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Hong-Jun Gao

Publications and source records attributed to Hong-Jun Gao.

At least 73 records · Page 4Linked to original sources

Emergent Electronic Kagome Lattice in Correlated Charge-Density-Wave State of 1T-TaS$_2$

Quantum materials with tunable correlated and/or topological electronic states, such as the electronic Kagome lattice, provide an ideal platform to study the exotic quantum properties. However, the real-space investigations on the correlated electronic Kagome lattice have been rarely reported. Herein, we report on the electronic Kagome lattice emerging in the correlated charge-density-wave (CDW) state of 1T-TaS$_2$ at ~200 K via variable-temperature scanning tunneling microscopy (VT-STM). This emergent Kagome lattice can be considered a fractional electron-filling superstructure with reduced translational and rotational symmetries, confirmed by STM measurements and density functional theory simulations. The characteristic band structure and density of states of this electronic Kagome lattice are further explored based on theoretical calculations. Our results demonstrate a self-organized electronic Kagome lattice from the correlated CDW state via the effective tuning parameter of temperature and provide a platform to directly explore the interplay of correlated electrons and topological physics.

cond-mat.mtrl-sci↗

Non-trivial band topology and orbital-selective electronic nematicity in a new titanium-based kagome superconductor

Electronic nematicity that spontaneously breaks rotational symmetry has been shown as a generic phenomenon in correlated quantum systems including high-temperature superconductors and the AV3Sb5 (A = K, Rb, Cs) family with a kagome network. Identifying the driving force has been a central challenge for understanding nematicity. In iron-based superconductors, the problem is complicated because the spin, orbital and lattice degrees of freedom are intimately coupled. In vanadium-based kagome superconductors AV3Sb5, the electronic nematicity exhibits an intriguing entanglement with the charge density wave order (CDW), making understanding its origin difficult. Recently, a new family of titanium-based kagome superconductors ATi3Bi5 has been synthesized. In sharp contrast to its vanadium-based counterpart, the electronic nematicity occurs in the absence of CDW. ATi3Bi5 provides a new window to explore the mechanism of electronic nematicity and its interplay with the orbital degree of freedom. Here, we combine polarization-dependent angle-resolved photoemission spectroscopy with density functional theory to directly reveal the band topology and orbital characters of the multi-orbital RbTi3Bi5. The promising coexistence of flat bands, type-II Dirac nodal line and nontrivial Z2 topological states is identified in RbTi3Bi5. Remarkably, our study clearly unveils the orbital character change along the G-M and G-K directions, implying a strong intrinsic inter-orbital coupling in the Ti-based kagome metals, reminiscent of iron-based superconductors. Furthermore, doping-dependent measurements directly uncover the orbital-selective features in the kagome bands, which can be well explained by the d-p hybridization. The suggested d-p hybridization, in collaboration with the inter-orbital coupling, could account for the electronic nematicity in ATi3Bi5.

cond-mat.supr-con↗

Superconductivity and orbital-selective nematic order in a new titanium-based kagome metal CsTi3Bi5

Fabrication of new types of superconductors with novel physical properties has always been a major thread in the research of superconducting materials. An example is the enormous interests generated by the cascade of correlated topological quantum states in the newly discovered vanadium-based kagome superconductors AV3Sb5 (A=K, Rb, and Cs) with a Z2 topological band structure. Here we report the successful fabrication of single-crystals of titanium-based kagome metal CsTi3Bi5 and the observation of superconductivity and electronic nematicity. The onset of the superconducting transition temperature Tc is around 4.8 K. In sharp contrast to the charge density wave superconductor AV3Sb5, we find that the kagome superconductor CsTi3Bi5 preserves translation symmetry, but breaks rotational symmetry and exhibits an electronic nematicity. The angular-dependent magnetoresistivity shows a remarkable two-fold rotational symmetry as the magnetic field rotates in the kagome plane. The scanning tunneling microscopy and spectroscopic imaging detect rotational-symmetry breaking C2 quasiparticle interference patterns (QPI) at low energies, providing further microscopic evidence for electronic nematicity. Combined with first-principle calculations, we find that the nematic QPI is orbital-selective and dominated by the Ti dxz and dyz orbitals, possibly originating from the intriguing orbital bond nematic order. Our findings in the new "135" material CsTi3Bi5 provide new directions for exploring the multi-orbital correlation effect and the role of orbital or bond order in the electron liquid crystal phases evidenced by the symmetry breaking states in kagome superconductors.

