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Nanolaminated materials exhibit characteristic magnetic, mechanical, andthermoelectric properties, with large contemporary scientific and technologicalinterest. Here, we report on the anisotropic Seebeck coefficient innanolaminated Ti3SiC2 single-crystal thin films and trace the origin toanisotropies in element-specific electronic states. In bulk polycrystallineform, Ti3SiC2 has a virtually zero Seebeck coefficient over a wide temperaturerange. In contrast, we find that the in-plane (basal ab) Seebeck coefficient ofTi3SiC2, measured on single-crystal films has a substantial and positive valueof 4-6 muV/K. Employing a combination of polarized angle-dependent x-rayspectroscopy and density functional theory we directly show electronicstructure anisotropy in inherently nanolaminated Ti3SiC2 single-crystal thinfilms as a model system. The density of Ti 3d and C 2p states at the Fermilevel in the basal ab-plane is about 40 % higher than along the c-axis. TheSeebeck coefficient is related to electron and hole-like bands close to theFermi level but in contrast to ground state density functional theory modeling,the electronic structure is also influenced by phonons that need to be takeninto account. Positive contribution to the Seebeck coefficient of theelement-specific electronic occupations in the basal plane is compensated by 73% enhanced Si 3d electronic states across the laminate plane that give rise toa negative Seebeck coefficient in that direction. Strong phonon vibration modeswith three to four times higher frequency along the c-axis than along the basalab-plane also influence the electronic population and the measured spectra bythe asymmetric average displacements of the Si atoms. These results constituteexperimental evidence explaining why the average Seebeck coefficient of Ti3SiC2in polycrystals is negligible over a wide temperature range.

physical review. b, condensed matter and materials physics

The electronic-structure origin of the anisotropic thermopower of  nanolaminated Ti3SiC2 determined by polarized x-ray spectroscopy and Seebeck  measurements