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A theoretical ideal two-dimensional electron gas (2DEG) was characterized by a flat density of states independent of energy. Compared with conventional two-dimensional free-electron systems in semiconductor heterojunctions and noble metal surfaces, we report here the achievement of ideal 2DEG with multiple quantized states in few-layer InSe films. The multiple quantum well states (QWSs) in few-layer InSe films are found, and the number of QWSs is strictly equal to the number of atomic layers. The multiple stair-like DOS as well as multiple bands with parabolic dispersion both characterize ideal 2DEG features in these QWSs. Density functional theory calculations and numerical simulations based on quasi-bounded square potential wells described as the Kronig-Penney model provide a consistent explanation of 2DEG in the QWSs. Our work demonstrates that 2D van der Waals materials are ideal systems for realizing 2DEG hosted by multiple quantized Kronig-Penney states, and the semiconducting nature of the material provides a better chance for construction of high-performance electronic devices utilizing these states, for example, superlattice devices with negative differential resistance.

The adsorption and self-assembly structures of melamine molecules on an Ag(111) surface are studied by low temperature scanning tunneling microscopy (STM) combined with tip-enhanced Raman spectroscopy (TERS). Two ordered self-assembly phases of melamine molecules on Ag(111) were studied by STM and TERS, combining with first-principles simulations. The α-phase consists of flat-lying melamine molecules, while the β-phase consists of mixed up-standing/tilted melamine molecules. Moreover, dehydrogenation of melamine can be controlled by annealing the sample as well as by a tip-enhanced photo-catalytic effect. Our work demonstrates TERS as a powerful tool not only for investigating the configuration and vibration properties of molecules on a metal surface with high spatial resolution but also for manipulating the chemical reactions with tip and photo-induced effects.

Polaron is a composite quasiparticle derived from an excess carrier trapped by local lattice distortion, and it has been studied extensively for decades both theoretically and experimentally. However, atomic-scale creation and manipulation of single-polarons in real space have still not been achieved so far, which precludes the atomistic understanding of the properties of polarons as well as their applications. Herein, using scanning tunneling microscopy, we succeeded to create single polarons in a monolayer two-dimensional semiconductor, CoCl2. Combined with first-principles calculations, two stable polaron configurations, centered at on-top and hollow sites, respectively, have been revealed. Remarkably, a series of manipulation progresses, from creation, erasure to transition, can be accurately implemented on individual polarons. Our results pave the way to understand the polaronic physics at atomic level, and the easy control of single polarons in 2D semiconductor may open the door to 2D polaronics including the data storage.

The destructive interference of wavefunctions in a kagome lattice can give rise to topological flat bands (TFBs) with a highly degenerate state of electrons. Recently, TFBs have been observed in several kagome metals, including Fe

Shandite type Co3Sn2S2 has been reported as a magnetic Weyl semimetal recently and predicted to realize the quantum anomalous Hall effect in a two-dimensional limit. So far, electron transport stud...

Dirac materials, which feature Dirac cones in the reciprocal space, have been one of the hottest topics in condensed matter physics in the past decade. To date, 2D and 3D Dirac Fermions have been extensively studied, while their 1D counterparts are rare. Recently, Si nanoribbons (SiNRs), which are composed of alternating pentagonal Si rings, have attracted intensive attention. However, the electronic structure and topological properties of SiNRs are still elusive. Here, by angle-resolved photoemission spectroscopy, scanning tunneling microscopy/spectroscopy measurements, first-principles calculations, and tight-binding model analysis, we demonstrate the existence of 1D Dirac Fermions in SiNRs. Our theoretical analysis shows that the Dirac cones derive from the armchairlike Si chain in the center of the nanoribbon and can be described by the Su-Schrieffer-Heeger model. These results establish SiNRs as a platform for studying the novel physical properties in 1D Dirac materials., 4 figures

