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1.
Nano Lett ; 23(21): 9704-9710, 2023 Nov 08.
Article in English | MEDLINE | ID: mdl-37870505

ABSTRACT

Quantum spins, also known as spin operators that preserve SU(2) symmetry, lack a specific orientation in space and are hypothesized to display unique interactions with superconductivity. However, spin-orbit coupling and crystal field typically cause a significant magnetic anisotropy in d/f shell spins on surfaces. Here, we fabricate atomically precise S = 1/2 magnetic nanographenes on Pb(111) through engineering sublattice imbalance in the graphene honeycomb lattice. Through tuning the magnetic exchange strength between the unpaired spin and Cooper pairs, a quantum phase transition from the singlet to the doublet state has been observed, consistent with the quantum spin models. From our calculations, the particle-hole asymmetry is induced by the Coulomb scattering potential and gives a transition point about kBTk ≈ 1.6Δ. Our work demonstrates that delocalized π electron magnetism hosts highly tunable magnetic bound states, which can be further developed to study the Majorana bound states and other rich quantum phases of low-dimensional quantum spins on superconductors.

2.
J Am Chem Soc ; 145(13): 7136-7146, 2023 Apr 05.
Article in English | MEDLINE | ID: mdl-36951172

ABSTRACT

The emergence of quantum magnetism in nanographenes provides ample opportunities to fabricate purely organic devices for spintronics and quantum information. Although heteroatom doping is a viable way to engineer the electronic properties of nanographenes, the synthesis of doped nanographenes with collective quantum magnetism remains elusive. Here, a set of nitrogen-doped nanographenes (N-NGs) with atomic precision are fabricated on Au(111) through a combination of imidazole [2+2+2]-cyclotrimerization and cyclodehydrogenation reactions. High-resolution scanning probe microscopy measurements reveal the presence of collective quantum magnetism for nanographenes with three radicals, with spectroscopic features which cannot be captured by mean-field density functional theory calculations but can be well reproduced by Heisenberg spin model calculations. In addition, the mechanism of magnetic exchange interaction of N-NGs has been revealed and compared with their counterparts with pure hydrocarbons. Our findings demonstrate the bottom-up synthesis of atomically precise N-NGs which can be utilized to fabricate low-dimensional extended graphene nanostructures for realizing ordered quantum phases.

3.
Nano Lett ; 22(18): 7651-7658, 2022 Sep 28.
Article in English | MEDLINE | ID: mdl-36066512

ABSTRACT

The metal-intercalated bilayer graphene has a flat band with a high density of states near the Fermi energy and thus is anticipated to exhibit an enhanced strong correlation effect and associated fascinating phenomena, including superconductivity. By using a self-developed multifunctional scanning tunneling microscope, we succeeded in observing the superconducting energy gap and diamagnetic response of a Ca-intercalated bilayer graphene below a critical temperature of 8.83 K. The revealed high value of gap ratio, 2Δ/kBTc ≈ 5.0, indicates a strong coupling superconductivity, while the variation of penetration depth with temperature and magnetic field indicates an isotropic s-wave superconductor. These results provide crucial experimental clues for understanding the origin and mechanism of superconductivity in carrier-doped graphene.

4.
Phys Rev Lett ; 128(20): 206802, 2022 May 20.
Article in English | MEDLINE | ID: mdl-35657877

ABSTRACT

High-quality stanene films have been actively pursued for realizing not only quantum spin Hall edge states without backscattering, but also intrinsic superconductivity, two central ingredients that may further endow the systems to host topological superconductivity. Yet to date, convincing evidence of topological edge states in stanene remains to be seen, let alone the coexistence of these two ingredients, owing to the bottleneck of growing high-quality stanene films. Here we fabricate one- to five-layer stanene films on the Bi(111) substrate and observe the robust edge states using scanning tunneling microscopy/spectroscopy. We also measure distinct superconducting gaps on different-layered stanene films. Our first-principles calculations further show that hydrogen passivation plays a decisive role as a surfactant in improving the quality of the stanene films, while the Bi substrate endows the films with nontrivial topology. The coexistence of nontrivial topology and intrinsic superconductivity renders the system a promising candidate to become the simplest topological superconductor based on a single-element system.

