arXiv subjects

Ying-Shuang Fu

Publications and source records attributed to Ying-Shuang Fu.

At least 19 recordsLinked to original sources

arXiv2026

Imaging Intermediate Melting Phases of Dual Magnetic-Field-Stabilized Wigner Crystals

The competition between Coulomb repulsion and kinetic energy in correlated systems can allow electrons to crystallize into Wigner solids. Despite researches across diverse two-dimensional Wigner platforms, the microscopic melting processes through possible intermediate phases remains largely unknown. Here, we present the visualization of electron-lattice melting in monolayer VCl3 on graphite, where two Wigner crystals coexist with markedly different critical temperatures Tc and lattice periods as stabilized by high magnetic field. One Wigner crystal possesses both record-high Tc and electron density, and undergoes melting through an intermediate nematic phase upon decreasing magnetic field. In contrast, the other Wigner crystal with a lower Tc yields a different intermediate phase during melting, exhibiting an anomalous electron liquid with an energy-independent modulation period. First-principles calculations corroborate the band-selective occupations of interface-transferred electrons in the formation of dual Wigner crystals. Our atomically resolved intermediate phases provide crucial insights into the microscopic melting pathways of Wigner crystals, enabling a phase diagram parameterized by both quantum and thermal fluctuations.

cond-mat.str-el↗

arXiv2026

Spectral Visualization of Excitonic Pair Breaking at Individual Impurities in Ta2Pd3Te5

Excitonic insulators host the condensates of bound electron-hole pairs, offering a platform for studying correlated bosonic quantum states. Yet, how macroscopic coherence emerges from locally collapsed pairing remains elusive. Here, using scanning tunnelling spectroscopy, we report the impurity-induced pair breaking in an excitonic insulator Ta2Pd3Te5. Individual Te vacancies are found to generate a pair of spectral peaks within the excitonic gap. Their energies depend sensitively on the defect configurations and are continuously tunable by tip electric field, indicating controllable impurity scatterings. Spectral mapping shows spatially anisotropic and electronically coupled electron-hole components of the subgap states. These observations, together with mean-field modelling, suggest an excitonic pair-breaking origin. In the strongly electron-hole imbalanced region, a secondary pair-breaking effect, manifesting as an additional pair of subgap states with distinctly lower energies, can emerge, presenting the interplay of pairing breakings with different excitonic order parameters. Our findings demonstrate the spectroscopic 'fingerprint' of local excitonic depairing at the atomic level, offering a crucial clue to the critical behavior across excitonic condensation.

cond-mat.str-el↗

arXiv2025

Self-stabilized charge states in a double-decker molecular magnet on Pb(111)

Electron charging play key roles in physiochemical processes, whose intrinsic stabilization in single molecules is desirable for tailoring molecular functionality and developing molecular devices, but remains elusive on surfaces. Here, we show molecular charge states can be self-stabilized via intramolecular distortion in single bis(phthalocyaninato)terbium(III) (TbPc2) double-decker molecules, that were grown on Pb(111) substrate. Using scanning tunneling microscopy and spectroscopy, we identify fractions of TbPc2 molecules reduce to 2-fold symmetry, expressing energy-split molecular orbitals and two types of different spin states. Our first principles calculations unveil that the symmetry reduction is induced by charging-triggered Jahn-Teller distortions, which lifts the degenerate orbitals into two 2-fold symmetric orbitals. Single or double occupancy of the lower-energy orbital results in different molecular spin states. Such intramolecular distortion traps the excess electrons stably without explicit involvement of the substrate, in contrast to previously observed molecular charge states. These charged single molecule can be manipulated with the tip individually. This study offers a new avenue for tailoring the charge and spin states of molecules.