cond-mat.supr-con↗

Tunable vortex Majorana modes controlled by strain in homogeneous LiFeAs

The iron-based superconductors (FeSCs) have recently emerged as a promising single-material Majorana platform by hosting isolated Majorana zero modes (MZMs) at relatively high temperatures. To further verify its Majorana nature and move forward to build topological quantum qubit, it is highly desirable to achieve tunability for MZMs on homogeneous FeSCs. Here, with an in-situ strain device, we can controllably create MZMs on the homogeneous surface of stoichiometric superconductor LiFeAs by inducing a topological phase transition. The evolution of discrete energy modes inside a strained vortex is found to mimics exactly as the predicted topological vortex case, proving the Majorana nature of emerging zero modes of vortex. Such tunability of MZMs in a homogeneous superconductor is an important step toward their application in topological quantum computation.

cond-mat.supr-con↗

Titanium doped kagome superconductor CsV3-xTixSb5 and two distinct phases

The vanadium-based kagome superconductor CsV3Sb5 has attracted tremendous attention due to its unexcepted anomalous Hall effect (AHE), charge density waves (CDWs), nematicity, and a pseudogap pair density wave (PDW) coexisting with unconventional strong-coupling superconductivity (SC). The origins of CDWs, unconventional SC, and their correlation with different electronic states in this kagome system are of great significance, but so far, are still under debate. Chemical doping in the kagome layer provides one of the most direct ways to reveal the intrinsic physics, but remains unexplored. Here, we report, for the first time, the synthesis of Ti-substituted CsV3Sb5 single crystals and its rich phase diagram mapping the evolution of intertwining electronic states. The Ti atoms directly substitute for V in the kagome layers. CsV3-xTixSb5 shows two distinct SC phases upon substitution. The Ti slightly-substituted phase displays an unconventional V-shaped SC gap, coexisting with weakening CDW, PDW, AHE, and nematicity. The Ti highly-substituted phase has a U-shaped SC gap concomitant with a short-range rotation symmetry breaking CDW, while long-range CDW, twofold symmetry of in-plane resistivity, AHE, and PDW are absent. Furthermore, we also demonstrate the chemical substitution of V atoms with other elements such as Cr and Nb, showing a different modulation on the SC phase and CDWs. These findings open up a way to synthesise a new family of doped CsV3Sb5 materials, and further representing a new platform for tuning the different correlated electronic states and superconducting pairing in kagome superconductors.

cond-mat.supr-con↗

Interweaving Polar Charge Orders in a Layered Metallic Super-atomic Crystal

Electronic properties of super-atomic crystals have not been sufficiently explored due to the versatility of their building units; moreover, their inter-unit couplings are even poorly understood. Here, we present a joint experiment-theory investigation of a rational-designed layered super-atomic crystal of Au6Te12Se8 cubes, stacked by non-covalent inter-cube quasi-bonds. We found a sequential-emerged anisotropic triple-cube charge-density-wave (tc-CDW) and polarized metallic states below 120 K, as revealed via scanning tunneling microscopy/spectroscopy, angle-resolved photoemission spectroscopy, transport measurement, Raman spectra, and density functional theory. The polarized states are locked in an anti-parallel configuration, which is required for maintaining the inversion symmetry of the center-cube in the tc-CDW. The anti-polar metallic states are thus interweaved by the charge-density-wave and the polarized metallic states, and primarily ascribed to electronic effects via theoretical calculations. This work not only demonstrates a microscopic picture of the interweaved CDW and polarized charge orders in the super-atomic crystal of ATS, but also sheds light on expanding the existing category of quantum materials to non-covalent solids.

