Possible Nodeless Superconducting Gaps in Bi_2Sr_2CaCu_2O_(8+δ) and YBa_2Cu_3O_(7-x) Revealed by Cross-Sectional Scanning Tunneling Spectroscopy

Pairing in the cuprate high-temperature superconductors and its origin remain among the most enduring mysteries in condensed matter physics. With cross-sectional scanning tunneling microscopy/spectroscopy, we clearly reveal the spatial-dependence or inhomogeneity of the superconducting gap structure of Bi2Sr2CaCu2O8＋δ （Bi2212） and YBa2Cu3O7-x （YBCO） along their c-axes on a scale shorter than the interlayer spacing. By tunneling into the （100） plane of a Bi2212 single crystal and a YBCO film, we observe both U-shaped tunneling spectra with extended fiat zero-conductance bottoms, and V-shaped gap structures, in different regions of each sample. On the YBCO film, tunneling into a （110） surface only reveals a U-shaped gap without any zero-bias peak. Our analysis suggests that the U-shaped gap is likely a nodeless superconducting gap. The V-shaped gap has a very small amplitude, and is likely proximity-induced by regions having the larger U-shaped gap.

Superconducting state in Ba_((1-x)) Sr_(x)Ni_(2)As_(2) near the quantum critical point

In the phase diagram of the nickel-based superconductor Ba_(1-x)Sr_(x)Ni_(2)As_(2),T_(C) has been found to be enhanced sixfold near the quantum critical point(QCP) x=0.71 compared with the parent compound.However,the mechanism is still under debate.Here,we report a detailed investigation of the superconducting properties near the QCP(x≈0.7) by utilizing scanning tunneling microscopy and spectroscopy.The temperature-dependent superconducting gap and magnetic vortex state were obtained and analyzed in the framework of the Bardeen-Cooper-Schrieffer model.The ideal isotropic s-wave superconducting gap excludes the long-speculated nematic fluctuations while preferring strong electron-phonon coupling as the mechanism for T_(C) enhancement near the QCP.The lower than expected gap ratio of Δ/(k_(B) T_(C)) is rooted in the fact that Ba_(1-x)Sr_(x)Ni_(2)As_(2) falls into the dirty limit with a serious pair breaking effect similar to the parent compound.

Microscopic growth mechanism and edge states of monolayer 1T'-MoTe_(2)

Transition metal ditellurides(TMTDs)have versatile physical properties,including non-trivial topology,Weyl semimetal states and unique spin texture.Controlled growth of high-quality and large-scale monolayer TMTDs with preferred crystal phases is crucial for their applications.Here,we demonstrate the epitaxial growth of 1T'-MoTe_(2) on Au(111)and graphitized silicon carbide(Gr/SiC)by molecular beam epitaxy(MBE).We investigate the morphology of the grown1T'-MoTe_(2) at the atomic level by scanning tunnelling microscopy(STM)and reveal the corresponding microscopic growth mechanism.It is found that the unique ordered Te structures preferentially deposited on Au(111)regulate the growth of monolayer single crystal 1T'-MoTe_(2),while the Mo clusters were preferentially deposited on the Gr/SiC substrate,which impedes the ordered growth of monolayer MoTe_(2).We confirm that the size of single crystal 1T'-MoTe_(2) grown on Au(111)is nearly two orders of magnitude larger than that on Gr/SiC.By scanning tunnelling spectroscopy(STS),we observe that the STS spectrum of the monolayer 1T'-MoTe_(2) nano-island at the edge is different from that at the interior,which exhibits enhanced conductivity.

Electronic states of domain walls in commensurate charge density wave ground state and mosaic phase in 1T-TaS_(2)

Domain walls(DWs)in the charge-density-wave(CDW)Mott insulator 1T-TaS_(2)have unique localized states,which play an important role in exploring the electronic properties of the material.However,the electronic states in DWs in 1TTaS_(2)have not been clearly understood,mostly due to the complex structures,phases,and interlayer stacking orders in the DW areas.Here,we explored the electronic states of DWs in the large-area CDW phase and mosaic phase of 1T-TaS_(2)by scanning tunneling spectroscopy.Due to the different densities of DWs,the electronic states of DWs show distinct features in these phases.In the large area CDW phase,both the domain and the DWs(DW1,DW2,DW4)have zero conductance at the Fermi level;while in the mosaic phase,they can be metallic or insulating depending on their environments.In areas with a high density of DWs,some electronic states were observed both on the DWs and within the domains,indicating delocalized states over the whole region.Our work contributes to further understanding of the interplay between CDW and electron correlations in 1T-TaS_(2).

