Large Enhancements of Thermopower and Carrier Mobility in Quantum Dot Engineered Bulk Semiconductors

• Published in: Journal of the American Chemical Society Vol. 135; no. 20; pp. 7486 - 7495
• Main Authors: Liu, Yuanfeng, Sahoo, Pranati, Makongo, Julien P. A, Zhou, Xiaoyuan, Kim, Sung-Joo, Chi, Hang, Uher, Ctirad, Pan, Xiaoqing, Poudeu, Pierre F. P
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 22.05.2013
• Subjects: Particle Size; Quantum Dots; Semiconductors; Surface Properties; Temperature
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/ja311059m

The thermopower (S) and electrical conductivity (σ) in conventional semiconductors are coupled adversely through the carriers’ density (n) making it difficult to achieve meaningful simultaneous improvements in both electronic properties through doping and/or substitutional chemistry. Here, we demonstrate the effectiveness of coherently embedded full-Heusler (FH) quantum dots (QDs) in tailoring the density, mobility, and effective mass of charge carriers in the n-type Ti0.1Zr0.9NiSn half-Heusler matrix. We propose that the embedded FH QD forms a potential barrier at the interface with the matrix due to the offset of their conduction band minima. This potential barrier discriminates existing charge carriers from the conduction band of the matrix with respect to their relative energy leading to simultaneous large enhancements of the thermopower (up to 200%) and carrier mobility (up to 43%) of the resulting Ti0.1Zr0.9Ni1+x Sn nanocomposites. The improvement in S with increasing mole fraction of the FH-QDs arises from a drastic reduction (up to 250%) in the effective carrier density coupled with an increase in the carrier’s effective mass (m*), whereas the surprising enhancement in the mobility (μ) is attributed to an increase in the carrier’s relaxation time (τ). This strategy to manipulate the transport behavior of existing ensembles of charge carriers within a bulk semiconductor using QDs is very promising and could pave the way to a new generation of high figure of merit thermoelectric materials.