Superconductivity in Layered van der Waals Hydrogenated Germanene at High Pressure.

The emergence of superconductivity in two-dimensional (2D) materials has attracted tremendous research efforts because the origins and mechanisms behind the unexpected and fascinating superconducting phenomena remain unclear. In particular, the superconductivity can survive in 2D systems even with weakened disorder and broken spatial inversion symmetry. Here, structural and superconducting transitions of 2D van der Waals (vdW) hydrogenated germanene (GeH) are observed under compression and decompression processes. GeH possesses a superconducting transition with a critical temperature (Tc) of 5.41 K at 8.39 GPa. A crystalline to amorphous transition occurs at 16.80 GPa, while superconductivity remains. An abnormal increase of Tc up to 6.11 K was observed during the decompression process, while the GeH remained in the 2D amorphous phase. A combination study of in situ high-pressure synchrotron X-ray diffraction, in situ high-pressure Raman spectroscopy, transition electron microscopy, and density functional theory simulations suggests that the superconductivity in 2D vdW GeH is attributed to the increased density of states at the Fermi level as well as the enhanced electron-phonon coupling effect under high pressure even in the form of an amorphous phase. The unique pressure-induced phase transition of GeH from 2D crystalline to 2D amorphous metal hydride provides a promising platform to study the mechanisms of amorphous hydride superconductivity.

Kondo Holes in the Two-Dimensional Itinerant Ising Ferromagnet Fe3GeTe2.

Heavy Fermion (HF) states emerge in correlated quantum materials due to the intriguing interplay between localized magnetic moments and itinerant electrons but rarely appear in 3d-electron systems due to high itinerancy of d-electrons. Here, an anomalous enhancement of Kondo screening is observed at the Kondo hole of local Fe vacancies in Fe3GeTe2 which is a recently discovered 3d-HF system featuring Kondo lattice and two-dimensional itinerant ferromagnetism. An itinerant Kondo-Ising model is established to reproduce the experimental results and provides insight into the competition between Ising ferromagnetism and Kondo screening. Our work explains the microscopic origin of the d-electron HF states in Fe3GeTe2 and inspires future studies of the enriched quantum many-body effects with Kondo holes.

Moiré-Potential-Induced Band Structure Engineering in Graphene and Silicene.

A moiré pattern results from the projection of one periodic pattern to another with relative lattice constant or misalignment and provides great periodic potential to modify the electronic properties of pristine materials. In this Review, recent research on the effect of the moiré superlattice on the electronic structures of graphene and silicene, both of which possess a honeycomb lattice, is focused on. The moiré periodic potential is introduced by the interlayer interaction to realize abundant phenomena, including new generation of Dirac cones, emergence of Van Hove singularities (vHs) at the cross point of two sets of Dirac cones, Mott-like insulating behavior at half-filling state, unconventional superconductivity, and electronic Kagome lattice and flat band with nontrivial edge state. The role of interlayer coupling strength, which is determined by twist angle and buckling degree, in these exotic properties is discussed in terms of both the theoretical prediction and experimental measurement, and finally, the challenges and outlook for this field are discussed.

Experimental Realization of Two-Dimensional Buckled Lieb Lattice.

Two-dimensional (2D) materials with a Lieb lattice host exotic electronic band structures. Such a system does not exist in nature, and it is also difficult to obtain in the laboratory due to its structural instability. Here, we experimentally realized a 2D system composed of a tin overlayer on an aluminum substrate by molecular beam epitaxy. The specific arrangement of Sn atoms on the Al(100) surface, which benefits from favorable interface interactions, forms a stabilized buckled Lieb lattice. Theoretical calculations indicate a partially broken nodal line loop and a topologically nontrivial insulating state with a spin-orbital coupling effect in the band structure of this Lieb lattice. The electronic structure of this system is experimentally characterized by angle-resolved photoemission spectroscopy, in which the hybridized states between topmost Al atoms and Sn atoms are revealed. Our work provides an appealing method for constructing 2D quantum materials based on the Lieb lattice.

Reversible Oxidation of Blue Phosphorus Monolayer on Au(111).