Gate-controlled localization to delocalization transition of flat band wavefunction in twisted monolayer–bilayer graphene

Twisted graphene systems with flat bands have attracted much attention for they are excellent platforms to research novel quantum phases. Recently, transport measurements about twisted monolayer–bilayer graphene(t MBG) have shown the existence of correlated states and topological states in this system. However, the direct observations of the band structures and the corresponding spatial distributions are still not sufficient. Here we show that the distributions of flat bands in t MBG host two different modes by scanning tunneling microscopy and spectroscopy(STM/S). By tuning our t MBG device from the empty filling state to the full filling state through the back gate, we observe that the distributions of two flat bands develop from localized mode to delocalized mode. This gate-controlled flat band wavefunction polarization is unique to the t MBG system. Our work suggests that t MBG is promising to simulate both twisted bilayer graphene(TBG) and twisted double bilayer graphene(t DBG) and would be an ideal platform to explore novel moiré physics.

Identifi cation of Molecular Flipping of an Asymmetric Tris(phthalocyaninato)Lutetium Triple-Decker Complex by Scanning Tunneling Microscopy/Spectroscopy

The assembling behavior and electronic properties of asymmetric tris(phthalocyaninato)lutetium triple-decker sandwich complex molecules(Lu2Pc3)on highly oriented pyrolytic graphite(HOPG)surfaces have been studied by scanning tunneling microscopy/spectroscopy(STM/STS)methods.Phase transitions were observed at different bias polarities,involving an ordered packing arrangement with fourfold symmetry at negative bias and an amorphous arrangement at positive bias.Molecular switching behaviour for individual Lu2Pc3 molecules was reported here according to the bias-polarity-induced flipping phenomena and the peak shift in dI/dV versus V curves at different voltage scanning directions.The sensitive response of the strong intrinsic molecular dipole to an external electric field is proposed to be responsible for molecular switching of Lu_(2)Pc_(3)at the solid/liquid interface.

Bis(phthalocyaninato)yttrium Grown on Au(111): Electronic Structure of a Single Molecule and the Stability of Two- dimensional Films Investigated by Scanning Tunneling Microscopy/Spectroscopy at 4.8 K

Scanning tunneling microscopy/spectroscopy(STM/STS)at 4.8 K has been used to examine the growth of a double-decker bis(phthalocyaninato)yttrium(YP_(c2))molecule on a reconstructed Au(111)substrate.Local differential conductance spectra(dI/dV)of a single YPc2 molecule allow the characteristics of the highest occupied molecular orbital(HOMO)and the lowest unoccupied molecular orbital(LUMO)to be identified.Furthermore,lateral distributions of the local density of states(LDOS)have also been obtained by dI/dV mapping and confirmed by first principles simulations.These electronic feature mappings and theoretical calculations provide a basis for understanding the unique STM morphology of YPc2,which is usually imaged as an eight-lobed structure.In addition,we demonstrate that bias-dependent STM morphologies and simultaneous dI/dV maps can provide a way of understanding the stability of two-dimensional YP_(c2) films.

Chevron-type graphene nanoribbons with a reduced energy band gap:Solution synthesis,scanning tunneling microscopy and electrical characterization

Graphene nanoribbons(GNRs)attract a growing interest due to their tunable physical properties and promise for device applications.A variety of atomically precise GNRs have recently been synthesized by on-surface and solution approaches.While on-surface GNRs can be conveniently visualized by scanning tunneling microscopy(STM),and their electronic structure can be probed by scanning tunneling spectroscopy(STS),such characterization remains a great challenge for the solution-synthesized GNRs.Here,we report solution synthesis and detailed STM/STS characterization of atomically precise GNRs with a meandering shape that are structurally related to chevron GNRs but have a reduced energy band gap.The ribbons were synthesized by Ni0-mediated Yamamoto polymerization of specially designed molecular precursors using triflates as the leaving groups and oxidative cyclodehydrogenation of the resulting polymers using Scholl reaction.The ribbons were deposited onto III-V semiconducting InAs(110)substrates by a dry contact transfer technique.High-resolution STM/STS characterization not only confirmed the GNR geometry,but also revealed details of electronic structure including energy states,electronic band gap,as well as the spatial distribution of the local density of states.The experimental STS band gap of GNRs is about 2 eV,which is very close to 2.35 eV predicted by the density functional theory simulations with GW correction,indicating a weak screening effect of InAs(110)substrate.Furthermore,several aspects of GNR-InAs(110)substrate interactions were also probed and analyzed,including GNR tunable transparency,alignment to the substrate,and manipulations of GNR position by the STM tip.The weak interaction between the GNRs and the InAs(110)surface makes InAs(110)an ideal substrate for investigating the intrinsic properties of GNRs.Because of the reduced energy band gap of these ribbons,the GNR thin films exhibit appreciably high electrical conductivity and on/off ratios of about 10 in field-effect transistor measurements,suggesting their promise for device applications.