cond-mat.mes-hall↗

arXiv2025

Visualization of intervalley coherent phase in PtSe2/HOPG heterojunction

Intervalley coherent (IVC) phase in graphene systems arises from the coherent superposition of wave functions of opposite valleys, whose direct microscopic visualization provides pivotal insight into the emergent physics but remains elusive. Here, we successfully visualize the IVC phase in a heterostructure of monolayer PtSe2 on highly oriented pyrolytic graphite. Using spectroscopic imaging scanning tunneling microscopy, we observe a Root3 by Root3 modulation pattern superimposed on the higher-order moire superlattice of the heterostructure, which correlates with a small gap opening around the Fermi level and displays an anti-phase real-space conductance distribution of the two gap edges. Such modulation pattern and small-gap vanish on the heterostructure of monolayer PtSe2 on bilayer-graphene-covered SiC substrate, due to the increased carrier density in the bilayer graphene. We provide a theoretical mechanism that the Root3 by Root3 modulation pattern originates from the IVC phase of few-layer graphene, which is magnified by the higher-order moire superlattice. Our work achieves visualization of the IVC phase, and develops an avenue for its generation and amplification via a moir\'e interface.

cond-mat.mes-hall↗

arXiv2024

Regulated magnetic anisotropy and charge density wave in uniformly fabricated Janus CrTeSe monolayer

Two-dimensional materials with Janus structure host novel physical properties due to their inversional symmetry breaking. However, it remains elusive to synthesize Janus monolayer crystals with tailored long-range magnetic orders. Here, we have developed a general method to fabricate uniform Janus CrTeSe monolayers by selective selenization of preformed CrTe2 monolayers with molecular beam epitaxy. The uniform Janus structure of CrTeSe with high crystal quality is confirmed by high-resolution scanning transmission electron microscopy. Spin-polarized scanning tunneling microscopy/spectroscopy measurements unveil that the Janus CrTeSe undergoes a charge density wave (CDW) transition and a robust antiferromagnetic order. The magnetic anisotropy of CrTeSe is drastically altered compared to monolayer CrTe2 by the breaking symmetries induced from the Janus structure and the CDW transition, as is substantiated with first principles calculations. Our research achieves the construction of large-area Janus structures, and artificially tailors the electronic and magnetic properties of Janus systems at the two-dimensional limit.

cond-mat.mtrl-sci↗

arXiv2024

High-Resolution Spectroscopy of the Intermediate Impurity States near a Quantum Phase Transition

The intermediate behavior near a quantum phase transition is crucial for understanding the quantum criticality of various competing phases and their separate origins, yet remains unexplored for the multiple Yu-Shiba-Rusinov (YSR) states. Here, we investigated the detailed spectroscopic change of the exchange coupling-dependent YSR states near a quantum phase transition. The initially developed one pair of YSR states, induced by the Fe vacancy in monolayer Fe(Te,Se) superconductor, are clearly resolved with high resolution showing an evolution into two pairs of YSR peaks yet with dichotomy in their spectral features. Interestingly, while the lower-energy YSR branch enters the quantum phase transition region, the higher-lying one remains rigidly away from the lower-energy counterpart with a constant energy difference. Spectral weight analysis of the higher-energy branch yields an exponential dependence on the exchange coupling, which can be well rationalized by taking the two pairs of YSR states as a result of field splitting by the magnetic anisotropy. Our results unveil the intermediate region of a quantum phase transition with a magnetic anisotropy-induced splitting of the YSR resonance, and highlight a prospect for developing functional electronics based on the flexibly controllable multiple quantum states.

cond-mat.supr-con↗

arXiv2024

Visualizing uniform lattice-scale pair density wave in single-layer FeSe/SrTiO3 films

Typical BCS superconductors are microscopically homogeneous in real space governed by the coherent Cooper pairs with high phase stiffness of superfluid density, which is characterized by a coherence length. However, a periodic oscillation of superconducting order parameter may develop driven by breaking the time-reversal or translational invariance. To date, such modulated orders were specific to each material systems, with a periodicity much larger than the lattice constant. Here we report the direct observation of a uniform lattice-scale pair density wave (PDW) in single-layer FeSe/SrTiO3 films, enforced by peculiar interfacial structure of crystal symmetries breaking. Our spectroscopic imaging scanning tunneling microscopy unravels a spatial modulation of Cooper-pairing gap within a single unit-cell, depending on inequivalent atomic sites. Prominent periodic variation of superfluid density is visualized via Josephson current by a superconducting tip, indicating a real-space oscillation of phase stiffness. Such a lattice-scale superconducting modulation, which coexists with a larger length scale of PDW order, indicates the lattice-scale variation of both pairing strength and phase stiffness. Our findings provide new insights into the intertwined density-wave orders of quasiparticle character in correlated electronic systems, and provoke future studies on the unconventional pairing interaction and phase stiffness in the two-dimensional limit.