Practical applications of two-dimensional (2D) black phosphorus (BP) are limited by its fast degradation under ambient conditions, for which many different mechanisms have been proposed; however, an atomic level understanding of the degradation process is still hindered by the absence of bottom-up methods for the growth of large-scale few-layer black phosphorus. Recent experimental success in the fabrication of single-layer blue phosphorus provides a model system to probe the oxidation mechanism of two-dimensional (2D) phosphorene down to single-layer thicknesses. Here, we report an atomic-scale investigation of the interaction between molecular oxygen and blue phosphorus. The atomic structure of blue phosphorus and the local binding sites of oxygen have been precisely identified using qPlus-based noncontact atomic force microscopy. A combination of low-temperature scanning tunneling microscopy and X-ray photoelectron spectroscopy measurements reveal a thermally reversible oxidation process of blue phosphorus in a pure oxygen atmosphere. Our study clearly demonstrates the essential role of oxygen in the initial oxidation process, and it sheds further light on the fundamental pathways of the degradation mechanism.

A Gallium-Based Magnetocaloric Liquid Metal Ferrofluid.

We demonstrate a magnetocaloric ferrofluid based on a gadolinium saturated liquid metal matrix, using a gallium-based liquid metal alloy as the solvent and suspension medium. The material is liquid at room temperature, while exhibiting spontaneous magnetization and a large magnetocaloric effect. The magnetic properties were attributed to the formation of gadolinium nanoparticles suspended within the liquid gallium alloy, which acts as a reaction solvent during the nanoparticle synthesis. High nanoparticle weight fractions exceeding 2% could be suspended within the liquid metal matrix. The liquid metal ferrofluid shows promise for magnetocaloric cooling due to its high thermal conductivity and its liquid nature. Magnetic and thermoanalytic characterizations reveal that the developed material remains liquid within the temperature window required for domestic refrigeration purposes, which enables future fluidic magnetocaloric devices. Additionally, the observed formation of nanometer-sized metallic particles within the supersaturated liquid metal solution has general implications for chemical synthesis and provides a new synthetic pathway toward metallic nanoparticles based on highly reactive rare earth metals.

Br-Vacancies Induced Variable Ranging Hopping Conduction in High-Order Topological Insulator Bi4Br4.

The defects have a remarkable influence on the electronic structures and the electric transport behaviors of the matter, providing the additional means to engineering their physical properties. In this work, a comprehensive study on the effect of Br-vacancies on the electronic structures and transport behaviors in the high-order topological insulator Bi4Br4 is performed by the combined techniques of the scanning tunneling microscopy (STM), angle-resolved photoemission spectroscopy (ARPES), and physical properties measurement system along with the first-principle calculations. The STM results show the defects on the cleaved surface of a single crystal and reveal that the defects are correlated to the Br-vacancies with the support of the simulated STM images. The role of the Br-vacancies in the modulation of the band structures has been identified by ARPES spectra and the calculated energy-momentum dispersion. The relationship between the Br-vacancies and the semiconducting-like transport behaviors at low temperature has been established, implying a Mott variable ranging hopping conduction in Bi4Br4. The work not only resolves the unclear transport behaviors in this matter, but also paves a way to modulate the electric conduction path by the defects engineering.

Epitaxial Growth of Monolayer SnP3 with High Mobility and Chiral Boundary Junctions.

Two-dimensional materials with layered structures, appropriate band gaps, and high carrier mobility have attracted tremendous interest for their potential applications. Here we report the growth of monolayer SnP3 on Au(111) surfaces by molecular beam epitaxy. The kinetic processes for the growth and the crystalline properties are studied by scanning tunneling microscopy. The weak interaction between SnP3 and its Au(111) substrate is signified by the random crystal orientation distributions of SnP3 nanosheets. The electronic structures exhibit a band gap of ∼0.25 eV and high charge carrier mobility comparable to that of black phosphorus engineered by compressive strain. Additionally, domain boundary junctions with opposite chirality are observed, resulting from the strained film in the epitaxial growth process. Our work provides a method to fabricate high-quality monolayer SnP3 and suggests that the monolayer SnP3 is a promising candidate for applications in nanoelectronics and optoelectronics.