Realization of semiconducting Cu_(2)Se by direct selenization of Cu(111)

Bulk group IB transition-metal chalcogenides have been widely explored due to their applications in thermoelectrics.However,a layered two-dimensional form of these materials has been rarely reported.Here,we realize semiconducting Cu_(2)Se by direct selenization of Cu(111).Scanning tunneling microcopy measurements combined with first-principles calculations allow us to determine the structural and electronic properties of the obtained structure.X-ray photoelectron spectroscopy data reveal chemical composition of the sample,which is Cu_(2)Se.The observed moire pattern indicates a lattice mismatch between Cu_(2)Se and the underlying Cu(111)-√3×√3 surface.Differential conductivity obtained by scanning tunneling spectroscopy demonstrates that the synthesized Cu_(2)Se exhibits a band gap of 0.78 eV.Furthermore,the calculated density of states and band structure demonstrate that the isolated Cu_(2)Se is a semiconductor with an indirect band gap of-0.8 eV,which agrees quite well with the experimental results.Our study provides a simple pathway varying toward the synthesis of novel layered 2D transition chalcogenides materials.

Robustness of the unidirectional stripe order in the kagome superconductor CsV_(3)Sb_(5)

V-based kagome materials AV_(3)Sb_(5)(A=K,Rb,Cs)have attracted much attention due to their novel properties such as unconventional superconductivity,giant anomalous Hall effect,charge density wave(CDW)and pair density wave.Except for the 2a_(0)×2a_(0)CDW(charge density wave with in-plane 2×2 superlattice modulation)in AV_(3)Sb_(5),an additional 1×4(4a_(0))unidirectional stripe order has been observed at the Sb surface of Rb V3 Sb5 and CsV_(3)Sb_(5).However,the stability and electronic nature of the 4a_(0) stripe order remain controversial and unclear.Here,by using low-temperature scanning tunneling microscopy/spectroscopy(STM/S),we systematically study the 4a_(0) stripe order on the Sb-terminated surface of CsV_(3)Sb_(5).We find that the 4a_(0) stripe order is visible in a large energy range.The STM images with positive and negative bias show contrast inversion,which is the hallmark for the Peierls-type CDW.In addition,below the critical temperature about 60 K,the 4a_(0)stripe order keeps unaffected against the topmost Cs atoms,point defects,step edges and magnetic field up to 8 T.Our results provide experimental evidences on the existence of unidirectional CDW in CsV_(3)Sb_(5).

Recent advances in atomic imaging of organic-inorganic hybrid perovskites

Three-dimensional organic-inorganic hybrid perovskites(OHPs)hold a great prospect for photovoltaic applications due to their outstanding electronic and optical properties.These fascinating properties of OHPs in combination with their scalable and low-cost production make OHPs promising candidates for next-generation optoelectronic devices.The ability to obtain atomistic insights into physicochemical properties of this class of materials is crucial for the future development of this field.Recent advances in various scanning probe microscopy techniques have demonstrated their extraordinary capability in real-space imaging and spectroscopic measurements of the structural and electronic properties of OHPs with atomic-precision.Moreover,these techniques can be combined with light illumination to probe the structural and optoelectronic properties of OHPs close to the real device operation conditions.The primary focus of this review is to summarize the recent progress in atomic-scale studies of OHPs towards a deep understanding of the phenomena discovered in OHPs and OHP-based optoelectronic devices.

Edge-and strain-induced band bending in bilayer-monolayer Pb_(2)Se_(3) heterostructures

By using scanning tunneling microscope/microscopy(STM/STS), we reveal the detailed electronic structures around the sharp edges and strained terraces of lateral monolayer-bilayer Pd_(2)Se_(3) heterostructures. We find that the edges of such heterostructures are well-defined zigzag type. Band bending and alignment are observed across the zigzag edge, forming a monolayer-bilayer heterojunction. In addition, an n-type band bending is induced by strain on a confined bilayer Pd_(2)Se_(3) terrace. These results provide effective toolsets to tune the band structures in Pd_(2)Se_(3)-based heterostructures and devices.