cond-mat.mtrl-sci↗

Titanium-based kagome superconductor CsTi_3Bi_5 and topological states

Since the discovery of a new family of vanadium-based kagome superconductor AV3Sb5 (A=K, Rb, and Cs) with topological band structures, extensive effort has been devoted to exploring the origin of superconducting states and the intertwined orders. Meanwhile, searching for new types of superconductors with novel physical properties and higher superconducting transition temperatures has always been a major thread in the history of superconductor research. Here we report a successful fabrication and the topological states of a Titanium-based kagome metal CsTi3Bi5 (CT3B5) crystal. The as-grown CT3B5 crystal is of high quality and possesses a perfect two-dimensional kagome net of Titanium. The superconductivity of the CT3B5 crystal shows that the critical temperature Tc is of ~4.8 K. First-principle calculations predict that the CT3B5 has robust topological surface states, implying that CT3B5 is a Z2 topological kagome superconductor. This finding provides a new type of superconductors and the base for exploring the origin of superconductivity and topological states in kagome superconductors.

cond-mat.supr-con↗

One-step exfoliation method for plasmonic activation of large-area 2D crystals

Advanced exfoliation techniques are crucial for exploring the intrinsic properties and applications of 2D materials. Though the recently discovered Au-enhanced exfoliation technique provides an effective strategy for preparation of large-scale 2D crystals, the high cost of gold hinders this method from being widely adopted in industrial applications. In addition, direct Au contact could significantly quench photoluminescence (PL) emission in 2D semiconductors. It is therefore crucial to find alternative metals that can replace gold to achieve efficient exfoliation of 2D materials. Here, we present a one-step Ag-assisted method that can efficiently exfoliate many large-area 2D monolayers, where the yield ratio is comparable to Au-enhanced exfoliation method. Differing from Au film, however, the surface roughness of as-prepared Ag films on SiO2/Si substrate is much higher, which facilitates the generation of surface plasmons resulting from the nanostructures formed on the rough Ag surface. More interestingly, the strong coupling between 2D semiconductor crystals (e.g. MoS2, MoSe2) and Ag film leads to a unique PL enhancement that has not been observed in other mechanical exfoliation techniques, which can be mainly attributed to enhanced light-matter interaction as a result of extended propagation of surface plasmonic polariton (SPP). Our work provides a lower-cost and universal Ag-assisted exfoliation method, while at the same offering enhanced SPP-matter interactions.

cond-mat.mtrl-sci↗

Ordered and tunable Majorana-zero-mode lattice in naturally strained LiFeAs

Majorana zero modes (MZMs) obey non-Abelian statistics and are considered building blocks for constructing topological qubits. Iron-based superconductors with topological band structures have emerged as promising hosting materials, since isolated candidate MZMs in the quantum limit have been observed inside the topological vortex cores. However, these materials suffer from issues related to alloying-induced disorder, uncontrolled vortex lattices and a low yield of topological vortices. Here, we report the formation of an ordered and tunable MZM lattice in naturally-strained stoichiometric LiFeAs by scanning tunneling microscopy/spectroscopy (STM/S). We observe biaxial charge density wave (CDW) stripes along the Fe-Fe and As-As directions in the strained regions. The vortices are pinned on the CDW stripes in the As-As direction and form an ordered lattice. We detect more than 90 percent of the vortices to be topological and possess the characteristics of isolated MZMs at the vortex center, forming an ordered MZM lattice with the density and the geometry tunable by an external magnetic field. Remarkably, with decreasing the spacing of neighboring vortices, the MZMs start to couple with each other. Our findings provide a new pathway towards tunable and ordered MZM lattices as a platform for future topological quantum computation.

cond-mat.supr-con↗

Layer-by-layer growth of bilayer graphene single-crystals enabled by self-transmitting catalytic activity

Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by self-transmitting catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This self-transmitting catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals.

cond-mat.mtrl-sci↗

Atomic-Scale Visualization of Chiral Charge Density Wave States and Their Reversible Transition

Chirality is essential for various amazing phenomena in life and matter. However,chirality and its switching in electronic superlattices, such as charge density wave(CDW) arrays, remain elusive. In this study, we characterize the chirality transition with atom-resolution imaging in a single-layer NbSe2 CDW pattern by technique of scanning tunneling microscopy. The atomic lattice of the CDW array is found continuous and intact although its chirality is switched. Several intermediate states are tracked by time-resolved imaging, revealing the fast and dynamic chirality transition. Importantly, the switching is reversibly realized with an external electric-field. Our findings unveil the delicate transition process of chiral CDW array in a 2D crystal down to the atomic scale and may be applicable for future nanoscale devices.

