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Coupling between thermal and charge transport in crystalline materials has always been one of the greatest challenges in understanding the underlying physics of thermoelectric materials. In this sense, CaO(CaMnO 3 )  m  Ruddlesden-Popper layered perovskites, comprising m perovskite subcells separated by CaO planes, exhibit intriguing thermal and electronic transport properties that can be tuned by altering their crystal periodicities. Applying the well-established phonon glass electron crystal (PGEC) concept enables us to increase the transparency of these CaO planes to electron transport at the same time while preserving their opacity to phonon transport. First-principles calculations indicate that the total local potential at CaO planes, where Y substitutes for Ca, is lower by ca. 50% compared to La substitution. Measurements of the electrical conductivity and Seebeck coefficients for Ca 2- x  R  x  MnO 4 (R = La or Y; x = 0.01, 0.05, 0.1, and 0.15) bulk materials in the range of 300-1000 K confirm that compounds doped with Y exhibit higher electrical conductivity values than their La-doped counterparts. We attribute this to lower polaron hopping energy values (up to 23%) evaluated using the small polaron hopping model. This study introduces an original way to employ the PGEC approach for thermoelectric oxides.

Enhanced Charge Transport in Ca2MnO4-Layered Perovskites by Point Defect Engineering

Enhanced Charge Transport in Ca₂MnO₄-Layered Perovskites by Point Defect Engineering