5.
Phys Rev Lett ; 126(17): 176102, 2021 Apr 30.
Article in English | MEDLINE | ID: mdl-33988396

ABSTRACT

Deposition of Bi on InSb(111)B reveals a striking Sierpinski-triangle (ST)-like structure in Bi thin films. Such a fractal geometric topology is further shown to turn off the intrinsic electronic topology in a thin film. Relaxation of a huge misfit strain of about 30% to 40% between Bi adlayer and substrate is revealed to drive the ST-like island formation. A Frenkel-Kontrova model is developed to illustrate the enhanced strain relief in the ST islands offsetting the additional step energy cost. Besides a sufficiently large tensile strain, forming ST-like structures also requires larger adlayer-substrate and intra-adlayer elastic stiffnesses, and weaker intra-adlayer interatomic interactions.

6.
J Am Chem Soc ; 142(43): 18532-18540, 2020 Oct 28.
Article in English | MEDLINE | ID: mdl-32959653

ABSTRACT

The porphyrin macrocycle can stabilize a set of magnetic metal ions, thus introducing localized net spins near the center. However, it remains elusive but most desirable to introduce delocalized spins in porphyrins with wide implications, for example, for building correlated quantum spins. Here, we demonstrate that metal-free porphyrins host delocalized π-electron magnetism, as revealed by scanning probe microscopy and a different level of theory calculations. Our results demonstrate that engineering of π-electron topologies introduces a spin-polarized singlet state and delocalized net spins in metal-free porphyrins. In addition, the π-electron magnetism can be switched on/off via scanning tunneling microscope manipulation by tuning the interfacial charge transfer. Our results provide an effective way to precisely control the π-electron magnetism in metal-free porphyrins, which can be further extended to design new magnetic functionalities of porphyrin-based architectures.

7.
J Am Chem Soc ; 142(22): 10034-10041, 2020 Jun 03.
Article in English | MEDLINE | ID: mdl-32372644

ABSTRACT

The quinoid structure, a resonance structure of benzenoid, gives rise to peculiar chemical reactivity and physical properties. A complete characterization of its geometric and electronic properties on the atomic scale is of vital importance to understand and engineer the chemical and physical properties of quinoid molecules. Here, we report a real-space structural and electronic characterization of quinoid poly(para-phenylene) (PPP) chains by using noncontact atomic force microscopy and scanning tunneling microscopy. Our results reveal that quinoid PPP chains adopt a coplanar adsorption configuration on Cu(111) and host in-gap states near Fermi level. In addition, intra- and interchain hopping of quinoid structure are observed, indicative of a quasiparticle behavior originating from charge-lattice interactions. The experimental results are nicely reproduced by tight-binding calculations. Our study provides a comprehensive understanding of the structural and electronic properties of quinoid PPP chains in real space and may be further extended to address the dynamics of nonlinear excitations in quinoid molecules.

8.
Phys Rev Lett ; 125(4): 046801, 2020 Jul 24.
Article in English | MEDLINE | ID: mdl-32794806

ABSTRACT

A quantum spin hall insulator is manifested by its conducting edge channels that originate from the nontrivial topology of the insulating bulk states. Monolayer 1T^{'}-WTe_{2} exhibits this quantized edge conductance in transport measurements, but because of its semimetallic nature, the coherence length is restricted to around 100 nm. To overcome this restriction, we propose a strain engineering technique to tune the electronic structure, where either a compressive strain along the a axis or a tensile strain along the b axis can drive 1T^{'}-WTe_{2} into an full gap insulating phase. A combined study of molecular beam epitaxy and in situ scanning tunneling microscopy or spectroscopy then confirmed such a phase transition. Meanwhile, the topological edge states were found to be very robust in the presence of strain.

