Topological semimetals represent a novel class of quantum materials displaying non‐trivial topological states that host Dirac/Weyl fermions. The intersection of Dirac/Weyl points gives rise to essential properties in a wide range of innovative transport phenomena, including extreme magnetoresistance, high mobilities, weak antilocalization, electron hydrodynamics, and various electro‐optical phenomena. In this study, the electronic, transport, phonon scattering, and interrelationships are explored in single crystals of the topological semimetal HfAs2. It reveals a weak antilocalization effect at low temperatures with high carrier density, which is attributed to perfectly compensated topological bulk and surface states. The angle‐resolved photoemission spectroscopy (ARPES) results show anisotropic Fermi surfaces and surface states indicative of the topological semimetal, further confirmed by first‐principle density functional theory (DFT) calculations. Moreover, the lattice dynamics in HfAs2are investigated both with the Raman scattering and density functional theory. The phonon dispersion, density of states, lattice thermal conductivity, and the phonon lifetimes are computed to support the experimental findings. The softening of phonons, the broadening of Raman modes, and the reduction of phonon lifetimes with temperature suggest the enhancement of phonon anharmonicity in this new topological material, which is crucial for boosting the thermoelectric performance of topological semimetals.
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Topological insulators and semimetals have been shown to possess intriguing thermoelectric properties promising for energy harvesting and cooling applications. However, thermoelectric transport associated with the Fermi arc topological surface states on topological Dirac semimetals remains less explored. This work systematically examines thermoelectric transport in a series of topological Dirac semimetal Cd3As2thin films grown by molecular beam epitaxy. Surprisingly, significantly enhanced Seebeck effect and anomalous Nernst effect are found at cryogenic temperatures when the Cd3As2layer is thin. In particular, a peak Seebeck coefficient of nearly 500 µV K−1and a corresponding thermoelectric power factor over 30 mW K−2 m−1are observed at 5 K in a 25‐nm‐thick sample. Combining angle‐dependent quantum oscillation analysis, magnetothermoelectric measurement, transport modeling, and first‐principles simulation, the contributions from bulk and surface conducting channels are isolated and the unusual thermoelectric properties are attributed to the topological surface states. The analysis showcases the rich thermoelectric transport physics in quantum‐confined topological Dirac semimetal thin films and suggests new routes to achieving high thermoelectric performance at cryogenic temperatures.
more » « less- Award ID(s):
- 2118523
- PAR ID:
- 10550543
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 36
- Issue:
- 28
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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