cond-mat.supr-con↗

arXiv2023

Spin-resolved imaging of atomic-scale helimagnetism in monolayer NiI2

Identifying intrinsic noncollinear magnetic order in monolayer van der Waals (vdW) crystals is highly desirable for understanding the delicate magnetic interactions at reduced spatial constraints and miniaturized spintronic applications, but remains elusive in experiments. Here, we achieved spin-resolved imaging of helimagnetism at atomic scale in monolayer NiI2 crystals, that were grown on graphene-covered SiC(0001) substrate, using spin-polarized scanning tunneling microscopy. Our experiments identify the existence of a spin spiral state with canted plane in monolayer NiI2. The spin modulation Q vector of the spin spiral is determined as (0.2203, 0, 0), which is different from its bulk value or its in-plane projection, but agrees well with our first principles calculations. The spin spiral surprisingly indicates collective spin switching behavior under magnetic field, whose origin is ascribed to the incommensurability between the spin spiral and the crystal lattice. Our work unambiguously identifies the helimagnetic state in monolayer NiI2, paving the way for illuminating its expected type-II multiferroic order and developing spintronic devices based on vdW magnets.

cond-mat.mes-hall↗

arXiv2023

Small polarom formation by electron-electron interaction

In a solid, electrons can be scattered both by phonons and other electrons. First proposed by Landau, scattering by phonons can lead to a composite entity called a polaron, in which a lattice distortion traps an itinerant electron (or hole) such that the distortion and carrier move in unison as a single particle with larger effective mass. While this is the traditional view of polarons, the rise of 2D systems, especially strongly correlated ones, open the prospect of electron scattering taking on a larger role in spontaneous carrier localization for such material systems. Here, we show that in transition metal halides, such electron-electron interactions can lead to polaron formation even in the absence of lattice distortion. This suggests an alternative direction for polaron formation, transport, and control in solids. This new mechanism of polaron formation is confirmed by first-principles calculation of 2D transition metal halides, CrI2, CoCl2 and CoBr2. These theoretical predictions are supported by scanning tunneling microscopy/spectroscopy measurements of polarons in CrI2.

cond-mat.mtrl-sci↗

arXiv2022

Manipulating single excess electrons in monolayer transition metal dihalide

Polarons are entities of excess electrons dressed with local response of lattices, whose atomic-scale characterization is essential for understanding the many body physics arising from the electron-lattice entanglement, but yet difficult to achieve. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we show the visualization and manipulation of single polarons with different origin, i.e., electronic and conventional polarons, in monolayer CoCl2, that are grown on HOPG substrate via molecular beam epitaxy. Four types of polarons are identified, all inducing upward local band bending, but exhibiting distinct appearances, lattice occupations, polaronic states and local lattice distortions. First principles calculations unveil three types of polarons are stabilized by electron-electron interaction. The type-4 polaron, however, are driven by conventional lattice distortions. All the four types of polarons can be created, moved, erased, and moreover interconverted individually by the STM tip, allowing precise control of single polarons unprecedently. This finding identifies the rich category of polarons and their feasibility of manipulation in CoCl2, which can be generalized to other transition metal halides.

cond-mat.mes-hall↗

arXiv2021

Spin mapping of intralayer antiferromagnetism and spin-flop transition in monolayer CrTe$_2$

Intrinsic antiferromagnetism in van der Waals (vdW) monolayer (ML) crystals enriches the understanding regarding two-dimensional (2D) magnetic orders and holds special virtues over ferromagnetism in spintronic applications. However, the studies on intrinsic antiferromagnetism are sparse, owing to the lack of net magnetisation. In this study, by combining spin-polarised scanning tunnelling microscopy and first-principles calculations, we investigate the magnetism of vdW ML CrTe2, which has been successfully grown through molecular beam epitaxy. Surprisingly, we observe a stable antiferromagnetic (AFM) order at the atomic scale in the ML crystal, whose bulk is a strong ferromagnet, and correlate its imaged zigzag spin texture with the atomic lattice structure. The AFM order exhibits an intriguing noncollinear spin-flop transition under magnetic fields, consistent with its calculated moderate magnetic anisotropy. The findings of this study demonstrate the intricacy of 2D vdW magnetic materials and pave the way for their in-depth studies.

