Electronic structures and photoemission spectroscopy

Abstract:

Thermoelectric materials (TMs) can uniquely convert waste heat into electricity, which provides a potential solution for the global energy crisis that is increasingly severe. Bulk Cu₂Se, with ionic conductivity of Cu ions, exhibits a significant enhancement of its thermoelectric figure of merit zT by a factor of ~3 near its structural transition around 400 K. Here, we show a systematic study of the electronic structure of Cu₂Se and its temperature evolution using high-resolution angle-resolved photoemission spectroscopy. Upon heating across the structural transition, the electronic states near the corner of the Brillouin zone gradually disappear, while the bands near the centre of Brillouin zone shift abruptly towards high binding energies and develop an energy gap. Interestingly, the observed band reconstruction well reproduces the temperature evolution of the Seebeck coefficient of Cu₂Se, providing an electronic origin for the drastic enhancement of the thermoelectric performance near 400 K. The current results not only bridge among structural phase transition, electronic structures and thermoelectric properties in a condensed matter system, but also provide valuable insights into the search and design of new generation of thermoelectric materials.

Abstract:

We exploit a high-performing resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi₂ O₂ Se nanoplates. Scanning tunneling microscopy combined with first-principle calculations confirms an amorphous Se atomic layer formed on the surface of 2D Bi₂ O₂ Se exposed to oxygen, which contributes to larger specific surface area and abundant active adsorption sites. Such 2D Bi₂ O₂ Se oxygen sensors have remarkable oxygen-adsorption induced variations of carrier density/mobility, and exhibit an ultrahigh sensitivity featuring minimum detection limit of 0.25 ppm, long-term stability, high durativity, and wide-range response to concentration up to 400 ppm at room temperature. 2D Bi₂ O₂ Se arrayed sensors integrated in parallel form are found to possess an oxygen detection minimum of sub-0.25 ppm ascribed to an enhanced signal-to-noise ratio. These advanced sensor characteristics involving ease integration show 2D Bi₂ O₂ Se is an ideal candidate for trace oxygen detection.

Abstract:

The discoveries of intrinsically magnetic topological materials, including semimetals with a large anomalous Hall effect and axion insulators^1-3, have directed fundamental research in solid-state materials. Topological quantum chemistry⁴ has enabled the understanding of and the search for paramagnetic topological materials^5,6. Using magnetic topological indices obtained from magnetic topological quantum chemistry (MTQC)⁷, here we perform a high-throughput search for magnetic topological materials based on first-principles calculations. We use as our starting point the Magnetic Materials Database on the Bilbao Crystallographic Server, which contains more than 549 magnetic compounds with magnetic structures deduced from neutron-scattering experiments, and identify 130 enforced semimetals (for which the band crossings are implied by symmetry eigenvalues), and topological insulators. For each compound, we perform complete electronic structure calculations, which include complete topological phase diagrams using different values of the Hubbard potential. Using a custom code to find the magnetic co-representations of all bands in all magnetic space groups, we generate data to be fed into the algorithm of MTQC to determine the topology of each magnetic material. Several of these materials display previously unknown topological phases, including symmetry-indicated magnetic semimetals, three-dimensional anomalous Hall insulators and higher-order magnetic semimetals. We analyse topological trends in the materials under varying interactions: 60 per cent of the 130 topological materials have topologies sensitive to interactions, and the others have stable topologies under varying interactions. We provide a materials database for future experimental studies and open-source code for diagnosing topologies of magnetic materials.