title: Designing high-performance layered thermoelectric materials through orbital engineering.
abstract: Thermoelectric technology, which possesses potential application in recycling industrial waste heat as energy, calls for novel high-performance materials. The systematic exploration of novel thermoelectric materials with excellent electronic transport properties is severely hindered by limited insight into the underlying bonding orbitals of atomic structures. Here we propose a simple yet successful strategy to discover and design high-performance layered thermoelectric materials through minimizing the crystal field splitting energy of orbitals to realize high orbital degeneracy. The approach naturally leads to design maps for optimizing the thermoelectric power factor through forming solid solutions and biaxial strain. Using this approach, we predict a series of potential thermoelectric candidates from layered CaAl2Si2-type Zintl compounds. Several of them contain nontoxic, low-cost and earth-abundant elements. Moreover, the approach can be extended to several other non-cubic materials, thereby substantially accelerating the screening and design of new thermoelectric materials.
authors.affiliation: Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, Langelandsgade 140, Aarhus DK-8000, Denmark.
authors.forename: Jiawei
authors.initials: J
authors.lastname: Zhang
authors.affiliation: Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, Langelandsgade 140, Aarhus DK-8000, Denmark.
authors.forename: Lirong
authors.initials: L
authors.lastname: Song
authors.affiliation: Computational Materials Discovery, ICAMS, Ruhr-Universität Bochum, Bochum 44801, Germany.
authors.forename: Georg K H
authors.initials: GK
authors.lastname: Madsen
authors.affiliation: Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, Langelandsgade 140, Aarhus DK-8000, Denmark.
authors.forename: Karl F F
authors.initials: KF
authors.lastname: Fischer
authors.affiliation: State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, China.|Materials Genome Institute, Shanghai University, Shanghai 200444, China.
authors.forename: Wenqing
authors.initials: W
authors.lastname: Zhang
authors.affiliation: State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, China.
authors.forename: Xun
authors.initials: X
authors.lastname: Shi
authors.affiliation: Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University, Langelandsgade 140, Aarhus DK-8000, Denmark.
authors.forename: Bo B
authors.initials: BB
authors.lastname: Iversen