Two-dimensional (2D) materials and their heterostructures have been intensively studied in recent years due to their potential applications in electronic, optoelectronic, and spintronic devices. Nonetheless, the realization of 2D heterostructures with atomically flat and clean interfaces remains challenging, especially for air-sensitive materials, which hinders the in-depth investigation of interface-induced phenomena and the fabrication of high-quality devices. Here, we circumvented this challenge by exfoliating 2D materials in an ultrahigh vacuum. Remarkably, ultraflat and clean substrate surfaces can assist the exfoliation of 2D materials, regardless of the substrate and 2D material, thus providing a universal method for the preparation of heterostructures with ideal interfaces. In addition, we studied the properties of two prototypical systems that cannot be achieved previously, including the electronic structure of monolayer phospherene and optical responses of transition metal dichalcogenides on different metal substrates. Our work paves the way to engineer rich interface-induced phenomena, such as proximity effects and moir\'{e} superlattices., Comment: 17 pages, 4 figures

2D van der Waals heterojunction provides an attractive opportunity for realizing novel electronic or optoelectronic devices. It remains challenging to realize high-quality heterostructures through scalable methods such as molecular epitaxy growth (MBE). Here, growth of few-layer SnS thin films is reported on mica and Nb-doped SrTiO

As the nearest-neighbour element to carbon, boron is theoretically predicted to have a planar two-dimensional form, named borophene, with novel properties, such as Dirac fermions and superconductivity. Several polymorphs of monolayer borophene have been grown on metal surfaces, yet thicker bilayer and few-layer nanosheets remain elusive. Here we report the synthesis of large-size, single-crystalline bilayer borophene on the Cu(111) surface by molecular beam epitaxy. Combining scanning tunnelling microscopy and first-principles calculations, we show that bilayer borophene consists of two stacked monolayers that are held together by covalent interlayer boron-boron bonding, and each monolayer has β12-like structures with zigzag rows. The formation of a bilayer is associated with a large transfer and redistribution of charge in the first boron layer on Cu(111), which provides additional electrons for the bonding of additional boron atoms, enabling the growth of the second layer. The bilayer borophene is shown to possess metallic character, and be less prone to being oxidized than its monolayer counterparts.

The destructive interference of wavefunctions in a kagome lattice can give rise to topological flat bands (TFBs) with a highly degenerate state of electrons. Recently, TFBs have been observed in several kagome metals, including Fe$_3$Sn$_2$, FeSn, CoSn, and YMn$_6$Sn$_6$. Nonetheless, kagome materials that are both exfoliable and semiconducting are lacking, which seriously hinders their device applications. Herein, we show that Nb$_3$Cl$_8$, which hosts a breathing kagome lattice, is gapped out because of the absence of inversion symmetry, while the TFBs survive because of the protection of the mirror reflection symmetry. By angle-resolved photoemission spectroscopy measurements and first-principles calculations, we directly observe the TFB and a moderate band gap in Nb$_3$Cl$_8$. By mechanical exfoliation, we successfully obtain monolayers of Nb$_3$Cl$_8$ and confirm that they are stable under ambient conditions. In addition, our calculations show that monolayers of Nb$_3$Cl$_8$ have a magnetic ground state, thus providing opportunities to study the interplay between geometry, topology, and magnetism., Comment: 6 pages, 4 figures

The complexity of the chemical bonds in boron results in the polymorphism of borophene. To date, a variety of borophene polymorphs have been predicted. Because of its high chemical reactivity, boron reacts easily with other elements. Therefore, the most suitable method for the synthesis of borophene is molecular beam epitaxy, which is performed in an ultrahigh vacuum. In addition, some catalytic metal substrates can assist the growth process that leads to the experimental synthesis of borophene. In this chapter, we will review the synthesis processes of the different borophene polymorphs.

In the previous chapters, we have seen that borophene has been predicted to form numerous polymorphs, and some of these polymorphs have been experimentally synthesized by molecular beam epitaxy. Theoretically, borophenes are expected to host a rich variety of physical and chemical properties and a study of their electronic structures is thus highly desirable. In this chapter, we will review recent studies on the electronic structures of borophenes, with particular emphasis on experimental works. We will see that borophene hosts various exotic properties, including massless Dirac fermions, Dirac nodal line fermions, and superconductivity. These novel properties make borophene a promising material for use in future quantum devices.

