Oxygen nonstoichiometry effects in spin Seebeck insulating Y3−xPrxFe5O12+ δ materials

Yttrium iron garnet (Y3Fe5O12) and its derivatives are ferrimagnetic spin Seebeck insulating materials crucial for the spin transport based phenomena such as the spin Seebeck effect (SSE) and spin Hall magnetoresistance. Structure–property correlation studies of such materials under different conditions are useful for optimizing the relevant constraint in the existed phenomena. The usage of Y3Fe5O12 type materials over the broad range of temperature conditions (27–450 °C) in SSE is under study. We report here the structure–property correlation in spin Seebeck insulating Y3−xPrxFe5O12+δ oxides as a representative material and introduce the additional degrees of freedom in the crystal system relevant to the spin transport based phenomena under high temperature conditions. The natural tendency of having oxygen nonstoichiometry in an iron garnet family of materials strengthens the Fe–O–Fe superexchange interaction, which, in turn, tends to increase the spin voltage correlated magnetic parameters. The analysis of experimental high temperature neutron diffraction data (over 27–450 °C) reveals the oxide ion nonstoichiometry and excess oxide ion transport pathways at moderate temperature 150 °C in the crystal lattices of studied garnet materials. Oxide ion nonstoichiometry, ionic transport, and electron hopping in crystal lattices cause a tremendous variation of electrical conductivity (10−11–10−2 S cm−1) over a moderate change of temperature (27–450 °C). The occurrence of electrical transport in the required thermal gradient over the garnet material in SSE can evoke the additional degrees of freedom in the usage of such materials at high temperatures. The present work provides a new outlook in terms of structure–property correlation for spin transport based materials.