Abstract 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. 
                        more » 
                        « less   
                    
                            
                            Enhanced Electron Correlation and Significantly Suppressed Thermal Conductivity in Dirac Nodal‐Line Metal Nanowires by Chemical Doping
                        
                    
    
            Abstract Enhancing electron correlation in a weakly interacting topological system has great potential to promote correlated topological states of matter with extraordinary quantum properties. Here, the enhancement of electron correlation in a prototypical topological metal, namely iridium dioxide (IrO2), via doping with 3d transition metal vanadium is demonstrated. Single‐crystalline vanadium‐doped IrO2nanowires are synthesized through chemical vapor deposition where the nanowire yield and morphology are improved by creating rough surfaces on substrates. Vanadium doping leads to a dramatic decrease in Raman intensity without notable peak broadening, signifying the enhancement of electron correlation. The enhanced electron correlation is further evidenced by transport studies where the electrical resistivity is greatly increased and follows an unusual dependence on the temperature (T). The lattice thermal conductivity is suppressed by an order of magnitude via doping even at room temperature where phonon‐impurity scattering becomes less important. Density functional theory calculations suggest that the remarkable reduction of thermal conductivity arises from the complex phonon dispersion and reduced energy gap between phonon branches, which greatly enhances phase space for phonon–phonon Umklapp scattering. This work demonstrates a unique system combining 3d and 5d transition metals in isostructural materials to enrich the system with various types of interactions. 
        more » 
        « less   
        
    
    
                            - PAR ID:
- 10382176
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Science
- Volume:
- 10
- Issue:
- 2
- ISSN:
- 2198-3844
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            Abstract Scalable substitutional doping of 2D transition metal dichalcogenides is a prerequisite to developing next‐generation logic and memory devices based on 2D materials. To date, doping efforts are still nascent. Here, scalable growth and vanadium (V) doping of 2D WSe2at front‐end‐of‐line and back‐end‐of‐line compatible temperatures of 800 and 400 °C, respectively, is reported. A combination of experimental and theoretical studies confirm that vanadium atoms substitutionally replace tungsten in WSe2, which results inp‐type doping via the introduction of discrete defect levels that lie close to the valence band maxima. Thep‐type nature of the V dopants is further verified by constructed field‐effect transistors, where hole conduction becomes dominant with increasing vanadium concentration. Hence, this study presents a method to precisely control the density of intentionally introduced impurities, which is indispensable in the production of electronic‐grade wafer‐scale extrinsic 2D semiconductors.more » « less
- 
            Abstract An emerging chalcogenide perovskite, CaZrSe3, holds promise for energy conversion applications given its notable optical and electrical properties. However, knowledge of its thermal properties is extremely important, e.g. for potential thermoelectric applications, and has not been previously reported in detail. In this work, we examine and explain the lattice thermal transport mechanisms in CaZrSe3using density functional theory and Boltzmann transport calculations. We find the mean relaxation time to be extremely short corroborating an enhanced phonon–phonon scattering that annihilates phonon modes, and lowers thermal conductivity. In addition, strong anharmonicity in the perovskite crystal represented by the Grüneisen parameter predictions, and low phonon number density for the acoustic modes, results in the lattice thermal conductivity to be limited to 1.17 W m−1 K−1. The average phonon mean free path in the bulk CaZrSe3sample (N → ∞) is 138.1 nm and nanostructuring CaZrSe3sample to ~10 nm diminishes the thermal conductivity to 0.23 W m−1 K−1. We also find that p-type doping yields higher predictions of thermoelectric figure of merit than n-type doping, and values ofZT~0.95–1 are found for hole concentrations in the range 1016–1017 cm−3and temperature between 600 and 700 K.more » « less
- 
            Abstract Polarons and spin-orbit (SO) coupling are distinct quantum effects that play a critical role in charge transport and spin-orbitronics. Polarons originate from strong electron-phonon interaction and are ubiquitous in polarizable materials featuring electron localization, in particular 3d transition metal oxides (TMOs). On the other hand, the relativistic coupling between the spin and orbital angular momentum is notable in lattices with heavy atoms and develops in 5d TMOs, where electrons are spatially delocalized. Here we combine ab initio calculations and magnetic measurements to show that these two seemingly mutually exclusive interactions are entangled in the electron-doped SO-coupled Mott insulator Ba2Na1−xCaxOsO6(0 < x < 1), unveiling the formation ofspin-orbital bipolarons. Polaron charge trapping, favoured by the Jahn-Teller lattice activity, converts the Os 5d1spin-orbital Jeff = 3/2 levels, characteristic of the parent compound Ba2NaOsO6(BNOO), into a bipolaron 5d2Jeff = 2 manifold, leading to the coexistence of different J-effective states in a single-phase material. The gradual increase of bipolarons with increasing doping creates robust in-gap states that prevents the transition to a metal phase even at ultrahigh doping, thus preserving the Mott gap across the entire doping range from d1BNOO to d2Ba2CaOsO6(BCOO).more » « less
- 
            Abstract The lattice thermal conductivity (κph) of metals and semimetals is limited by phonon‐phonon scattering at high temperatures and by electron‐phonon scattering at low temperatures or in some systems with weak phonon‐phonon scattering. Following the demonstration of a phonon band engineering approach to achieve an unusually high κphin semiconducting cubic‐boron arsenide (c‐BAs), recent theories have predicted ultrahigh κphof the semimetal tantalum nitride in the θ‐phase (θ‐TaN) with hexagonal tungsten carbide (WC) structure due to the combination of a small electron density of states near the Fermi level and a large phonon band gap, which suppress electron‐phonon and three‐phonon scattering, respectively. Here, measurements on the thermal and electrical transport properties of polycrystalline θ‐TaN converted from the ε phase via high‐pressure synthesis are reported. The measured thermal conductivity of the θ‐TaN samples shows weak temperature dependence above 200 K and reaches up to 90 Wm−1K−1, one order of magnitude higher than values reported for polycrystalline ε‐TaN and δ‐TaN thin films. These results agree with theoretical calculations that account for phonon scattering by 100 nm‐level grains and suggest κphincrease above the 249 Wm−1K−1value predicted for single‐crystal WC when the grain size of θ‐TaN is increased above 400 nm.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
