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Lattice thermal conductivity of topological insulator Bi<inf>2</inf>Se<inf>3</inf> nanocrystals: comparison from theoretical and experimental

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01-01-2023
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Lattice thermal conductivity (κL) calculations using the Wiedemann-Franz law involve electrical conductivity, which introduces an error in the actual value of κL. We have adopted a non-contact measurement technique and calculated the κL from the temperature and power-dependent Raman spectra of the Bi2Se3 nanocrystals with truncated hexagon plate morphology stabilized in a hexagonal crystal structure. The hexagon plates of Bi2Se3 are 37 to 55 nm thick with lateral dimensions around 550 nm. These Bi2Se3 nanocrystals show three Raman lines, which agree with the theoretical prediction of A11g, E2g and A21g modes. Although the first-order thermal coefficient (−0.016) of Bi2Se3 nanocrystals is quite low, the room temperature κL ∼1.72 W m−1 K−1 is close to the value obtained from the simulation adopting a three-phonon process. The phonon lifetime of Bi2Se3 nanocrystals observed between ∼0.2 ps and 2 ps confirmed carrier-carrier thermalization with a small contribution from electron-electron and intraband electron-longitudinal-optical-phonon relaxation. The variations of phonon lifetime, Gruneisen parameter and κL of the mode frequencies outline the crucial role of the anharmonicity and acoustic-optical phonon scattering in reducing the κL of Bi2Se3. The non-contact measurements and relevant thermal property parameters open up exciting opportunities to address the anharmonic effects in other thermoelectric materials for obtaining a high figure of merit.
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