Observation of Anomalous Planar Hall Effect Induced by One-Dimensional Weak Antilocalization.

The confinement of electrons in one-dimensional (1D) space highlights the prominence of the role of electron interactions or correlations, leading to a variety of fascinating physical phenomena. The quasi-1D electron states can exhibit a unique spin texture under spin-orbit interaction (SOI) and thus could generate a robust spin current by forbidden electron backscattering. Direct detection of such 1D spin or SOI information, however, is challenging due to complicated techniques. Here, we identify an anomalous planar Hall effect (APHE) in the magnetotransport of quasi-1D van der Waals (vdW) topological materials as exemplified by Bi4Br4, which arises from the quantum interference correction of 1D weak antilocalization (WAL) to the ordinary planar Hall effect and demonstrates a deviation from the usual sine and cosine curves. The occurrence of 1D WAL is correlated to the line-shape Fermi surface and persistent spin texture of (100) topological surface states of Bi4Br4, as revealed by both our angle-resolved photoemission spectroscopy and first-principles calculations. By generalizing the observation of APHE to other non-vdW bulk materials, this work provides a possible characteristic of magnetotransport for identifying the spin/SOI information and quantum interference behavior of 1D states in 3D topological material.

Towards layer-selective quantum spin hall channels in weak topological insulator Bi4Br2I2.

Weak topological insulators, constructed by stacking quantum spin Hall insulators with weak interlayer coupling, offer promising quantum electronic applications through topologically non-trivial edge channels. However, the currently available weak topological insulators are stacks of the same quantum spin Hall layer with translational symmetry in the out-of-plane direction-leading to the absence of the channel degree of freedom for edge states. Here, we study a candidate weak topological insulator, Bi4Br2I2, which is alternately stacked by three different quantum spin Hall insulators, each with tunable topologically non-trivial edge states. Our angle-resolved photoemission spectroscopy and first-principles calculations show that an energy gap opens at the crossing points of different Dirac cones correlated with different layers due to the interlayer interaction. This is essential to achieve the tunability of topological edge states as controlled by varying the chemical potential. Our work offers a perspective for the construction of tunable quantized conductance devices for future spintronic applications.

Electronic Flat Band in Distorted Colouring Triangle Lattice.

Dispersionless flat bands (FBs) in momentum space, given rise to electron destructive interference in frustrated lattices, offer opportunities to enhance electronic correlations and host exotic many-body phenomena, such as Wigner crystal, fractional quantum hall state, and superconductivity. Despite successes in theory, great challenges remain in experimentally realizing FBs in frustrated lattices due to thermodynamically structural instability. Here, the observation of electronic FB in a potassium distorted colouring triangle (DCT) lattice is reported, which is supported on a blue phosphorene-gold network. It is verified that the interaction between potassium and the underlayer dominates and stabilizes the frustrated structures. Two-dimensional electron gas is modulated by the DCT lattice, and in turn results in a FB dispersion due to destructive quantum interferences. The FB exhibits suppressed bandwidth with high density of states, which is directly observed by scanning tunneling microscopy and confirmed by the first-principles calculation. This work demonstrates that DCT lattice is a promising platform to study FB physics and explore exotic phenomena of correlation and topological matters.

Topological Flat Bands in 2D Breathing-Kagome Lattice Nb3 TeCl7.

Flat bands (FBs) can appear in two-dimensional (2D) geometrically frustrated systems caused by quantum destructive interference (QDI). However, the scarcity of pure 2D frustrated crystal structures in natural materials makes FBs hard to be identified, let alone modulate FBs relating to electronic properties. Here, the experimental evidence of the complete electronic QDI induced FB contributed by the 2D breathing-kagome layers of Nb atoms in Nb3 TeCl7 (NTC) is reported. An identical chemical state and 2D localization characteristics of the Nb breathing-kagome layers are experimentally confirmed, based on which NTC is demonstrated to be a superior concrete candidate for the breathing-kagome tight-binding model. Furthermore, it theoretically establishes the tunable roles of the on-site energy over Nb sites on bandwidth, energy position, and topology of FBs in NTC. This work opens an aveanue to manipulate FB characteristics in these 4d transition-metal-based breathing-kagome materials.