Artificial lattices provide a tunable platform to realize exotic quantum devices. A well-known example is artificial graphene (AG), in which electrons are confined in honeycomb lattices and behave as massless Dirac fermions. Recently, AG systems have been constructed by manipulating molecules using scanning tunnelling microscope tips, but the nanoscale size typical for these constructed systems are impossible for practical device applications and insufficient for direct investigation of the electronic structures using angle-resolved photoemission spectroscopy (ARPES). Here, we demonstrate the synthesis of macroscopic AG by self-assembly of C$_{60}$ molecules on metal surfaces. Our theoretical calculations and ARPES measurements directly confirm the existence of Dirac cones at the $K$ ($K^\prime$) points of the Brillouin zone (BZ), in analogy to natural graphene. These results will stimulate ongoing efforts to explore the exotic properties in artificial lattices and provide an important step forward in the realization of novel molecular quantum devices., to appear in Physical Review B

Magnetic topological materials, in which the time-reversal symmetry is broken, host various exotic quantum phenomena, including the quantum anomalous Hall effect, axion insulator states, and Majorana fermions. The study of magnetic topological materials is at the forefront of condensed matter physics. Recently, a variety of magnetic topological materials have been reported, such as Mn$_3$Sn, Co$_3$Sn$_2$S$_2$, Fe$_3$Sn$_2$, and MnBi$_2$Te$_4$. Here, we report the observation of a topological electronic structure in an antiferromagnet, HoSbTe, a member of the ZrSiS family of materials, by angle-resolved photoemission spectroscopy measurements and first-principles calculations. We demonstrate that HoSbTe is a Dirac nodal line semimetal when spin-orbit coupling (SOC) is neglected. However, our theoretical calculations show that the strong SOC in HoSbTe fully gaps out the nodal lines and drives the system to a weak topological insulator state, with each layer being a two-dimensional topological insulator. Because of the strong SOC in HoSbTe, the gap is as large as hundreds of meV along specific directions, which is directly observed by our ARPES measurements. The existence of magnetic order and topological properties in HoSbTe makes it a promising material for realization of exotic quantum devices., 5 pages, 3 figures

The polymorphism of borophene makes it a promising system to realize tunable physical or chemical properties. Various pure borophene phases consisting of quasi-1D boron chains with different widths have been commonly obtained in experimental studies. Here, it is shown that, due to a substrate mediation effect, artificial long-range ordered phases of borophene consisting of different combinations of boron chains seamlessly joined together can be achieved on Ag(100). Scanning tunneling microscopy measurements and theoretical calculations reveal that mixed-chain phases are more stable than the pure phase, and interact only weakly with the substrate. The mixed-chain phases with various proportions of different chains can be well separated based on the crystal direction of the substrate. The successful growth of mixed-chain phases is expected to deepen the impact of substrate tailored synthesis of borophene.

Monolayer AlB$_2$ is composed of two atomic layers: honeycomb borophene and triangular aluminum. In contrast with the bulk phase, monolayer AlB$_2$ is predicted to be a superconductor with a high critical temperature. Here, we demonstrate that monolayer AlB$_2$ can be synthesized on Al(111) via molecular beam epitaxy. Our theoretical calculations revealed that the monolayer AlB$_2$ hosts several Dirac cones along the $\Gamma$--M and $\Gamma$--K directions; these Dirac cones are protected by crystal symmetries and are thus resistant to external perturbations. The extraordinary electronic structure of the monolayer AlB$_2$ was confirmed via angle-resolved photoemission spectroscopy measurements. These results are likely to stimulate further research interest to explore the exotic properties arising from the interplay of Dirac fermions and superconductivity in two-dimensional materials., Comment: 5 pages, 4 figures

The emergence of quantization at the nanoscale, the quantum size effect (QSE), allows flexible control of matter and is a rich source of advanced functionalities. A QSE-induced transition into an insulating phase in semimetallic nanofilms was predicted for bismuth a half-century ago and has regained new interest with regard to its surface states exhibiting nontrivial electronic topology. Here, we reveal an unexpected mechanism of the transition by high-resolution angle-resolved photoelectron spectroscopy combined with theoretical calculations. Anomalous evolution and degeneracy of quantized energy levels indicate that increased Coulomb repulsion from the surface states deforms a quantum confinement potential with decreasing thickness. The potential deformation drastically modulates spatial distributions of quantized wave functions, which leads to acceleration of the transition even beyond the original QSE picture. This discovery establishes a complete picture of the long-discussed problem in bismuth and highlights the new class of size effects dominating nanoscale transport in systems with metallic surface states., 22 pages, 10 figures (Supplementary Information included), accepted for publication in Science Advances

