Topology is being widely adopted to understand and to categorize quantum matter in modern physics. The nexus of topology orders, which engenders distinct quantum phases with benefits to both fundamental research and practical applications for future quantum devices, can be driven by topological phase transition through modulating intrinsic or extrinsic ordering parameters. The conjoined topology, however, is still elusive in experiments due to the lack of suitable material platforms. Here we use scanning tunneling microscopy, angle-resolved photoemission spectroscopy, and theoretical calculations to investigate the doping-driven band structure evolution of a quasi-one-dimensional material system, bismuth halide, which contains rare multiple band inversions in two time-reversal-invariant momenta. According to the unique bulk-boundary correspondence in topological matter, we unveil a composite topological phase, the coexistence of a strong topological phase and a high-order topological phase, evoked by the band inversion associated with topological phase transition in this system. Moreover, we reveal multiple-stage topological phase transitions by varying the halide element ratio: from high-order topology to weak topology, the unusual dual topology, and trivial/weak topology subsequently. Our results not only realize an ideal material platform with composite topology, but also provide an insightful pathway to establish abundant topological phases in the framework of band inversion theory.
The design of low-cost yet high-efficiency electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) over a wide pH range is highly challenging. We now report a hierarchical co-assembly of interacting MoS2 and Co9S8 nanosheets attached on Ni3S2 nanorod arrays which are supported on nickel foam (NF). This tiered structure endows high performance toward HER and OER over a very broad pH range. By adjusting the molar ratio of the Co:Mo precursors, we have created CoMoNiS-NF- xy composites ( x: y means Co:Mo molar ratios ranging from 5:1 to 1:3) with controllable morphology and composition. The three-dimensional composites have an abundance of active sites capable of universal pH catalytic HER and OER activity. The CoMoNiS-NF-31 demonstrates the best electrocatalytic activity, giving ultralow overpotentials (113, 103, and 117 mV for HER and 166, 228, and 405 mV for OER) to achieve a current density of 10 mA cm-2 in alkaline, acidic, and neutral electrolytes, respectively. It also shows a remarkable balance between electrocatalytic activity and stability. Based on the distinguished catalytic performance of CoMoNiS-NF-31 toward HER and OER, we demonstrate a two-electrode electrolyzer performing water electrolysis over a wide pH range, with low cell voltages of 1.54, 1.45, and 1.80 V at 10 mA cm-2 in alkaline, acidic, and neutral media, respectively. First-principles calculations suggest that the high OER activity arises from electron transfer from Co9S8 to MoS2 at the interface, which alters the binding energies of adsorbed species and decreases overpotentials. Our results demonstrate that hierarchical metal sulfides can serve as highly efficient all-pH (pH = 0-14) electrocatalysts for overall water splitting.
The negative thermal expansion (NTE) materials, which can act as thermal-expansion compensators to counteract the positive thermal expansion, have great applications merit in precision engineering. However, the exploration of NTE behavior with a wide temperature range has reached its upper ceiling through traditional doping strategies due to composition limitations. The unique sluggish characteristic in phase transition and extended optimization space in recent high entropy systems has great potential to broaden the temperature range in electronic transitions-induced NTE materials. Mn-based anti-perovskites offer an ideal platform for the exploration of high entropy NTE material due to their abundant element selection and controllable NTE performance. In this paper, the high entropy strategy is first introduced to broaden the NTE temperature range by relaxing the abrupt phase transition in Mn-based anti-perovskite nitride. We propose an empirical screening method to synthesize the high-entropy anti-perovskite (HEAP). it is found that magnetic phase separation from anti-ferromagnetic CII to paramagnetic CI surviving in an ultra-wide temperature range of 5K<=T<=350K (Delta_T=345K), revealing a unique sluggish characteristic. Consequently, a remarkable NTE behavior (up to Delta_T=235K, 5K<=T<=240K) with a coefficient of thermal expansion of -4.7x10-6/K, has been obtained in HEAP. It is worth noting that the temperature range is two/three times wider than that of low-entropy systems. The sluggish characteristic has been further experimentally proved to come from disturbed phase transition dynamics due to distortion in atomic spacing and chemical environmental fluctuation observed by the spherical aberration-corrected electron microscope. Our demonstration provides a unique paradigm for broadening the temperature range of NTE materials induced by phase transition through entropy engineering.
Heterostructures of two-dimensional (2D) layered materials with selective compositions play an important role in creating novel functionalities. Effective interface coupling between 2D ferromagnet and electronic materials would enable the generation of exotic physical phenomena caused by intrinsic symmetry breaking and proximity effect at interfaces. Here, epitaxial growth of bilayer Bi(110) on 2D ferromagnetic Fe3GeTe2 (FGT) with large magnetic anisotropy has been reported. Bilayer Bi(110) islands are found to extend along fixed lattice directions of FGT. The six preferred orientations could be divided into two groups of three-fold symmetry axes with the difference approximately to 26{\deg}. Moreover, dI/dV measurements confirm the existence of interface coupling between bilayer Bi(110) and FGT. A variation of the energy gap at the edges of bilayer Bi(110) is also observed which is modulated by the interface coupling strengths associated with its buckled atomic structure. This system provides a good platform for further study of the exotic electronic properties of epitaxial Bi(110) on 2D ferromagnetic substrate and promotes potential applications in the field of spin devices.
As a rising star in the family of graphene analogues, germanene shows great potential for electronic and optical device applications due to its unique structure and electronic properties. It is revealed that the hydrogen terminated germanene not only maintains a high carrier mobility similar to that of germanene, but also exhibits strong light-matter interaction with a direct band gap, exhibiting great potential for photoelectronics. In this work, few-layer germanane (GeH) nanosheets with controllable thickness are successfully synthesized by a solution-based exfoliation-centrifugation route. Instead of complicated microfabrication techniques, a robust photoelectrochemical (PEC)-type photodetector, which can be extended to flexible device, is developed by simply using the GeH nanosheet film as an active electrode. The device exhibits an outstanding photocurrent density of 2.9 µA cm-2 with zero bias potential, excellent responsivity at around 22 µA W-1 under illumination with intensity ranging from 60 to 140 mW cm-2 , as well as short response time (with rise and decay times, tr = 0.24 s and td = 0.74 s). This efficient strategy for a constructing GeH-based PEC-type photodetector suggests a path to promising high-performance, self-powered, flexible photodetectors, and it also paves the way to a practical application of germanene.
Hydrogenation is an effective approach to improve the performance of photocatalysts within defect engineering methods. The mechanism of hydrogenation and synergetic effects between hydrogen atoms and local electronic structures, however, remain unclear due to the limits of available photocatalytic systems and technical barriers to observation and measurement. Here, we utilize oxygen vacancies as residential sites to host hydrogen atoms in a layered bismuth oxychloride material containing defects. It is confirmed theoretically and experimentally that the hydrogen atoms interact with the vacancies and surrounding atoms, which promotes the separati30on and transfer processes of photo-generated carriers via the resulting band structure. The efficiency of catalytic activity and selectivity of defective bismuth oxychloride regarding nitric oxide oxidation has been improved. This work clearly reveals the role of hydrogen atoms in defective crystalline materials and provides a promising way to design catalytic materials with controllable defect engineering.
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