Topological electronic structure and spin texture of quasi-one-dimensional higher-order topological insulator Bi4Br4.

The notion of topological insulators (TIs), characterized by an insulating bulk and conducting topological surface states, can be extended to higher-order topological insulators (HOTIs) hosting gapless modes localized at the boundaries of two or more dimensions lower than the insulating bulk. In this work, by performing high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements with submicron spatial and spin resolution, we systematically investigate the electronic structure and spin texture of quasi-one-dimensional (1D) HOTI candidate Bi4Br4. In contrast to the bulk-state-dominant spectra on the (001) surface, we observe gapped surface states on the (100) surface, whose dispersion and spin-polarization agree well with our ab-initio calculations. Moreover, we reveal in-gap states connecting the surface valence and conduction bands, which is a signature of the hinge states inside the (100) surface gap. Our findings provide compelling evidence for the HOTI phase of Bi4Br4. The identification of the higher-order topological phase promises applications based on 1D spin-momentum locked current in electronic and spintronic devices.

Large-Gap Quantum Spin Hall State and Temperature-Induced Lifshitz Transition in Bi4Br4.

Searching for quantum spin Hall insulators with large fully opened energy gap to overcome the thermal disturbance at room temperature has attracted tremendous attention because of the robustness of one-dimensional (1D) spin-momentum locked topological edge states in the practical applications of electronic devices and spintronics. Here, we report the investigation of topological nature of monolayer Bi4Br4 by the techniques of angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy. The possible topological nontriviality of 1D edge state integrals within the large energy gap (∼0.2 eV) is revealed by the first-principle calculations. The ARPES measurements at different temperatures show a temperature-induced Lifshitz transition, corresponding to the resistivity anomaly evoked by the chemical potential shift. The connection between the emergency of superconductivity and the Lifshitz transition is discussed.

Epitaxial Growth of Quasi-One-Dimensional Bismuth-Halide Chains with Atomically Sharp Topological Non-Trivial Edge States.

Quantum spin Hall insulators (QSHIs) have one-dimensional (1D) spin-momentum locked topological edge states (ES) inside the bulk band gap, which can serve as dissipationless channels for the practical applications in low consumption electronics and high performance spintronics. However, obtaining the clean and atomically sharp ES which serves as ideal 1D spin-polarized nondissipative conducting channels is demanding and still a challenge. Here, we report the formation of the quasi-1D Bi4I4 nanoribbons on the surface of Bi(111) with the support of the graphene-terminated 6H-SiC(0001) and the direct observation of the topological ES at the step edges by the scanning tunneling microscopy (STM) and spectroscopic-imaging results. The ES reside surround the edge of Bi4I4 nanoribbons and exhibits noteworthy robustness against nontime reversal symmetry (non-TRS) perturbations. The theoretical simulations verify the topological nontriviality of 1D ES, which is retained after considering the presence of the underlying Bi(111). Our study supports the existence of topological ES in Bi4I4 nanoribbons, benefiting to engineer the topological features by using the 1D nanoribbons as building blocks.

Germanium Nanosheets with Dirac Characteristics as a Saturable Absorber for Ultrafast Pulse Generation.

Bulk germanium as a group-IV photonic material has been widely studied due to its relatively large refractive index and broadband and low propagation loss from near-infrared to mid-infrared. Inspired by the research of graphene, the 2D counterpart of bulk germanium, germanene, has been discovered and the characteristics of Dirac electrons have been observed. However, the optical properties of germanene still remain elusive. In this work, several layers of germanene are prepared with Dirac electronic characteristics and its morphology, band structure, carrier dynamics, and nonlinear optical properties are systematically investigated. It is surprisingly found that germanene has a fast carrier-relaxation time comparable to that of graphene and a relatively large nonlinear absorption coefficient, which is an order of magnitude higher than that of graphene in the near-infrared wavelength range. Based on these findings, germanene is applied as a new saturable absorber to construct an ultrafast mode-locked laser, and sub-picosecond pulse generation in the telecommunication band is realized. The results suggest that germanene can be used as a new type of group-IV material for various nonlinear optics and photonic applications.