9.
Phys Rev Lett ; 125(13): 136802, 2020 Sep 25.
Article in English | MEDLINE | ID: mdl-33034492

ABSTRACT

Superconducting topological crystalline insulators (TCIs) have been proposed to be a new type of topological superconductor where multiple Majorana zero modes may coexist under the protection of lattice symmetries. The bulk superconductivity of TCIs has been realized, but it is quite challenging to detect the superconductivity of topological surface states inside their bulk superconducting gaps. Here, we report high-resolution scanning tunneling spectroscopy measurements on lateral Sn_{1-x}Pb_{x}Te-Pb heterostructures using superconducting tips. Both the bulk superconducting gap and the multiple in-gap states with energy differences of ∼0.3 meV can be clearly resolved on TCI Sn_{1-x}Pb_{x}Te at 0.38 K. Quasiparticle interference measurements further confirm the in-gap states are gapless. Our work demonstrates that the unique topological superconductivity of a TCI can be directly distinguished in the density of states, which helps to further investigate the multiple Dirac and Majorana fermions inside the superconducting gap.

10.
Phys Rev Lett ; 124(14): 147206, 2020 Apr 10.
Article in English | MEDLINE | ID: mdl-32338972

ABSTRACT

Nanographenes with sublattice imbalance host a net spin according to Lieb's theorem for bipartite lattices. Here, we report the on-surface synthesis of atomically precise nanographenes and their atomic-scale characterization on a gold substrate by using low-temperature noncontact atomic force microscopy and scanning tunneling spectroscopy. Our results clearly confirm individual nanographenes host a single spin of S=1/2 via the Kondo effect. In covalently linked nanographene dimers, two spins are antiferromagnetically coupled with each other as revealed by inelastic spin-flip excitation spectroscopy. The magnetic exchange interaction in dimers can be well engineered by tuning the local spin density distribution near the connection region, consistent with mean-field Hubbard model calculations. Our work clearly reveals the emergence of magnetism in nanographenes and provides an efficient way to further explore the carbon-based magnetism.

11.
Nanotechnology ; 31(30): 305708, 2020 Jul 24.
Article in English | MEDLINE | ID: mdl-32259801

ABSTRACT

Low dimensional superconductors have many unusual properties. When 0-dimensional superconductors reach the nanometer scale, the superconducting energy gap can be enhanced due to the shell effect. At the same time, the single electron Coulomb blockade effect can also be observed on metal nanoparticles if they are weakly coupled to the environment. So, if a superconducting nanoparticle is isolated well from the environment, the superconducting gap and the Coulomb gap would couple together, making the tunneling spectrum more complicated and interesting. Here Sn nanoparticles were deposited on the surface of STO (111). The charging energy of a nanoparticle mainly depends on its size and is comparable to the superconducting gap when the isolated particle is large enough. The superconducting energy gap can be deduced from the coupling tunneling spectrum and the shell effect is observed. The method to deduce the superconducting gap here is simpler than when fit using the Dynes density of states. Owing to the increased superconducting gap and critical field, the studied nanoparticles may find applications in studies of the properties of Majorana fermions.

12.
Phys Rev Lett ; 123(25): 257001, 2019 Dec 20.
Article in English | MEDLINE | ID: mdl-31922797

ABSTRACT

Intrigued by the discovery of high-temperature superconductivity in a single unit-cell layer of FeSe film on SrTiO_{3}, researchers recently found large superconductinglike energy gaps in K-adsorbed multilayer FeSe films by angle-resolved photoemission and scanning tunneling spectroscopy. However, the existence and nature of the high-temperature superconductivity inferred by the spectroscopic studies has not been investigated by measurements of zero resistance or the Meissner effect due to the fragility of K atoms in air. Using a self-developed multifunctional scanning tunneling microscope, we succeed in observing the diamagnetic response of K-adsorbed multilayer FeSe films, and thus find a dome-shaped relation between the critical temperature (T_{c}) and K coverage. Intriguingly, T_{c} exhibits an approximately linear dependence on the superfluid density in the whole K adsorbed region. Moreover, the quadratic low-temperature variation in the London penetration depth indicates a sign-reversal order parameter. These results provide compelling information towards further understanding of the high-temperature superconductivity in FeSe-derived superconductors.

