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Silver Atom Off-Centering in Diamondoid Solid Solutions Causes Crystallographic Distortion and Suppresses Lattice
Hongyao Xie1, Zhi Li2, Yukun Liu2
1Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
Abstract:
The class I-III-VI2 diamondoid compounds with tetrahedral bonding are important semiconductors widely applied in optoelectronics. Understanding their heat transport properties and developing an effective method to predict the diamondoid solid solutions' thermal conductivity will help assess their impact as thermoelectrics. In this work, we investigated in detail the heat transport properties of CuGa1-InTe2 and Cu1-AgGaTe2 and found that in the Ag-alloyed solid solutions, the Ag atom off-centering effect results in crystallographic distortion and extra strong acoustic-optical phonon scattering and an extremely low lattice thermal conductivity. Moreover, we integrate the alloy scattering and the off-centering effect with the crystallographic distortion parameter to develop a modified Klemens model that predicts the thermal conductivity of diamondoid solid solutions. Finally, we demonstrate that Cu1-AgGaTe2 solid solutions are promising p-type thermoelectric materials, with a maximum ZT of 1.23 at 850 K for Cu0.58Ag0.4GaTe2.
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