We report the synthesis of single-crystal NbC, a transition metal carbide with various unusual properties. Transport, magnetic susceptibility, and specific heat measurements demonstrate that NbC is a conventional superconductor with a superconducting transition temperature ($T_c$) of 11.5 K. Our theoretical calculations show that NbC is a type-II Dirac semimetal with strong Fermi surface nesting, which is supported by our ARPES measurement results. We also observed the superconducting gaps of NbC using angle-resolved photoemission spectroscopy (ARPES) and found some unconventional behaviors. These intriguing superconducting and topological properties, combined with the high corrosion resistance, make NbC an ideal platform for both fundamental research and device applications., Comment: to appear in Physical Review B

Two-dimensional topological insulators (2DTIs), which host the quantum spin Hall (QSH) effect, are one of the key materials in next-generation spintronic devices. To date, experimental evidence of the QSH effect has only been observed in a few materials, and thus, the search for new 2DTIs is at the forefront of physical and materials science. Here, we report experimental evidence of a 2DTI in the van der Waals material Ta$_2$Pd$_3$Te$_5$. First-principles calculations show that each monolayer of Ta$_2$Pd$_3$Te$_5$ is a 2DTI with weak interlayer interactions. Combined transport, angle-resolved photoemission spectroscopy, and scanning tunneling microscopy measurements confirm the existence of a band gap at the Fermi level and topological edge states inside the gap. These results demonstrate that Ta$_2$Pd$_3$Te$_5$ is a promising material for fabricating spintronic devices based on the QSH effect., Comment: 6 pages, 3 figures

Breaking bonds selectively in molecules is vital in many chemistry reactions and custom nanoscale device fabrications. The scanning tunneling microscope (STM) has proved to be an ideal tool to initiate and view bond-selective chemistry at the single-molecule level, offering opportunities for the further study of the dynamics in single molecules on metal surfaces. We demonstrate $\mathrm{H}─\mathrm{HS}$ and $\mathrm{H}─\mathrm{S}$ bond breaking on Au(111) induced by tunneling electrons using low-temperature STM. An experimental study combined with theoretical calculations shows that the dissociation pathway is facilitated by vibrational excitations. Furthermore, the dissociation probabilities of the two different dissociation processes are bias dependent due to different inelastic-tunneling probabilities, and they are also closely linked to the lifetime of inelastic-tunneling electrons. Combined with time-dependent ab initio nonadiabatic molecular dynamics simulations, the dynamics of the injected electron and the phonon-excitation-induced molecule dissociation can be understood at the atomic scale, demonstrating the potential application of STM for the investigation of excited-state dynamics of single molecules on surfaces.

Atomic scale engineering of two-dimensional materials could create devices with rich physical and chemical properties. External periodic potentials can enable the manipulation of the electronic band structures of materials. A prototypical system is 3x3-silicene/Ag(111), which has substrate-induced periodic modulations. Recent angle-resolved photoemission spectroscopy measurements revealed six Dirac cone pairs at the Brillouin zone boundary of Ag(111), but their origin remains unclear [Proc. Natl. Acad. Sci. USA 113, 14656 (2016)]. We used linear dichroism angle-resolved photoemission spectroscopy, the tight-binding model, and first-principles calculations to reveal that these Dirac cones mainly derive from the original cones at the K (K') points of free-standing silicene. The Dirac cones of free-standing silicene are split by external periodic potentials that originate from the substrate-overlayer interaction. Our results not only confirm the origin of the Dirac cones in the 3x3-silicene/Ag(111) system, but also provide a powerful route to manipulate the electronic structures of two-dimensional materials., Comment: 6 pages, 3 figures

Two-dimensional (2D) materials have attracted great attention and spurred rapid development in both fundamental research and device applications. The search for exotic physical properties, such as magnetic and topological order, in 2D materials could enable the realization of novel quantum devices and is therefore at the forefront of materials science. Here, we report the discovery of two-fold degenerate Weyl nodal lines in a 2D ferromagnetic material, a single-layer gadolinium-silver compound, based on combined angle-resolved photoemission spectroscopy measurements and theoretical calculations. These Weyl nodal lines are symmetry protected and thus robust against external perturbations. The coexistence of magnetic and topological order in a 2D material is likely to inform ongoing efforts to devise and realize novel nanospintronic devices., 4 figures

