X-ray diffraction, Raman spectroscopy, and electrical conductivity measurements of molybdenum disulfide MoS(2) are performed at pressures up to 81 GPa in diamond anvil cells. Above 20 GPa, we find discontinuous changes in Raman spectra and x-ray diffraction patterns which provide evidence for isostructural phase transition from 2H(c) to 2H(a) modification through layer sliding previously predicted theoretically. This first-order transition, which is completed around 40 GPa, is characterized by a collapse in the c-lattice parameter and volume and also by changes in interlayer bonding. After the phase transition completion, MoS(2) becomes metallic. The reversibility of the phase transition is identified from all these techniques.
Tungsten ditelluride has attracted intense research interest due to the recent discovery of its large unsaturated magnetoresistance up to 60 T. Motivated by the presence of a small, sensitive Fermi surface of 5d electronic orbitals, we boost the electronic properties by applying a high pressure, and introduce superconductivity successfully. Superconductivity sharply appears at a pressure of 2.5 GPa, rapidly reaching a maximum critical temperature (Tc) of 7 K at around 16.8 GPa, followed by a monotonic decrease in Tc with increasing pressure, thereby exhibiting the typical dome-shaped superconducting phase. From theoretical calculations, we interpret the low-pressure region of the superconducting dome to an enrichment of the density of states at the Fermi level and attribute the high-pressure decrease in Tc to possible structural instability. Thus, tungsten ditelluride may provide a new platform for our understanding of superconductivity phenomena in transition metal dichalcogenides.
The design of efficient and stable photocatalysts for robust CO 2 reduction without sacrifice reagent or extra photosensitizer is still challenging. Herein, a single-atom catalyst of isolated single atom cobalt incorporated into Bi 3 O 4 Br atomic layers is successfully prepared. The cobalt single atoms in the Bi 3 O 4 Br favors the charge transition, carrier separation, CO 2 adsorption and activation. It can lower the CO 2 activation energy barrier through stabilizing the COOH* intermediates and tune the rate-limiting step from the formation of adsorbed intermediate COOH* to be CO* desorption. Taking advantage of cobalt single atoms and two-dimensional ultrathin Bi 3 O 4 Br atomic layers, the optimized catalyst can perform light-driven CO 2 reduction with a selective CO formation rate of 107.1 µmol g −1 h −1 , roughly 4 and 32 times higher than that of atomic layer Bi 3 O 4 Br and bulk Bi 3 O 4 Br, respectively.
Solar photocatalysis is a potential solution to satisfying energy demand and its resulting environmental impact. However, the low electron–hole separation efficiency in semiconductors has slowed the development of this technology. The effect of defects on electron–hole separation is not always clear. A model atomically thin structure of single‐unit‐cell Bi3O4Br nanosheets with surface defects is proposed to boost photocatalytic efficiency by simultaneously promoting bulk‐ and surface‐charge separation. Defect‐rich single‐unit‐cell Bi3O4Br displays 4.9 and 30.9 times enhanced photocatalytic hydrogen evolution and nitrogen fixation activity, respectively, than bulk Bi3O4Br. After the preparation of single‐unit‐cell structure, the bismuth defects are controlled to tune the oxygen defects. Benefiting from the unique single‐unit‐cell architecture and defects, the local atomic arrangement and electronic structure are tuned so as to greatly increase the charge separation efficiency and subsequently boost photocatalytic activity. This strategy provides an accessible pathway for next‐generation photocatalysts.
