Carrier Mobility Modulation in Cu2Se Composites Using Coherent Cu4TiSe4 Inclusions Leads to Enhanced Thermoelectric Performance

Chen, Yixuan; Zhang, Yinying; Uher, Ctirad; Poudeu, Pierre F. P.

doi:10.1021/acsami.2c17146

Carrier Mobility Modulation in Cu₂Se Composites Using Coherent Cu₄TiSe₄ Inclusions Leads to Enhanced Thermoelectric Performance

Journal Article · Thu Dec 15 00:00:00 EST 2022 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c17146· OSTI ID:2513481

^[1]; ^[1]; Uher, Ctirad ^[1]; ^[1]

University of Michigan, Ann Arbor, MI (United States)

Carrier transport engineering in bulk semiconductors using inclusion phases often results in the deterioration of carrier mobility (μ) owing to enhanced carrier scattering at phase boundaries. Here, we show by leveraging the temperature-induced structural transition between the α-Cu₂Se and β-Cu₂Se polymorphs that the incorporation of Cu₄TiSe₄ inclusions within the Cu₂Se matrix results in a gradual large drop in the carrier mobility at temperatures below 400 K (α-Cu₂Se), whereas the carrier mobility remains unchanged at higher temperatures, where the β-Cu₂Se polymorph dominates. The sharp discrepancy in the electronic transport within the α-Cu₂Se and β-Cu₂Se matrices is associated with the formation of incoherent α-Cu₂Se/Cu₄TiSe₄ interfaces, owing to the difference in their atomic structures and lattice parameters, which results in enhanced carrier scattering. In contrast, the similarity of the Se sublattices between β-Cu₂Se and Cu₄TiSe₄ gives rise to coherent phase boundaries and good band alignment, which promote carrier transport across the interfaces. Interestingly, the different cation arrangements in Cu₄TiSe₄ and β-Cu₂Se contribute to enhanced phonon scattering at the interfaces, which leads to a reduction in the lattice thermal conductivity. The large reduction in the total thermal conductivity while preserving the high power factor of β-Cu₂Se in the (1–x)Cu₂Se/(x)Cu₄TiSe₄ composites results in an improved ZT of 1.2 at 850 K, with an average ZT of 0.84 (500–850 K) for the composite with x = 0.01. Furthermore, this work highlights the importance of structural similarity between the matrix and inclusions when designing thermoelectric materials with improved energy conversion efficiency.

View Accepted Manuscript (DOE)

Research Organization:: University of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0018941

OSTI ID:: 2513481

Alternate ID(s):: OSTI ID: 2417785

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 51 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
band alignment
carrier transport engineering
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low thermal conductivity
thermoelectric
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