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Poudeu, Pierre P.

Publications and source records attributed to Poudeu, Pierre P..

Ultrafine Interwoven Dendritic Cu 2 Se/CuFeSe 2 Composites with Enhanced Thermoelectric Performance

As an effort to develop high-performance and stable copper chalcogenide thermoelectrics, several (1-x)Cu 2 Se/(x)CuFeSe 2 composites were successfully synthesized via a one-step solid-state transformation of CuSe 2 template. Uniform ultrafine dendritic structures consisting of interweaving Cu 2 Se and CuFeSe 2 nanofibers were observed in samples with low Fe content (0.05 ≤ x ≤ 0.1). Increasing the Fe content to x = 0.5 led to phase segregation into Cu 2 Se-rich region with embedded CuFeSe 2 fine structures interwoven with CuFeSe 2 -rich region containing Cu 2 Se nanofibers. The formation of such an entwined dendritic structure is believed to arise from the temperature-dependent solubility of CuFeSe 2 in the Cu 2 Se matrix. The dynamic dissolution of CuFeSe 2 into the Cu 2 Se at high temperatures leads to temperature-dependent doping of the Cu 2 Se matrix, enabling drastic enhancements of thermoelectric power factor at high temperatures. As a result, such a strategy is expected to be a powerful tool for properties modulation in thermoelectric materials.

36 MATERIALS SCIENCE↗

Nanoscale Engineering of Polymorphism in Cu 2 Se-Based Composites

Crystal polymorphism selection during synthesis is extremely challenging. However, promoting the formation of a specific metastable polymorph enables modulation of the functional properties of phase-change materials through alteration of the relative abundance of various polymorphs. Here, we demonstrate the stabilization of the superionic β-Cu 2 Se phase under ambient conditions and the direct control over the relative ratio between the α-Cu 2 Se and β-Cu 2 Se polymorphs in (x)CuGaSe 2 /(1-x)Cu 2 Se composites using CuGaSe 2 nanoseeds. Here, we found that the small lattice mismatch between β-Cu 2 Se (cubic) and the ab plane of tetragonal CuGaSe 2 nanoseeds promotes the formation of low-energy coherent CuGaSe 2 /β-Cu 2 Se interfaces leading to preferential stabilization of β-Cu 2 Se. Astonishingly, the hierarchical microstructure of the resulting composites enables a remarkable decoupling of charge and heat transport, which is manifested by a breakdown of the Wiedemann-Franz law

36 MATERIALS SCIENCE↗

Semiconducting High-Entropy Chalcogenide Alloys with Ambi-ionic Entropy Stabilization and Ambipolar Doping

Entropy stabilization is a novel materials-design paradigm to realize new compounds with widely tunable properties. However, almost all entropy-stabilized materials so far are either conducting metals or insulating ceramics, with a clear dearth in the semiconducting regime. Here, a new class of the multi-cationic and -anionic entropy-stabilized chalcogenide alloys based on the (Ge,Sn,Pb)(S,Se,Te) formula are synthesized and characterized experimentally. The con-figurational entropy from the disorder of both the anion and the cation sublattices reaches a record value of ~2.2 R mol -1 for the equimolar composition and stabilizes the single-phase solid solution. Theoretical calculations and experiments both show that the synthesized alloys are thermodynamically stable at the growth temperature and kinetically metastable at room temperature, segregating by spinodal decomposition at moderate temperatures. In conclusion, doping and electronic transport measurements verify that the synthesized materials are ambipolarly dopable semiconductors, which paves the way for the wider adoption of entropy-stabilized chalcogenide alloys in functional applications.

36 MATERIALS SCIENCE↗