Localised Ag+ vibrations at the origin of ultralow thermal conductivity in layered thermoelectric AgCrSe2


F. Damay, S. Petit, S. Rols, M. Braendlein, R. Daou, E. Elkaïm, F. Fauth, F. Gascoin, C. Martin, and A. Maignan

 

[SciRep]

In materials science, the substructure approach consists in imagining complex materials in which a particular property is associated with a distinct structural feature, so as to combine different chosen physical characteristics, which otherwise have little chance to coexist. Applied to thermoelectric materials, it has been used to achieve simultaneously phonon-glass and electron-crystal properties. Mostly studied for its superionic conductivity, AgCrSe2 is a naturally layered compound, which achieves very low thermal conductivity, 0.4 W.K−1.m−1 at RT (room temperature), and is considered a promising thermoelectric. The Cr atoms of the [CrSe2]∞ layer bear a spin S = 3/2, which orders below TN = 55 K. Here we report low temperature inelastic neutron scattering experiments on AgCrSe2, alongside the magnetic field evolution of its thermal and electrical transport. We observe a very low frequency mode at 3 meV, ascribed to large anharmonic displacements of the Ag+ ions in the [Ag]∞ layer, and 2D magnetic fluctuations up to 3 TN in the chromium layer. The low thermal conductivity of AgCrSe2 is attributed to acoustic phonon scattering by a regular lattice of Ag+ oscillating in quasi-2D potential wells. These findings highlight a new way to achieve localised phonon modes in a perfectly crystalline solid.


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