arXiv subjects

Tiancong Zhu

Publications and source records attributed to Tiancong Zhu.

At least 19 recordsLinked to original sources

arXiv2025

Roadmap: 2D Materials for Quantum Technologies

Two-dimensional (2D) materials have emerged as a versatile and powerful platform for quantum technologies, offering atomic-scale control, strong quantum confinement, and seamless integration into heterogeneous device architectures. Their reduced dimensionality enables unique quantum phenomena, including optically addressable spin defects, tunable single-photon emitters, low-dimensional magnetism, gate-controlled superconductivity, and correlated states in Moiré superlattices. This Roadmap provides a comprehensive overview of recent progress and future directions in exploiting 2D materials for quantum sensing, computation, communication, and simulation. We survey advances spanning spin defects and quantum sensing, quantum emitters and nonlinear photonics, computational theory and data-driven discovery of quantum defects, spintronic and magnonic devices, cavity-engineered quantum materials, superconducting and hybrid quantum circuits, quantum dots, Moiré quantum simulators, and quantum communication platforms. Across these themes, we identify common challenges in defect control, coherence preservation, interfacial engineering, and scalable integration, alongside emerging opportunities driven by machine$-$learning$-$assisted design and integrated experiment$-$theory feedback loops. By connecting microscopic quantum states to mesoscopic excitations and macroscopic device architectures, this Roadmap outlines a materials-centric framework for integrating coherent quantum functionalities and positions 2D materials as foundational building blocks for next-generation quantum technologies.

quant-ph↗

arXiv2024

Antiferromagnetic order in a layered magnetic topological insulator MnBi$_2$Se$_4$ probed by resonant soft x-ray scattering

The quasi-two-dimensional magnetic topological insulator MnBi$_2$Se$_4$, stabilized via non-equilibrium molecular beam epitaxy, is investigated by resonant soft x-ray scattering. Kiessig fringes are observed, confirming a high sample quality and a thin film thickness of 10 septuple layers ($\sim$13 nm). An antiferromagnetic Bragg peak is observed at the structurally forbidden reflection, whose magnetic nature is validated by studying its temperature, energy, and polarization dependence. Through a detailed analysis, an A-type antiferromagetic order with in-plane moments is implied. This alternative spin structure in MnBi$_2$Se$_4$, in contrast to the Ising antiferromagnetic states in other magnetic topological insulators, might be relevant for hosting new topological states.

cond-mat.str-el↗

arXiv2023

Visualizing and manipulating chiral interface states in a moiré quantum anomalous Hall insulator

Moiré systems made from stacked two-dimensional materials host novel correlated and topological states that can be electrically controlled via applied gate voltages. We have used this technique to manipulate Chern domains in an interaction-driven quantum anomalous Hall insulator made from twisted monolayer-bilayer graphene (tMBLG). This has allowed the wavefunction of chiral interface states to be directly imaged using a scanning tunneling microscope (STM). To accomplish this tMBLG carrier concentration was tuned to stabilize neighboring domains of opposite Chern number, thus providing topological interfaces completely devoid of any structural boundaries. STM tip pulse-induced quantum dots were utilized to induce new Chern domains and thereby create new chiral interface states with tunable chirality at predetermined locations. Theoretical analysis confirms the chiral nature of observed interface states and enables the determination of the characteristic length scale of valley polarization reversal across neighboring tMBLG Chern domains. tMBLG is shown to be a useful platform for imaging the exotic topological properties of correlated moiré systems.

cond-mat.mes-hall↗

arXiv2023

Local spectroscopy of a gate-switchable moiré quantum anomalous Hall insulator

In recent years, correlated insulating states, unconventional superconductivity, and topologically non-trivial phases have all been observed in several moiré heterostructures. However, understanding of the physical mechanisms behind these phenomena is hampered by the lack of local electronic structure data. Here, we use scanning tunnelling microscopy and spectroscopy to demonstrate how the interplay between correlation, topology, and local atomic structure determines the behaviour of electron-doped twisted monolayer-bilayer graphene. Through gate- and magnetic field-dependent measurements, we observe local spectroscopic signatures indicating a quantum anomalous Hall insulating state with a total Chern number of $\pm 2$ at a doping level of three electrons per moiré unit cell. We show that the sign of the Chern number and associated magnetism can be electrostatically switched only over a limited range of twist angle and sample hetero-strain values. This results from a competition between the orbital magnetization of filled bulk bands and chiral edge states, which is sensitive to strain-induced distortions in the moiré superlattice.

cond-mat.mes-hall↗

arXiv2022

A novel $\sqrt{19}\times\sqrt{19}$ superstructure in epitaxially grown 1T-TaTe$_2$