Spin-orbit coupling (SOC) has gained much attention for its rich physical phenomena and highly promising applications in spintronic devices. The Rashba-type SOC in systems with inversion symmetry breaking is particularly attractive for spintronics applications since it allows for flexible manipulation of spin current by external electric fields. Here, we report the discovery of a giant anisotropic Rashba-like spin splitting along three momentum directions (3D Rashba-like spin splitting) with a helical spin polarization around the M points in the Brillouin zone of trigonal layered PtBi2. Due to its inversion asymmetry and reduced symmetry at the M point, Rashba-type as well as Dresselhaus-type SOC cooperatively yield a 3D spin splitting with alpha~ 4.36 eVA in PtBi2. The experimental realization of 3D Rashba-like spin splitting not only has fundamental interests but also paves the way to the future exploration of a new class of material with unprecedented functionalities for spintronics applications., Comment: 19 pages, 5 figures

We have performed scanning tunneling microscopy/spectroscopy (STM/STS) study and first-principles calculations to investigate the atomic structure and electronic properties of silicon nanoribbons (SiNRs) grown on Ag(110). Despite the extensive research on SiNRs in the last decades, its atomic structure is still not fully understood so far. In this report we determine that the structure of SiNRs/Ag(110) is armchair silicene nanoribbon with reconstructed edges. Meanwhile, pronounced quantum well states (QWS) in SiNRs were observed and their energy spectrum was systematically measured. The QWS are due to the confinement of quasiparticles perpendicular to the nanoribbon and can be well explained by the theory of one-dimensional (1D) “particle-in-a-box” model in quantum mechanics.

Some two-dimensional liquid systems are theoretically predicted to have an anomalous phase transition due to unique intermolecular interactions, for example the first-order transition between two-dimensional high-density water and low-density amorphous ice. However, it has never been experimentally observed, to the best of our knowledge. Here we report an entropy-driven phase transition between a high-density liquid crystal and low-density crystalline solid, directly observed by scanning tunneling microscope in carbon monoxide adsorbed on Cu(111). Combined with first principle calculations, we find that repulsive dipole–dipole interactions between carbon monoxide molecules lead to unconventional thermodynamics. This finding of unconventional thermodynamics in two-dimensional carbon monoxide not only provides a platform to study the fundamental principles of anomalous phase transitions in two-dimensional liquids at the atomic scale, but may also help to design and develop more efficient copper-based catalysis., Intermolecular interactions have a crucial role in the adsorption of molecules on a surface, however their role in promoting phase transitions is less well known. Here, the authors report an abnormal phase transition between a high-density liquid crystal and low-density solid in the case of carbon monoxide on Cu(111), driven by intermolecular interactions and entropy.

In a Dirac nodal line semimetal, the bulk conduction and valence bands touch at extended lines in the Brillouin zone. To date, most of the theoretically predicted and experimentally discovered nodal lines derive from the bulk bands of two- and three-dimensional materials. Here, based on combined angle-resolved photoemission spectroscopy measurements and first-principles calculations, we report the discovery of node-line-like surface states on the (001) surface of LaBi. These bands derive from the topological surface states of LaBi and bridge the band gap opened by spin-orbit coupling and band inversion. Our first-principles calculations reveal that these "nodal lines" have a tiny gap, which is beyond typical experimental resolution. These results may provide important information to understand the extraordinary physical properties of LaBi, such as the extremely large magnetoresistance and resistivity plateau., 6 pages, 4 figures

Graphene, a two-dimensional monatomic layer of crystal carbon, has recently emerged as a potential material for next-generation optoelectronic devices owing to unique properties arising from its massless Dirac fermions. However, the intrinsic carrier dynamics of graphene has remained a mystery even for the simple case of carrier cooling after the photoexcitation. This is because the observed temporal variations of the nonequilibrium carriers in graphene have been thoroughly described in terms of a defect-induced extrinsic effect known as ``supercollision'' (SC). The SC process is based on defect-mediated electron-acoustic phonon scattering and theoretically has been predicted to reduce with the increase of mobility of a material. Here, the authors have prepared extremely high mobility graphene and traced the dynamics of photoexcited carriers in the Dirac bands directly by time- and angle-resolved photoemission spectroscopy. They successfully observed suppression of SC and extracted the intrinsic dynamical properties of graphene, such as anharmonic decay of the optical phonons and the bottleneck relaxation at the Dirac point. Breaking the limit of SC, their research also has technological significance in developing graphene-based optoelectronic devices.