Evolution of zinc morphology during continuous electrodeposition

The morphology evolution of zinc continuous electrodeposits with nano-sized crystals on the ferrite substrate has been studied by in-situ scanning tunnel spectroscopy (STM). It is found that the morphology of zinc electrodeposits varies from initial granules with a size of about 30nm to layered platelets with increasing deposition time. Meanwhile, the crystal structure of the zinc electrodeposits is identified to be hexagonal η-phase by X-ray diffraction. The orientation relationship between zinc crystals and the substrate surface can be interpreted in terms of the misfit and the atomic correspondence of the interphase boundary between the η-phase deposits and α-Fe substrate.

Epitaxial synthesis and electronic properties of monolayer Pd2Se3

Two-dimensional(2D)materials received large amount of studies because of the enormous potential in basic science and industrial applications.Monolayer Pd2Se3 is a fascinating 2D material that was predicted to possess excellent thermoelectric,electronic,transport,and optical properties.However,the fabrication of large-scale and high-quality monolayer Pd2Se3 is still challenging.Here,we report the synthesis of large-scale and high-quality monolayer Pd2Se3 on graphene-SiC(0001)by a two-step epitaxial growth.The atomic structure of Pd2Se3 was investigated by scanning tunneling microscope(STM)and confirmed by non-contact atomic force microscope(nc-AFM).Two subgroups of Se atoms have been identified by nc-AFM image in agreement with the theoretically predicted atomic structure.Scanning tunneling spectroscopy(STS)reveals a bandgap of 1.2 eV,suggesting that monolayer Pd2Se3 can be a candidate for photoelectronic applications.The atomic structure and defect levels of a single Se vacancy were also investigated.The spatial distribution of STS near the Se vacancy reveals a highly anisotropic electronic behavior.The two-step epitaxial synthesis and characterization of Pd2Se3 provide a promising platform for future investigations and applications.

Signatures of strong interlayer coupling inγ-InSe revealed by local differential conductivity

Interlayer coupling in layered semiconductors can significantly affect their optoelectronic properties.However,understanding the mechanisms behind the interlayer coupling at the atomic level is not straightforward.Here,we study modulations of the electronic structure induced by the interlayer coupling in theγ-phase of indium selenide(γ-InSe)using scanning probe techniques.We observe a strong dependence of the energy gap on the sample thickness and a small effective mass along the stacking direction,which are attributed to strong interlayer coupling.In addition,the moirépatterns observed inγ-InSe display a small band-gap variation and nearly constant local differential conductivity along the patterns.This suggests that modulation of the electronic structure induced by the moirépotential is smeared out,indicating the presence of a significant interlayer coupling.Our theoretical calculations confirm that the interlayer coupling inγ-InSe is not only of the van der Waals origin,but also exhibits some degree of hybridization between the layers.Strong interlayer coupling might play an important role in the performance ofγ-InSe-based devices.

Selective formation of ultrathin PbSe on Ag(111)

Two-dimensional(2D)semiconductors,such as lead selenide(PbSe),locate at the key position of next-generation devices.However,the ultrathin PbSe is still rarely reported experimentally,particularly on metal substrates.Here,we report the ultrathin PbSe synthesized via sequential molecular beam epitaxy on Ag(111).The scanning tunneling microscopy is used to resolve the atomic structure and confirms the selective formation of ultrathin PbSe through the reaction between Ag5Se2 and Pb,as further evidenced by the theoretical calculation.It is also found that the increased accumulation of Pb leads to the improved quality of PbSe with larger and more uniform films.The detailed analysis demonstrates the bilayer structure of synthesized PbSe,which could be deemed to achieve the 2D limit.The differential conductance spectrum reveals a metallic feature of the PbSe film,indicating a certain interaction between PbSe and Ag(111).Moreover,the moirépattern originated from the lattice mismatch between PbSe and Ag(111)is observed,and this moirésystem provides the opportunity for studying physics under periodical modulation and for device applications.Our work illustrates a pathway to selectively synthesize ultrathin PbSe on metal surfaces and suggests a 2D experimental platform to explore PbSe-based opto-electronic and thermoelectric phenomena.

Uncovering the magnetic response of open-shell graphene nanostructures on metallic surfaces at different doping levels

Open-shell graphene nanostructures(GNs)are promising candidates for future spintronics and quantum technologies.Recent progress based on on-surface synthetic approach has successfully created such GNs on metallic surfaces.Meanwhile,the doping effect of metallic surfaces is inevitably present and can significantly tune their electronic and magnetic properties.Here,we investigate the zigzag end states of open-shell 7-armchair graphene nanoribbons(7-AGNRs)on Au(111),Au(100)and Ag(111)surfaces.Combined with the manipulation of a scanning tunneling microscope,we demonstrate that the end states can be tuned from empty states to singly occupied states and to doubly occupied states by substrate doping.Furthermore,the singly occupied states can be finely tuned,with the occupancy number of the states and related magnetic behaviors uncovered by experiments at different temperatures and magnetic fields.Our results provide a comprehensive study of the magnetic response of open-shell GNs on metallic surfaces at different doping levels.

