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Valence fluctuations of Fe^(2+) and Fe^(3+) were studied in a solid solution of Li_xFePO_4 by nuclear resonant forward scattering of synchrotron x rays while the sample was heated in a diamond-anvil pressure cell. The spectra acquired at different temperatures and pressures were analyzed for the frequencies of valence changes using the Blume-Tjon model of a system with a fluctuating Hamiltonian. These frequencies were analyzed to obtain activation enthalpies and an activation volume for polaron hopping. There was a large suppression of hopping frequency with pressure, giving an activation volume for polaron hopping of 5.8±0.7 A^ 3. This large, positive value is typical of ion diffusion, which indicates correlated motions of polarons and Li^+ ions that alter the dynamics of both. Monte Carlo simulations were used to estimate the strength of the polaron-ion interaction energy.

physical review. b, condensed matter and materials physics

Polaron-ion correlations in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi mathvariant="normal">Li</mml:mi><mml:mi>x</mml:mi></mml:msub><mml:msub><mml:mi mathvariant="normal">FePO</mml:mi><mml:mn>4</mml:mn></mml:msub></mml:math>studied by x-ray nuclear resonant forward scattering at elevated pressure and temperature

Polaron-ion correlations inLixFePO4studied by x-ray nuclear resonant forward scattering at elevated pressure and temperature