cond-mat.mtrl-sci↗

Chirality locking charge density waves in a chiral crystal

In Weyl semimetals, charge density wave (CDW) order can spontaneously break the chiral symmetry, gap out the Weyl nodes, and drive the material into the axion insulating phase. Investigations have however been limited since CDWs are rarely seen in Weyl semimetals. Here, using scanning tunneling microscopy/spectroscopy, we report the discovery of a novel unidirectional CDW order on the (001) surface of chiral crystal CoSi - a unique Weyl semimetal with unconventional chiral fermions. The CDW is incommensurate with both lattice momentum and crystalline symmetry directions, and exhibits an intra unit cell π phase shift in the layer stacking direction. The tunneling spectrum shows a particle-hole asymmetric V-shaped energy gap around the Fermi level that modulates spatially with the CDW wave vector. Combined with first-principle calculations, we identify that the CDW is locked to the crystal chirality and is related by a mirror reflection between the two enantiomers of the chiral crystal. Our findings reveal a novel correlated topological quantum state in chiral CoSi crystals and raise the potential for realizing an axion insulator and exploring the unprecedented physical behaviors of unconventional chiral fermions.

cond-mat.mtrl-sci↗

Roton pair density wave and unconventional strong-coupling superconductivity in a topological kagome metal

The transition-metal kagome lattice materials host frustrated, correlated, and topological quantum states of matter. Recently, a new family of vanadium-based kagome metals AV3Sb5 (A=K, Rb, and Cs) with topological band structures has been discovered. These layered compounds are nonmagnetic and undergo charge density wave transitions before developing superconductivity at low temperatures. Here we report the observation of unconventional superconductivity and pair density wave (PDW) in CsV3Sb5 using scanning tunneling microscope/spectroscopy (STM/STS) and Josephson STS. We find that CsV3Sb5 exhibits a V-shaped pairing gap Δ~0.5 meV and is a strong-coupling superconductor (2Δ/kBTc~5) that coexists with 4a0 unidirectional and 2a0X2a0 charge order. Remarkably, we discover a 3Q PDW accompanied by bidirectional 4a0/3 spatial modulations of the superconducting gap, coherence peak and gap-depth in the tunneling conductance. We term this novel quantum state a roton-PDW associated with an underlying vortex-antivortex lattice that can account for the observed conductance modulations. Probing the electronic states in the vortex halo in an applied magnetic field, in strong-field that suppresses superconductivity, and in zero-field above Tc reveals that the PDW is a primary state responsible for an emergent pseudogap and intertwined electronic order. Our findings show striking analogies and distinctions to the phenomenology of high-Tc cuprate superconductors, and provide groundwork for understanding the microscopic origin of correlated electronic states and superconductivity in vanadium-based kagome metals.

cond-mat.supr-con↗

PTCDA molecular monolayer on Pb thin films: An unusual π-electron Kondo system and its interplay with a quantum-confined superconductor

The hybridization of magnetism and superconductivity has been an intriguing playground for correlated electron systems, hosting various novel physical phenomena. Usually, localized d- or f-electrons are central to magnetism. In this study, by placing a PTCDA (3,4,9,10-perylene tetracarboxylic dianhydride) molecular monolayer on ultra-thin Pb films, we built a hybrid magnetism/superconductivity (M/SC) system consisting of only sp electronic levels. The magnetic moments reside in the unpaired molecular orbital originating from interfacial charge-transfers. We reported distinctive tunneling spectroscopic features of such a Kondo screened pi-electron impurity lattice on a superconductor in the regime of TK>>delta suggesting the formation of a two-dimensional bound states band. Moreover, moiré superlattices with tunable twist angle and the quantum confinement in the ultra-thin Pb films provide easy and flexible implementations to tune the interplay between the Kondo physics and the superconductivity, which are rarely present in M/SC hybrid systems.

