Alloy-Free Band Gap Tuning across the Visible Spectrum

We present evidence, from theory and experiment, that ZnSnN_{2} and MgSnN_{2} can be used to match the band gap of InGaN without alloying-by exploiting cation disorder in a controlled fashion. We base this on the determination of S, the long-range order parameter of the cation sublattice, for a series of epitaxial thin films of ZnSnN_{2} and MgSnN_{2} using three different techniques: x-ray diffraction, Raman spectroscopy, and in situ electron diffraction. We observe a linear relationship between S^{2} and the optical band gap of both ZnSnN_{2} (1.12-1.98 eV) and MgSnN_{2} (1.87-3.43 eV). The results clearly demonstrate the correlation between controlled heterovalent cation ordering and the optical band gap, which applies to a broad group of emerging ternary heterovalent compounds and has implications for similar trends in other material properties besides the band gap.