TY - JOUR AU - Eun, Su Min AU - Lee, Eui Seon AU - Oh, Sung-Tag AU - Jung, Chanwon AU - Choi, Byung Joon PY - 2026 TI - Decoupling carrier and phonon scattering in n-type Bi2Te2.7Se0.3 thermoelectrics via atomic layer deposition of TiO2 nanoshells JO - Journal of Materiomics SN - 2352-8478 VL - 12 IS - 5 AB - Breaking the intrinsic coupling between carrier and phonon transport remains a critical bottleneck limiting further enhancement of Bi2Te3-based thermoelectric materials. Herein, we report an interface engineering strategy employing atomic layer deposition (ALD) to construct TiO2–x nanoshells on Bi2Te2.7Se0.3 powders, followed by spark plasma sintering to form engineered interfacial layers in bulk pellets. By controlling the ALD cycle number, the thickness, crystallinity, and dispersion of TiO2–x interfaces were tuned to optimize energy filtering and phonon scattering. Conformal amorphous TiO2–x coatings with thicknesses ranging from 1.5 nm to 8.0 nm were obtained, whereas excessive deposition led to agglomeration and weakened the interfacial effects. The optimized interface enabled selective scattering of low-energy carriers while preserving carrier mobility, resulting in an enhanced Seebeck coefficient without severe loss of electrical conductivity. Simultaneously, enhanced phonon scattering effectively reduced lattice thermal conductivity. The optimized specimen fabricated with 100 ALD cycles achieved the best balance between electrical and thermal transport, yielding a maximum zT of 0.92 at 460 K, corresponding to a 27% improvement compared with pristine Bi2Te2.7Se0.3 bulk pellet. This work demonstrates that precise ALD-enabled interface engineering provides a scalable route to decouple carrier and phonon transport for high-performance thermoelectrics. UR - https://doi.org/10.1016/j.jmat.2026.101279 DO - 10.1016/j.jmat.2026.101279