An x-ray photoelectron spectroscopic (XPS) study of a thin film of S2N2 at −100 °C, involving the valence band, core-level and core-level shakeup, and energy-loss spectra, is reported. The results are analyzed in terms of a molecular orbital model and previous optical data. In addition, the thermally induced solid state polymerization of S2N2 to metallic (SN)x was studied by recording the XPS spectra at −40, 0, and 20 °C. The valence band data show changes of the highest filled molecular orbitals of S2N2, consistent with the process of polymerization to the metallic state.

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Earlier work based on specular reflectance measurements on single crystals of the cyclic polynitramine known as RDX indicated the presence of an absorption band near 340 nm. Since a similar band was not observed in dilute solution, the absorption was attributed to the formation of a charge-transfer self-complex in the crystalline state. This work compares measurements of the transmittance of thin single crystals and new specular reflectance measurements to absorption spectra of saturated solutions of the polynitramines known as RDX and HMX. The results are found to support the charge-transfer self-complex hypothesis.

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