Reversible Potassium Intercalation in Blue Phosphorene-Au Network Driven by an Electric Field.

Foreign atom intercalation into an interface alters the strength of interlayer interaction and leads to the novel types of desirable properties. Here, we report an investigation via scanning tunnelling microscopy (STM) and scanning tunnelling spectroscopy (STS) of reversible potassium (K) intercalation in the blue phosphorene (blueP)-Au network that can be locally induced by an external electric field. The unique structure of the blueP-Au network provides large space in its pores for the intercalation and deintercalation process. The X-ray photoemission spectroscopy results reveal that the intercalated K atoms are bonded with Au atoms in substrate, which weakens the interaction between the blueP-Au network and Au(111). The STS and angle-resolved photoemission spectroscopy results indicate that the electronic properties of the blueP-Au network have been modulated after the K intercalation. Such reversible intercalation and deintercalation transitions in the blueP-Au network are relevant for the design of the nanoelectronic devices as well as for its application in K-ion batteries.

Two-Dimensional Van der Waals Heterostructures for Synergistically Improved Surface-Enhanced Raman Spectroscopy.

Surface-enhanced Raman spectroscopy (SERS) is a precise and noninvasive analytical technique that is widely used in chemical analysis, environmental protection, food processing, pharmaceutics, and diagnostic biology. However, it is still a challenge to produce highly sensitive and reusable SERS substrates with a minimum fluorescence background. In this work, we propose the use of van der Waals heterostructures of two-dimensional materials to cover plasmonic metal nanoparticles to solve this challenge. The heterostructures of atomically thin boron nitride (BN) and graphene provide synergistic effects: (1) electrons could tunnel through the atomically thin BN, allowing the charge transfer between graphene and probe molecules to suppress the fluorescence background; (2) the SERS sensitivity is enhanced by graphene via a chemical enhancement mechanism in addition to an electromagnetic field mechanism; and (3) the atomically thin BN protects the underlying graphene and Ag nanoparticles from oxidation during heating for regeneration at 360 °C in the air so that the SERS substrates could be reused. These advances will facilitate wider applications of SERS especially on the detection of fluorescent molecules with higher sensitivity.

Native Surface Oxides Featured Liquid Metals for Printable Self-Powered Photoelectrochemical Device.

Constructing high-performance photo-electrodes by patterning the photo-active semiconducting components with desirable texture and architecture is one of the most promising approaches to achieve the practical and scale-up application of photo-electric or photoelectrochemical (PEC) devices. However, it is a still big challenge to efficiently and effectively handle nano-structural semiconducting materials into intergraded circuit devices, displaying good electric-contact and stability. Here, a facile manufacture strategy for fabricating native metal-oxides based photo-electrodes by directly printing Ga-based liquid metals is explored. The PEC device, functionalized by the native Ga-oxide functional layer, exhibits self-powered photo-detection behaviors and presents fast photo-electric responsibility in response to the simulated Sunlight illumination. This printable PEC device shows good potential for high sensitive self-powered photo-detector and provides a flexible and versatile approach for the design and fabrication of novel electrode structures.

Realization of Strained Stanene by Interface Engineering.

Stanene, the tin analogue of graphene, has been predicted to be a two-dimensional topological insulator, providing an ideal platform for the realization of the quantum spin Hall effect even at room temperature. Here, continuous stanene has been successfully formed on the Au(111) substrate, and its crystalline structure, phonon properties, and electronic structures are investigated by scanning tunneling microscopy and in situ Raman spectroscopy combined with first-principles calculations. The surface Sn-Au alloy with a coverage-dependent structural evolution is first identified. At coverage above a critical value, the Au-Sn alloy is gradually converted into epitaxial stanene with a √3 × âˆš7 superstructure. Distinctive vibrational phonon modes are discovered in √3 × âˆš7 stanene through in situ Raman spectroscopy, which are correlated with the tensile strain evoked by its singular buckled structure. Our results present clear evidence for the existence of epitaxial stanene and provide a platform for exploration of the exotic properties of this strained two-dimensional material.