As a new type of topological materials, ZrTe 5 shows many exotic properties under extreme conditions. Using resistance and ac magnetic susceptibility measurements under high pressure, while the resistance anomaly near 128 K is completely suppressed at 6.2 GPa, a fully superconducting transition emerges. The superconducting transition temperature T c increases with applied pressure, and reaches a maximum of 4.0 K at 14.6 GPa, followed by a slight drop but remaining almost constant value up to 68.5 GPa. At pressures above 21.2 GPa, a second superconducting phase with the maximum T c of about 6.0 K appears and coexists with the original one to the maximum pressure studied in this work. In situ high-pressure synchrotron X-ray diffraction and Raman spectroscopy combined with theoretical calculations indicate the observed two-stage superconducting behavior is correlated to the structural phase transition from ambient Cmcm phase to high-pressure C2/m phase around 6 GPa, and to a mixture of two high-pressure phases of C2/m and P-1 above 20 GPa. The combination of structure, transport measurement, and theoretical calculations enable a complete understanding of the emerging exotic properties in 3D topological materials under extreme environments.high pressure | Dirac semimetals | superconductivity | synchrotron X-ray diffraction S ince the first report of topological insulator, an extensive attention in recent years has been focused on newly emergent Dirac materials including topological insulators (1-3), Dirac semimetals (4, 5), and Weyl semimetals (5-7) for their unique quantum phenomena. ZrTe 5 has been studied for a long time due to its large thermoelectric power (8, 9), resistivity anomaly (10, 11), and large positive magnetoresistance (12). Recent theoretical works (13,14) have proposed that single-layer ZrTe 5 is a large gap quantum spin hall insulator, but the bulk ZrTe 5 behaves between the strong and weak topological insulator. These predictions spark the renewed interest in the investigation of its Dirac and topological characters. Indeed, the magnetotransport experiments (15) have observed the chiral magnetic effect, both angle-resolved photoemission spectroscopy (15) and magneto-infrared spectroscopy (16, 17) study show the electronic structure of ZrTe 5 is similar with other three-dimensional (3D) Dirac semimetals like Na 3 Bi (18-20) and Cd 3 As 2 (21-25). These results suggest that ZrTe 5 is a very promising system that hosts topological properties and might help to pave a new way for further experimental studies of topological phase transitions.As one of the fundamental state parameters, high pressure is an effective, clean way to tune lattice as well as electronic states, especially in quantum states (26)(27)(28). In this work, by performing resistance and ac magnetic susceptibility measurements on ZrTe 5 single crystal at various pressures up to 68.5 GPa, a superconducting transition at 1.8 K was first noticed at a pressure of 6.2 GPa. It was interesting to notice that the occurrence of the metallic pha...
Atomically thin two-dimensional materials have emerged as a promising system for optoelectronic applications; however, the low quantum yield, mainly caused by nonradiative energy dissipation, has greatly limited practical applications. To reveal the details for nonradiative energy channels, femtosecond pump-probe spectroscopy with a detection wavelength ranging from visible to near-infrared to mid-infrared is performed on few-layer MoS. With this method, the many-body effects, occupation effects, and phonon dynamics are clearly identified. In particular, thermalization of the MoS lattice via electron-phonon scattering is responsible for a redshift of the exciton resonance energy observed within tens to hundreds of picoseconds after photoexcitation, which provides a direct real-time sensor for measuring the change in lattice temperature. We find that the excess energy from the cooling of hot carriers and the formation of bound carriers is efficiently transferred to the internal phonon system within 2 ps, while that from Shockley-Read-Hall recombination (∼9 ps) is mainly dissipated from the MoS surfaces to external phonons.
Two-dimensional (2D) material-controllable degradation under light radiation is crucial for their photonics and medical-related applications, which are yet to be investigated. In this paper, we first report the laser illumination method to regulate the degradation rate of Ti3C2Tx nanosheets in aqueous solution. Comprehensive characterization of intermediates and final products confirmed that plasmonic laser promoting the oxidation was strikingly different from heating the aqueous solution homogeneously. Laser illumination would nearly 10 times accelerate the degradation of Ti3C2Tx nanosheets in initial stage and create many smaller-sized oxidized products in a short time.Laser-induced fast degradation was principally ascribed to surface plasmonic resonance effect of Ti3C2Tx nanosheets.The degradation ability of such illumination could be controlled either by tuning the excitation wavelength or changing the excitation power. Furthermore, the laser-or thermal-induced degradation could be retarded by surface protection of Ti3C2Tx nanosheets. Our results suggest that plasmonic electron excitation of Ti3C2Tx nanosheets could build a new reaction channel and lead to the fast oxidation of nanosheets in aqueous solution, potentially enabling a series of waterbased applications.
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