cond-mat.supr-con↗

Evidence of a hidden flux phase in the topological kagome metal CsV$_3$Sb$_5$

Phase transitions governed by spontaneous time reversal symmetry breaking (TRSB) have long been sought in many quantum systems, including materials with anomalous Hall effect (AHE), cuprate high temperature superconductors, Iridates and so on. However, experimentally identifying such a phase transition is extremely challenging because the transition is hidden from many experimental probes. Here, using zero-field muon spin relaxation (ZF-$μ$SR) technique, we observe strong TRSB signals below 70 K in the newly discovered kagome superconductor CsV$_3$Sb$_5$. The TRSB state emerges from the 2 x 2 charge density wave (CDW) phase present below ~ 95 K. By carrying out optical second-harmonic generation (SHG) experiments, we also find that inversion symmetry is maintained in the temperature range of interest. Combining all the experimental results and symmetry constraints, we conclude that the interlayer coupled chiral flux phase (CFP) is the most promising candidate for the TRSB state among all theoretical proposals of orbital current orders. Thus, this prototypical kagome metal CsV3Sb5 can be a platform to establish a TRSB current-ordered state and explore its relationship with CDW, giant AHE, and superconductivity.

cond-mat.supr-con↗

Intrinsically Honeycomb-patterned Hydrogenated Graphene with Spin Polarized Edge-states

Since the advent of graphene ushered the era of two-dimensional materials, many forms of hydrogenated graphene have been reported, exhibiting diverse properties ranging from a tunable band gap to ferromagnetic ordering. Patterned hydrogenated graphene with micron-scale patterns has been fabricated by lithographic means. Here we report successful millimeter-scale synthesis of an intrinsically honeycomb patterned form of hydrogenated graphene on Ru(0001) by epitaxial growth followed by hydrogenation. Combining scanning tunneling microscopy observations with density-functional-theory (DFT) calculations, we reveal that an atomic-hydrogen layer intercalates between graphene and Ru(0001). The result is a hydrogen honeycomb structure that serves as a template for the final hydrogenation, which converts the graphene into graphane only over the template, yielding honeycomb-patterned hydrogenated graphene (HPHG). In effect, HPHG is a form of patterned graphane. DFT calculations find that the unhydrogenated graphene regions embedded in the patterned graphane exhibit spin-polarized edge states. This type of growth mechanism provides new pathways for the fabrication of intrinsically patterned graphene-based materials.

cond-mat.mtrl-sci↗

Atomically sharp interface enabled ultrahigh-speed, nonvolatile memory devices

Development of memory devices with ultimate performance has played a key role in innovation of modern electronics. As a mainstream technology nonvolatile memory devices have manifested high capacity and mechanical reliability, however current major bottlenecks include low extinction ratio and slow operational speed. Although substantial effort has been employed to improve their performance, a typical hundreds of micro- or even milli- second write time remains a few orders of magnitude longer than their volatile counterparts. We have demonstrated nonvolatile, floating-gate memory devices based on van der Waals heterostructures with atomically sharp interfaces between different functional elements, and achieved ultrahigh-speed programming/erasing operations verging on an ultimate theoretical limit of nanoseconds with extinction ratio up to 10^10. This extraordinary performance has allowed new device capabilities such as multi-bit storage, thus opening up unforeseen applications in the realm of modern nanoelectronics and offering future fabrication guidelines for device scale-up.

physics.app-ph↗

Direct identification of Mott Hubbard band pattern beyond charge density wave superlattice in monolayer 1T-NbSe2

Understanding Mott insulators and charge density waves (CDW) is critical for both fundamental physics and future device applications. However, the relationship between these two phenomena remains unclear, particularly in systems close to two-dimensional (2D) limit. In this study, we utilize scanning tunneling microscopy/spectroscopy to investigate monolayer 1T-NbSe2 to elucidate the energy of the Mott upper Hubbard band (UHB), and reveal that the spin-polarized UHB is spatially distributed away from the dz2 orbital at the center of the CDW unit. Moreover, the UHB shows a root3 x root3 R30° periodicity in addition to the typically observed CDW pattern. Furthermore, a pattern similar to the CDW order is visible deep in the Mott gap, exhibiting CDW without contribution of the Mott Hubbard band. Based on these findings in monolayer 1T-NbSe2, we provide novel insights into the relation between the correlated and collective electronic structures in monolayer 2D systems.

cond-mat.str-el↗