Spin鈥揕attice Relaxation in Bismuth Chalcogenides

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• 作者：Robert E. Taylor ; Belinda Leung ; Michael P. Lake ; Louis-S. Bouchard
• 刊名：The Journal of Physical Chemistry C
• 出版年：2012
• 出版时间：August 16, 2012
• 年：2012
• 卷：116
• 期：32
• 页码：17300-17305
• 全文大小：319K
• 年卷期：v.116,no.32(August 16, 2012)
• ISSN：1932-7455

文摘

Bismuth chalcogenides Bi₂Se₃ and Bi₂Te₃ are semiconductors that can be both thermoelectric materials (TEs) and topological insulators (TIs). Lattice defects arising from vacancies, impurities, or dopants in these materials are important in that they provide the charge carriers in TE applications and compromise the performance of these materials as TIs. We present the first solid-state nuclear magnetic resonance (NMR) study of the ⁷⁷Se and ¹²⁵Te NMR resonances in polycrystalline powders of Bi₂Se₃ and Bi₂Te₃, respectively. The spin鈥搇attice (T₁) relaxation is modeled by at most two exponentials. Within the framework of this model, the NMR measurement is sensitive to the distribution of native defects within these materials. One component corresponds to a stoichiometric fraction, an insulator with a very long T₁, whereas the other component is attributed to a sample fraction with high defect content with a short T₁ resulting from interaction with the conduction carriers. The absence of a very long T₁ in the bismuth telluride suggests defects throughout the sample. For the bismuth selenide, defect regions segregate into domains. We also find a substantial difference in the short T₁ component for ¹²⁵Te nuclei (76 ms) and ⁷⁷Se (0.63 s) despite the fact that these materials have nearly identical lattice structures and chemical and physical properties. Investigations of the NMR shift and Korringa law indicate that the coupling to the conduction band electrons at the chalcogenide sites is much stronger in the telluride. The results are consistent with a stronger spin鈥搊rbit coupling (SOC) to the p-band electrons in the telluride. If most parameters of a given material are kept equal, then this type of experiment could provide a useful probe of SOC in engineered TI materials.