2Cu1.33S2 (blue, reproduced from the data published in ref. 15), and the collapsed phase (red). Dotted lines represent the absorption edges of reference standards MnO and Mn2O3, which correspond to the lowest-energy maxima on the d(χμ(E))/dE plot (See ref. 30 for their spectra). c Inverse molar susceptibility 1/χmol of the collapsed phase plotted against temperature (2 K ≤ T ≤ 300 K). Magnetisation (emu) was measured at the applied field H = 100 Oe after zero field cooling (ZFC) and converted into 1/χmol (emu-1 mol Oe) supposing the tentative formula Sr2MnO2S2 (molar mass = 326.31). The linear region (120 K ≤ T ≤ 280 K) of the obtained 1/χmol – T plot was fitted by Curie–Weiss law 1/χmol = (T/C) – (θ/C), where C and θ represented the Curie and Weiss constants, respectively. See Supplementary Fig. 17 for other magnetic data. d Raman spectra of Sr2MnO2Cu1.5S2 (black) and the collapsed phase (red). The measurement was performed under air with excitation wavelength λex = 532 nm. See Supplementary Fig. 19 for the spectra measured at λex = 785 nm.