Alkali-metal adsorption on the surface of materials is widely used for in situ surface electron doping, particularly for observing unoccupied band structures by angle-resolved photoemission spectroscopy (ARPES). However, the effects of alkali-metal atoms on the resulting band structures have yet to be fully investigated, owing to difficulties in both experiments and calculations. Here, we combine ARPES measurements on cesium-adsorbed ultrathin bismuth films with first-principles calculations of the electronic charge densities and demonstrate a simple method to evaluate alkali-metal induced band deformation. We reveal that deformation of bismuth surface bands is directly correlated with vertical charge-density profiles at each electronic state of bismuth. In contrast, a change in the quantized bulk bands is well described by a conventional rigid-band-shift picture. We discuss these two aspects of the band deformation holistically, considering spatial distributions of the electronic states and cesium-bismuth hybridization, and provide a prescription for applying alkali-metal adsorption to a wide range of materials., Comment: 8 pages, 7 figures

Silicene, analogous to graphene, is a one-atom-thick two-dimensional crystal of silicon which is expected to share many of the remarkable properties of graphene. The buckled honeycomb structure of silicene, along with its enhanced spin-orbit coupling, endows silicene with considerable advantages over graphene in that the spin-split states in silicene are tunable with external fields. Although the low-energy Dirac cone states lie at the heart of all novel quantum phenomena in a pristine sheet of silicene, the question of whether or not these key states can survive when silicene is grown or supported on a substrate remains hotly debated. Here we report our direct observation of Dirac cones in monolayer silicene grown on a Ag(111) substrate. By performing angle-resolved photoemission measurements on silicene(3x3)/Ag(111), we reveal the presence of six pairs of Dirac cones on the edges of the first Brillouin zone of Ag(111), other than expected six Dirac cones at the K points of the primary silicene(1x1) Brillouin zone. Our result shows clearly that the unusual Dirac cone structure originates not from the pristine silicene alone but from the combined effect of silicene(3x3) and the Ag(111) substrate. This study identifies the first case of a new type of Dirac Fermion generated through the interaction of two different constituents. Our observation of Dirac cones in silicene/Ag(111) opens a new materials platform for investigating unusual quantum phenomena and novel applications based on two-dimensional silicon systems., 15 Pages, 4 Figures

The topology of pure Bi is controversial because of its very small ($\sim$10 meV) band gap. Here we perform high-resolution angle-resolved photoelectron spectroscopy measurements systematically on 14$-$202 bilayers Bi films. Using high-quality films, we succeed in observing quantized bulk bands with energy separations down to $\sim$10 meV. Detailed analyses on the phase shift of the confined wave functions precisely determine the surface and bulk electronic structures, which unambiguously show nontrivial topology. The present results not only prove the fundamental property of Bi but also introduce a capability of the quantum-confinement approach., Comment: 6 pages, 5 figures

Honeycomb structures of group IV elements can host massless Dirac fermions with non-trivial Berry phases. Their potential for electronic applications has attracted great interest and spurred a broad search for new Dirac materials especially in monolayer structures. We present a detailed investigation of the \beta 12 boron sheet, which is a borophene structure that can form spontaneously on a Ag(111) surface. Our tight-binding analysis revealed that the lattice of the \beta 12-sheet could be decomposed into two triangular sublattices in a way similar to that for a honeycomb lattice, thereby hosting Dirac cones. Furthermore, each Dirac cone could be split by introducing periodic perturbations representing overlayer-substrate interactions. These unusual electronic structures were confirmed by angle-resolved photoemission spectroscopy and validated by first-principles calculations. Our results suggest monolayer boron as a new platform for realizing novel high-speed low-dissipation devices., Comment: accepted for publication in Physical Review Letters