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Published on: September 26, 2014
Entropy-driven dual-phase engineering in sulfides via synergizing metallic conduction and disorder-interface
Zhengyu Zhang1, Jun Li1, Zegeng Chen1
1School of Physics, Harbin Institute of Technology, Harbin 150001, China; Heilongjiang Provincial Key Laboratory of Plasma Physics and Application Technology, Harbin Institute of Technology, Harbin 150001, China.
None:
Polymetallic sulfides have emerged promising in modulating dielectric response, while their phase complexity obscures the contribution of specific elements on them, hindering dielectric optimization. Herein, we report the entropy-driven engineering that controllably synthesizes the consistent MS- and M9S8-type dual-phase (M = Fe, Co, Ni, Cr, Cu, Al) structures in medium/high-entropy sulfides, which pinpoint the role of specific metals. Entropy-driven (Cu/Al) doping optimizes metallic electron transport via filling the valley regions near the Fermi level in the density of states (DOS) to boost electron mobility, and promotes S deficiency degree, culminating in a 450% conduction loss enhancement. Concurrently, it promotes charge separation in lattice disorder areas and MS/M9S8 phase interfaces charge transfer capacities, boosting the disorder-interface polarization loss by 7.86 times. Therefore, the senary high-entropy sulfide (6-HES) achieves an improved effective absorption bandwidth (EAB) of 4.96 GHz. Particularly, it demonstrates practical potential through a genetic-algorithm-optimized metamaterial with an ultra-wide EAB of 11.06 GHz. This work deciphers the specific roles of entropy-driven (Cu/Al) doping in modulating electron structure, and establishes a general paradigm for designing programming dielectric properties in high-entropy systems.
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