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The natural periodic stacking of symmetry-inequivalent planes in layeredcompounds can lead to the formation of natural superlattices; albeit close intotal energy, (thus in their thermodynamic stability), such polytypesuperlattices can exhibit different structural symmetries, thus have markedlydifferent electronic properties which can in turn be used as "structuralmarkers". We illustrate this general principle on the layered LaOBiS2 compoundwhere density-functional theory (DFT) calculations on the (BiS2)/(LaO)/(BiS2)polytype superlattices reveal both qualitatively and quantitatively distinctelectronic structure markers associated with the Rashba physics, yet the totalenergies are only ~ 0.1 meV apart. This opens the exciting possibility ofidentifying subtle structural features via electronic markers. We show that thepattern of removal of band degeneracies in different polytypes by the differentforms of symmetry breaking leads to new Rashba "mini gaps" with characteristicRashba parameters that can be determined from spectroscopy, thereby narrowingdown the physically possible polytypes. By identifying these distinctDFT-predicted fingerprints via ARPES measurements on LaBiOS2 we found thedominant polytype with small amounts of mixtures of other polytypes. Thisconclusion, consistent with neutron scattering results, establishes ARPESdetection of theoretically established electronic markers as a powerful tool todelineate energetically quasidegenerate polytypes.

Predicted electronic markers for polytypes of LaOBiS2 examined via angular resolved photoemission spectroscopy