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Layered misfit cobaltate [Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$], which emerged asan important thermoelectric material~[A. C. Masset et al. Phys. Rev. B, 62, 166(2000)], has been explored extensively in the last decade for the exactmechanism behind its high Seebeck coefficient. Its complex crystal andelectronic structures have inhibited consensus among such investigations. Thissituation has arisen mainly due to difficulties in accurate identification ofthe chemical state, spin state, and site symmetries in its two subsystems(rocksalt [Ca$_2$CoO$_3$] and triangular [CoO$_2$]). By employing resonantphotoemission spectroscopy and x-ray absorption spectroscopy along with chargetransfer multiplet simulations (at the Co ions), we have successfullyidentified the site symmetries, valencies and spin states of the Co in bothlayers. Our site-symmetry observations explain the experimental value of thehigh Seebeck coefficient and also confirm that the carriers hop within therocksalt layer, which is in contrast to earlier reports where hopping withintriangular CoO$_2$ layer has been held responsible for the large Seebeckcoefficient.

physical review. b./physical review. b

Origin of the high Seebeck coefficient of the misfit  [Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$] cobaltate from site-specific valency and  spin-state determinations