Layered 1T-TaS2–xSex (0≤x≤2) single crystals have been systematically fabricated by a chemical vapor transport technique. Surprisingly, the superconductivity is induced by the Se doping. We demonstrate the appearance of a series of electronic states: the Mott phase melts into a nearly commensurate charge-density-wave (CDW) phase, superconductivity in a wide x range develops within the nearly commensurate CDW state, and finally commensurate CDW phase reproduces for heavy Se content. The rich phase diagram provides an ideal platform to investigate the interplay between electron correlation, CDW, and superconductivity, as well as the potential applications in electronic devices.
Current high-performance thermoelectric materials require elaborate doping and synthesis procedures, particularly in regard to the artificial structure, and the underlying thermoelectric mechanisms are still poorly understood. Here, we report that a natural chalcopyrite mineral, Cu1+x Fe1-x S2 , obtained from a deep-sea hydrothermal vent can directly generate thermoelectricity. The resistivity displayed an excellent semiconducting character, and a large thermoelectric power and high power factor were found in the low x region. Notably, electron-magnon scattering and a large effective mass was detected in this region, thus suggesting that the strong coupling of doped carriers and antiferromagnetic spins resulted in the natural enhancement of thermoelectric properties during mineralization reactions. The present findings demonstrate the feasibility of thermoelectric energy generation and electron/hole carrier modulation with natural materials that are abundant in the Earth's crust.
We have performed high-resolution angle-resolved photoemission spectroscopy of layered chalcogenide 1T-Fe(x)Ta(1-x)S(2) which undergoes a superconducting transition in the nearly commensurate charge-density-wave phase (melted Mott phase). We found a single electron pocket at the Brillouin-zone center in the melted Mott phase, which is created by the backfolding of bands due to the superlattice potential of charge-density-wave. This electron pocket appears in the x region where the samples show superconductivity, and is destroyed by the Mott- and Anderson-gap opening. Present results suggest that the melted Mott state and the superconductivity coexist in real space, providing a new insight into the interplay between electron correlation, charge order, and superconductivity.
Conventional PbTe-based semiconductors have been leading the development of thermoelectric community due to the rich capabilities for optimizing the electronic and phonon transport properties. However, the growing environmental concern related...
P-type lead telluride (PbTe) emerged as a promising thermoelectric material for intermediate-temperature waste-heat-energy harvesting. However, n-type PbTe still confronted with a considerable challenge owing to its relatively low figure of merit ZT and conversion efficiency η, limiting widespread thermoelectric applications. Here, we report that Ga-doping in n-type PbTe can optimize carrier concentration and thus improve the power factor. Moreover, further experimental and theoretical evidence reveals that Ga-doping-induced multiphase structures with nano- to micrometer size can simultaneously modulate phonon transport, leading to dramatic reduction of lattice thermal conductivity. As a consequence, a tremendous enhancement of ZT value at 823 K reaches ∼1.3 for n-type PbGaTe. In particular, in a wide temperature range from 323 to 823 K, the average ZT value of ∼0.9 and the calculated conversion efficiency η of ∼13% are achieved by Ga doping. The present findings demonstrate the great potential in Ga-doped PbTe thermoelectric materials through a synergetic carrier tuning and multiphase engineering strategy.
Interplay among various collective electronic states such as charge density wave and superconductivity is of tremendous significance in low-dimensional electron systems. However, the atomistic and physical nature of the electronic structures underlying the interplay of exotic states, which is critical to clarifying its effect on remarkable properties of the electron systems, remains elusive, limiting our understanding of the superconducting mechanism. Here, we show evidence that an ordering of selenium and sulphur atoms surrounding tantalum within star-of-David clusters can boost superconductivity in a layered chalcogenide 1T-TaS 2 À x Se x , which undergoes a superconducting transition in the nearly commensurate charge density wave phase. Advanced electron microscopy investigations reveal that such an ordered superstructure forms only in the x area, where the superconductivity manifests, and is destructible to the occurrence of the Mott metal-insulator transition. The present findings provide a novel dimension in understanding the relationship between lattice and electronic degrees of freedom.
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