cond-mat.mtrl-sci↗

arXiv2021

Manipulating Hubbard-type Coulomb blockade effect of metallic wires embedded in an insulator

Correlated states emerge in low-dimensional systems owing to enhanced Coulomb interactions. Elucidating these states requires atomic scale characterization and delicate control capabilities. In this study, spectroscopic imaging-scanning tunneling microscopy was employed to investigate the correlated states residing in the one-dimensional electrons of the monolayer and bilayer MoSe2 mirror twin boundary (MTB). The Coulomb energies, determined by the wire length, drive the MTB into two types of ground states with distinct respective out-of-phase and in-phase charge orders. The two ground states can be reversibly converted through a metastable zero-energy state with in situ voltage pulses, which tunes the electron filling of the MTB via a polaronic process, as substantiated by first-principles calculations. Our modified Hubbard model reveals the ground states as correlated insulators from an on-site U-originated Coulomb interaction, dubbed Hubbard-type Coulomb blockade effect. Our work sets a foundation for understanding correlated physics in complex systems and for tailoring quantum states for nano-electronics applications.

cond-mat.mes-hall↗

arXiv2021

Mott insulator tuning via structural distortion in monolayer 1T-NbSe2

Mott state in 1T-TaS2 is predicted to host quantum spin liquids (QSL). However, its insulating mechanism is controversial due to complications from interlayer coupling. Here, we study the Mott state in monolayer 1T-NbSe2, an electronic analogy to TaS2 exempt from interlayer coupling, using spectroscopic imaging scanning tunneling microscopy and first principles calculations. Monolayer NbSe2 surprisingly displays two types of Star-of-David (SD) motifs with different Mott gap sizes, that are interconvertible via temperature variation. And, bilayer 1T-NbSe2 shows Mott collapse by interlayer coupling. Our calculation unveils the two types of SDs possess distinct structural distortions, altering the effective Coulomb energies of the central Nb orbital. Our calculation suggests the Mott gap, the same parameter for determining the QSL regime, is tunable with strain. This finding offers a general strategy for manipulating the Mott state in 1T-NbSe2 and related systems via structural distortions, which may be tuned into the potential QSL regime.

cond-mat.mes-hall↗

arXiv2021

Realization of AlSb in the double layer honeycomb structure: a robust new class of two-dimensional material

Exploring new two-dimensional (2D) van der Waals (vdW) systems is at the forefront of materials physics. Here, through molecular beam epitaxy on graphene-covered SiC(0001), we report successful growth of AlSb in the double-layer honeycomb (DLHC) structure, a 2D vdW material which has no direct analogue to its 3D bulk and is predicted kinetically stable when freestanding. The structural morphology and electronic structure of the experimental 2D AlSb are characterized with spectroscopic imaging scanning tunneling microscopy and cross-sectional imaging scanning transmission electron microscopy, which compare well to the proposed DLHC structure. The 2D AlSb exhibits a bandgap of 0.93 eV versus the predicted 1.06 eV, which is substantially smaller than the 1.6 eV of bulk. We also attempt the less-stable InSb DLHC structure; however, it grows into bulk islands instead. The successful growth of a DLHC material here opens the door for the realization of a large family of novel 2D DLHC traditional semiconductors with unique excitonic, topological, and electronic properties.

cond-mat.mtrl-sci↗

arXiv2020

Possible phason-polaron effect on purely one dimensional charge order of Mo6Se6 nanowires