Superconductivity and pseudogap features of an isolated FeAs layer in KCa_(2)Fe_(4)As_(4)F_(2) unraveled by STM/STS

To reveal the intrinsic properties of the basic superconducting units,i.e.,the single layered FeSe/FeAs in iron-based superconductors or CuO_(2) planes in cuprate superconductors,is a necessary prerequisite for understanding the mechanism of high-Tc superconductivity.Up to now,an isolated FeAs layer has rarely been studied due to the difficulty in materials synthesis.Here,we report a scanning tunneling microscopy/spectroscopy(STM/STS)study on the iron-based superconductor KCa_(2)Fe_(4)As_(4)F_(2).In situ cleavage produced a single FeAs layer covered by a reconstructed K surface,which is isolated from the bulk by the underlying CaF layer and shows multi-band superconductivity with a much lower T_(c) than its bulk counterpart.In the exposed As-terminated regions with coverage of scattered K atoms,a pseudogap was observed,leading to an inhomogeneous superconductivity without long-range phase coherence in real space,which is remarkably similar to the high-T_(c) cuprate superconductors.These results provide a new perspective to understanding the origin of superconductivity in iron-based superconductors.

Atomically constructing a van der Waals heterostructure of CrTe_(2)/Bi_(2)Te_(3) by molecular beam epitaxy

A 2D heterostructure with proximity coupling of magnetism and topology can provide enthralling prospects for hosting new quantum states and exotic properties that are relevant to next-generation spintronic devices.Here,we synthesize a delicate van der Waals(vdW)heterostructure of CrTe_(2)/Bi_(2)Te_(3) at the atomic scale via molecular beam epitaxy.Low-temperature scanning tunneling microscopy/spectroscopy measurements are utilized to characterize the geometric and electronic properties of the CrTe_(2)/Bi_(2)Te_(3) heterostructure with a compressed vdW gap.Detailed structural analysis reveals complex interfacial structures with diversiform step heights and intriguing moirépatterns.The formation of the interface is ascribed to the embedded characteristics of CrTe_(2) and Bi_(2)Te_(3) by sharing Te atomic layer upon interfacing,showing intercoupled features of electronic structure for CrTe_(2) and Bi_(2)Te_(3).Our study demonstrates a possible approach to construct artificial heterostructures with different types of ordered states,which may be of use for achieving tunable interfacial Dzyaloshinsky–Moriya interactions and tailoring the functional building blocks in low dimensions.

Anisotropic monolayer of ReX_(2)on Au foils for exploring abnormal growth behavior and electronic properties

As an emerging class of semiconducting transition metal dichalcogenides(TMDCs),two-dimensional(2D)rhenium dichalcogenides(ReX_(2),X=S or Se)have recently aroused great research interest due to their unique anisotropic structure(1T′phase),and the related novel properties and applications.Recently,many efforts have been devoted to the controllable syntheses of high-quality monolayer or few-layer ReX_(2)flakes/films by chemical vapor deposition(CVD),wherein the metallic Au foil is found to be a unique substrate,due to the relatively strong interfacial coupling between monolayer ReX_(2)and Au.And the conductive nature of Au enables in situ characterizations of the as-grown ReX_(2)samples,which is essential for exploring the fundamental properties and internal growth mechanisms.Hereby,this review focuses on the recent progresses on the CVD syntheses and in situ characterizations of high-quality monolayer ReX_(2)flakes/films and their heterostructures with graphene on Au foils.The effects of Au foils on improving the crystal quality and inducing the growth of monolayer ReX_(2)single crystals are intensively addressed.The crystallinity,domain morphology,atomic and electronic structures,as well as the growth behaviors of monolayer ReX_(2)flakes/films and graphene/ReX_(2)heterostructures on Au revealed by in situ characterization techniques are also highlighted.As contrasts,the growth behaviors of monolayer or few-layer ReX_(2)on insulating substrates are also discussed.Besides,the potential applications of 2D ReX_(2)in new-generation electronic,optoelectronic devices,and energy-related fields are also introduced.Finally,future research directions are also prospected for propelling the practical applications of 2D ReX_(2)materials in more versatile fields.