13.
Chemphyschem ; 20(18): 2394-2397, 2019 09 17.
Article in English | MEDLINE | ID: mdl-31025456

ABSTRACT

On-surface synthesis provides a convenient route to many kinds of conjugated molecular nanostructures, but it has remained challenging to precisely control the reaction pathway for using multicomponent precursors. Herein, we demonstrate a two-step strategy to synthesize iron phthalocyanine (FePc) molecules using metal-organic coordination for templating by using high-resolution scanning tunnelling microscopy and non-contact atomic force microscopy. In a first step, 1,2,4,5-tetracyanobenzene (TCNB) precursors and Fe atoms self-assembly into Fe(TCNB)4 coordination complexes on a clean Au(111) surface. The Fe(TCNB)4 complexes further undergo cyclic tetramerization upon thermal annealing, forming single FePc molecules. We expect that our demonstrated synthetic strategy may shed light on the design and synthesis of two-dimensional extended conjugated systems.

14.
Nano Lett ; 17(5): 3035-3039, 2017 05 10.
Article in English | MEDLINE | ID: mdl-28415840

ABSTRACT

Ultrathin freestanding bismuth film is theoretically predicted to be one kind of two-dimensional topological insulators. Experimentally, the topological nature of bismuth strongly depends on the situations of the Bi films. Film thickness and interaction with the substrate often change the topological properties of Bi films. Using angle-resolved photoemission spectroscopy, scanning tunneling microscopy or spectroscopy and first-principle calculation, the properties of Bi(111) ultrathin film grown on the NbSe2 superconducting substrate have been studied. We find the band structures of the ultrathin film is quasi-freestanding, and one-dimensional edge state exists on Bi(111) film as thin as three bilayers. Superconductivity is also detected on different layers of the film and the pairing potential exhibits an exponential decay with the layer thicknesses. Thus, the topological edge state can coexist with superconductivity, which makes the system a promising platform for exploring Majorana Fermions.

15.
Nat Mater ; 14(3): 285-9, 2015 Mar.
Article in English | MEDLINE | ID: mdl-25419814

ABSTRACT

Recent experiments on FeSe films grown on SrTiO3 (STO) suggest that interface effects can be used as a means to reach superconducting critical temperatures (Tc) of up to 80 K (ref. ). This is nearly ten times the Tc of bulk FeSe and higher than the record value of 56 K for known bulk Fe-based superconductors. Together with recent studies of superconductivity at oxide heterostructure interfaces, these results rekindle the long-standing idea that electron pairing at interfaces between two different materials can be tailored to achieve high-temperature superconductivity. Subsequent angle-resolved photoemission spectroscopy measurements of the FeSe/STO system revealed an electronic structure distinct from bulk FeSe (refs , ), with an energy gap vanishing at around 65 K. However, ex situ electrical transport measurements have so far detected zero resistance-the key experimental signature of superconductivity-only below 30 K. Here, we report the observation of superconductivity with Tc above 100 K in the FeSe/STO system by means of in situ four-point probe electrical transport measurements. This finding confirms FeSe/STO as an ideal material for studying high-Tc superconductivity.

16.
Nat Mater ; 14(10): 1020-5, 2015 Oct.
Article in English | MEDLINE | ID: mdl-26237127

ABSTRACT

Following the first experimental realization of graphene, other ultrathin materials with unprecedented electronic properties have been explored, with particular attention given to the heavy group-IV elements Si, Ge and Sn. Two-dimensional buckled Si-based silicene has been recently realized by molecular beam epitaxy growth, whereas Ge-based germanene was obtained by molecular beam epitaxy and mechanical exfoliation. However, the synthesis of Sn-based stanene has proved challenging so far. Here, we report the successful fabrication of 2D stanene by molecular beam epitaxy, confirmed by atomic and electronic characterization using scanning tunnelling microscopy and angle-resolved photoemission spectroscopy, in combination with first-principles calculations. The synthesis of stanene and its derivatives will stimulate further experimental investigation of their theoretically predicted properties, such as a 2D topological insulating behaviour with a very large bandgap, and the capability to support enhanced thermoelectric performance, topological superconductivity and the near-room-temperature quantum anomalous Hall effect.