In one-dimensional (1D) metallic systems, the diverging electron susceptibility and electron-phonon coupling collaboratively drive the electrons into a charge density wave (CDW) state. However, strictly 1D system is unstable against perturbations, whose effect on CDW order requires clarification ideally with altered coupling to surroundings. Here, we fabricate such a system with nanowires of Mo6Se6 bundles, which are either attached to edges of monolayer MoSe2 or isolated freely, by post-annealing the preformed MoSe2. Using scanning tunneling microscopy (STM), we visualized charge modulations and CDW gaps with prominent coherent peaks in the edge-attached nanowires. Astonishingly, the CDW order becomes suppressed in the isolated nanowires, showing CDW correlation gaps without coherent peaks. The contrasting behavior, as revealed with theoretical modeling, is interpreted as the effect of phason-polarons on the 1D CDW state. Our work elucidates a possibly unprecedented many body effect that may be generic to strictly 1D system but undermined in quasi-1D system.

cond-mat.mes-hall↗

arXiv2019

Mott phase in a van der Waals transition-metal halide at single layer limit

Two-dimensional materials offer opportunities for unravelling unprecedented ordered states at single layer limit. Among such ordered states, Mott phase is rarely explored. Here, we report the Mott phase in van der Waals chromium (II) iodide (CrI2) films. High quality CrI2 films with atomically flat surface and macro size are grown on graphitized 6H-SiC(0001) substrate by molecular beam epitaxy. By in situ low temperature scanning tunneling microscopy and spectroscopy (STM/STS), we reveal that the film has a band gap as large as ~3.2 eV, which is nearly thickness independent. Density functional plus dynamic mean field theory calculations suggest that CrI2 films may be a strong Mott insulator with a ferromagnetically ordered ground state. The Mott phase is corroborated by the spectral band splitting, that is consistent with the extended Hubbard model, and gap reduction at charge dopants. Our study provides a platform for studying correlated electron states at single layer limit.

cond-mat.mes-hall↗

arXiv2019

Dimensional Crossover and Topological Phase Transition in Dirac Semimetal Na3Bi Films

Three-dimensional (3D) topological Dirac semimetal, when thinned down to 2D few layers, is expected to possess gapped Dirac nodes via quantum confinement effect and concomitantly display the intriguing quantum spin Hall (QSH) insulator phase. However, the 3D-to-2D crossover and the associated topological phase transition, which is valuable for understanding the topological quantum phases, remain unexplored. Here, we synthesize high-quality Na3Bi thin films with R3*R3 reconstruction on graphene, and systematically characterize their thickness-dependent electronic and topological properties by scanning tunneling microscopy/spectroscopy in combination with first-principles calculations. We demonstrate that Dirac gaps emerge in Na3Bi films, providing spectroscopic evidences of dimensional crossover from a 3D semimetal to a 2D topological insulator. Importantly, the Dirac gaps are revealed to be of sizable magnitudes on 3 and 4 monolayers (72 and 65 meV, respectively) with topologically nontrivial edge states. Moreover, the Fermi energy of a Na3Bi film can be tuned via certain growth process, thus offering a viable way for achieving charge neutrality in transport. The feasibility of controlling Dirac gap opening and charge neutrality enables realizing intrinsic high-temperature QSH effect in Na3Bi films and achieving potential applications in topological devices.

cond-mat.mtrl-sci↗

arXiv2018

Visualizing topological edge states of single and double bilayer Bi supported on multibilayer Bi(111) films

Freestanding single-bilayer Bi(111) is a two-dimensional topological insulator with edge states propagating along its perimeter. Given the interlayer coupling experimentally, the topological nature of Bi(111) thin films and the impact of the supporting substrate on the topmost Bi bilayer are still under debate. Here, combined with scanning tunneling microscopy and first-principles calculations, we systematically study the electronic properties of Bi(111) thin films grown on a NbSe2 substrate. Two types of non-magnetic edge structures, i.e., a conventional zigzag edge and a 2x1 reconstructed edge, coexist alternately at the boundaries of single bilayer islands, the topological edge states of which exhibit remarkably different energy and spatial distributions. Prominent edge states are persistently visualized at the edges of both single and double bilayer Bi islands, regardless of the underlying thickness of Bi(111) thin films. We provide an explanation for the topological origin of the observed edge states that is verified with first-principles calculations. Our paper clarifies the long-standing controversy regarding the topology of Bi(111) thin films and reveals the tunability of topological edge states via edge modifications.

cond-mat.mtrl-sci↗