Seebeck coefficient in the high temperature limit Public Deposited

http://ir.library.oregonstate.edu/concern/graduate_thesis_or_dissertations/cz30pw50n

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  • The Seebeck coefficient is examined in the high temperature limit, using an approach based on a grand partition function containing Hubbard Hamiltonian interaction terms. Although the carriers of interest occupy localized Wannier states, this work is prefaced by the case of delocalized Bloch states, which is examined using Boltzmann transport, and yields the Seebeck coefficient in the free-particle limit. Transfer matrix methods are used to consider both on-site and nearest-neighbor interactions for a Hubbard chain. Examination of results in limiting cases, specifically those of zero or infinite interactions, agree with those calculated in literature using a combinatoric approach. The least-bias approach is applied to the two-atom system for the case of CuSc₁₋ₓMgₓO₂₊y. Results are in reasonable agreement with the experimental Seebeck data for this material. It is determined that the double occupancy term in the grand partition function dominates any single occupancy contribution, thus the theoretical result for the temperature-dependent Seebeck coefficient for this system is a function of an intercalated atom concentration term, ρ, and a binding energy parameter, ε, for sites on oxygen atoms. Comparison to experimental data demonstrates that ε decreases as ρ increases, suggesting the formation of an oxygen band. Langmuir's model of surface adsorption is applied to the copper layer, treating this as a copper surface to which a free gas, oxygen, is adsorbed. Analysis using this model verifies the correlation between the oxygen pressure at which the samples are intercalated and the intercalated atom (oxygen) concentration. This conclusion provides a context for interpreting ρ that originated in the least-biased approach.
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