17.
Phys Rev Lett ; 116(25): 257003, 2016 Jun 24.
Article in English | MEDLINE | ID: mdl-27391745

ABSTRACT

Recently, theory has predicted a Majorana zero mode (MZM) to induce spin selective Andreev reflection (SSAR), a novel magnetic property which can be used to detect the MZM. Here, spin-polarized scanning tunneling microscopy or spectroscopy has been applied to probe SSAR of MZMs in a topological superconductor of the Bi_{2}Te_{3}/NbSe_{2} heterostructure. The zero-bias peak of the tunneling differential conductance at the vortex center is observed substantially higher when the tip polarization and the external magnetic field are parallel rather than antiparallel to each other. This spin dependent tunneling effect provides direct evidence of MZM and reveals its magnetic property in addition to the zero energy modes. Our work will stimulate MZM research on these novel physical properties and, hence, is a step towards experimental study of their statistics and application in quantum computing.

18.
Proc Natl Acad Sci U S A ; 110(8): 2758-62, 2013 Feb 19.
Article in English | MEDLINE | ID: mdl-23382185

ABSTRACT

Topological insulators and graphene present two unique classes of materials, which are characterized by spin-polarized (helical) and nonpolarized Dirac cone band structures, respectively. The importance of many-body interactions that renormalize the linear bands near Dirac point in graphene has been well recognized and attracted much recent attention. However, renormalization of the helical Dirac point has not been observed in topological insulators. Here, we report the experimental observation of the renormalized quasiparticle spectrum with a skewed Dirac cone in a single Bi bilayer grown on Bi(2)Te(3) substrate from angle-resolved photoemission spectroscopy. First-principles band calculations indicate that the quasiparticle spectra are likely associated with the hybridization between the extrinsic substrate-induced Dirac states of Bi bilayer and the intrinsic surface Dirac states of Bi(2)Te(3) film at close energy proximity. Without such hybridization, only single-particle Dirac spectra are observed in a single Bi bilayer grown on Bi(2)Se(3), where the extrinsic Dirac states Bi bilayer and the intrinsic Dirac states of Bi(2)Se(3) are well separated in energy. The possible origins of many-body interactions are discussed. Our findings provide a means to manipulate topological surface states.

19.
Sensors (Basel) ; 16(4)2016 Apr 09.
Article in English | MEDLINE | ID: mdl-27070618

ABSTRACT

Arc faults can produce very high temperatures and can easily ignite combustible materials; thus, they represent one of the most important causes of electrical fires. The application of arc fault detection, as an emerging early fire detection technology, is required by the National Electrical Code to reduce the occurrence of electrical fires. However, the concealment, randomness and diversity of arc faults make them difficult to detect. To improve the accuracy of arc fault detection, a novel arc fault detector (AFD) is developed in this study. First, an experimental arc fault platform is built to study electrical fires. A high-frequency transducer and a current transducer are used to measure typical load signals of arc faults and normal states. After the common features of these signals are studied, high-frequency energy and current variations are extracted as an input eigenvector for use by an arc fault detection algorithm. Then, the detection algorithm based on a weighted least squares support vector machine is designed and successfully applied in a microprocessor. Finally, an AFD is developed. The test results show that the AFD can detect arc faults in a timely manner and interrupt the circuit power supply before electrical fires can occur. The AFD is not influenced by cross talk or transient processes, and the detection accuracy is very high. Hence, the AFD can be installed in low-voltage circuits to monitor circuit states in real-time to facilitate the early detection of electrical fires.

20.
Phys Rev Lett ; 114(1): 017001, 2015 Jan 09.
Article in English | MEDLINE | ID: mdl-25615497

ABSTRACT

Majorana fermions have been intensively studied in recent years for their importance to both fundamental science and potential applications in topological quantum computing. They are predicted to exist in a vortex core of superconducting topological insulators. However, it is extremely difficult to distinguish them experimentally from other quasiparticle states for the tiny energy difference between Majorana fermions and these states, which is beyond the energy resolution of most available techniques. Here, we circumvent the problem by systematically investigating the spatial profile of the Majorana mode and the bound quasiparticle states within a vortex in Bi(2)Te(3) films grown on a superconductor NbSe(2). While the zero bias peak in local conductance splits right off the vortex center in conventional superconductors, it splits off at a finite distance ∼20 nm away from the vortex center in Bi(2)Te(3). This unusual splitting behavior has never been observed before and could be possibly due to the Majorana fermion zero mode. While the Majorana mode is destroyed by the interaction between vortices, the zero bias peak splits as a conventional superconductor again. This work provides self-consistent evidences of Majorana fermions and also suggests a possible route to manipulating them.

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