The spontaneous formation of electronic orders is a crucial element for understanding complex quantum states and engineering heterostructures in two-dimensional materials. We report a novel $\sqrt{19}\times\sqrt{19}$ charge order in few-layer thick 1T-TaTe$_2$ transition metal dichalcogenide films grown by molecular beam epitaxy, which has not been realized. Our photoemission and scanning probe measurements demonstrate that monolayer 1T-TaTe$_2$ exhibits a variety of metastable charge density wave orders, including the $\sqrt{19}\times\sqrt{19}$ superstructure, which can be selectively stabilized by controlling the post-growth annealing temperature. Moreover, we find that only the $\sqrt{19}\times\sqrt{19}$ order persists in 1T-TaTe$_2$ films thicker than a monolayer, up to 8 layers. Our findings identify the previously unrealized novel electronic order in a much-studied transition metal dichalcogenide and provide a viable route to control it within the epitaxial growth process.

cond-mat.mtrl-sci↗

arXiv2022

Large-gap insulating dimer ground state in monolayer IrTe2

Monolayers of two-dimensional van der Waals materials exhibit novel electronic phases distinct from their bulk due to the symmetry breaking and reduced screening in the absence of the interlayer coupling. In this work, we combine angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy to demonstrate the emergence of a unique insulating 2 x 1 dimer ground state in monolayer 1T-IrTe2 that has a large band gap in contrast to the metallic bilayer-to-bulk forms of this material. First-principles calculations reveal that phonon and charge instabilities as well as local bond formation collectively enhance and stabilize a charge-ordered ground state. Our findings provide important insights into the subtle balance of interactions having similar energy scales that occurs in the absence of strong interlayer coupling, which offers new opportunities to engineer the properties of 2D monolayers.

cond-mat.mtrl-sci↗

arXiv2022

Evidence for a spinon Kondo effect in cobalt atoms on single-layer 1T-TaSe$_2$

Quantum spin liquids (QSLs) are highly entangled, disordered magnetic states that arise in frustrated Mott insulators and host exotic fractional excitations such as spinons and chargons. Despite being charge insulators some QSLs are predicted to exhibit gapless itinerant spinons that yield metallic behavior in the spin channel. We have deposited isolated magnetic atoms onto single-layer (SL) 1T-TaSe$_2$, a gapless QSL candidate, to experimentally probe how itinerant spinons couple to impurity spin centers. Using scanning tunneling spectroscopy we observe the emergence of new, impurity-induced resonance peaks at the 1T-TaSe$_2$ Hubbard band edges when cobalt adatoms are positioned to have maximal spatial overlap with the Hubbard band charge distribution. These resonance peaks disappear when the spatial overlap is reduced or when the magnetic impurities are replaced with non-magnetic impurities. Theoretical simulations using a modified Anderson impurity model integrated with a gapless quantum spin liquid show that these resonance peaks are consistent with a Kondo resonance induced by spinons combined with spinon-chargon binding effects that arise due to QSL gauge-field fluctuations.

cond-mat.str-el↗

arXiv2021

Imaging gate-tunable Tomonaga-Luttinger liquids in 1H-MoSe$_2$ mirror twin boundaries

One-dimensional electron systems (1DESs) exhibit properties that are fundamentally different from higher-dimensional systems. For example, electron-electron interactions in 1DESs have been predicted to induce Tomonaga-Luttinger liquid behavior. Naturally-occurring grain boundaries in single-layer semiconducting transition metal dichalcogenides provide 1D conducting channels that have been proposed to host Tomonaga-Luttinger liquids, but charge density wave physics has also been suggested to explain their behavior. Clear identification of the electronic ground state of this system has been hampered by an inability to electrostatically gate such boundaries and thereby tune their charge carrier concentration. Here we present a scanning tunneling microscopy/spectroscopy study of gate-tunable mirror twin boundaries (MTBs) in single-layer 1H-MoSe$_2$ devices. Gating here enables STM spectroscopy to be performed for different MTB electron densities, thus allowing precise characterization of electron-electron interaction effects. Visualization of MTB electronic structure under these conditions allows unambiguous identification of collective density wave excitations having two distinct velocities, in quantitative agreement with the spin-charge separation predicted by finite-length Tomonaga-Luttinger-liquid theory.

cond-mat.str-el↗

arXiv2021

Visualizing delocalized correlated electronic states in twisted double bilayer graphene

The discovery of interaction-driven insulating and superconducting phases in moiré van der Waals heterostructures has sparked considerable interest in understanding the novel correlated physics of these systems. While a significant number of studies have focused on twisted bilayer graphene, correlated insulating states and a superconductivity-like transition up to 12 K have been reported in recent transport measurements of twisted double bilayer graphene. Here we present a scanning tunneling microscopy and spectroscopy study of gate-tunable twisted double bilayer graphene devices. We observe splitting of the van Hove singularity peak by ~20 meV at half-filling of the conduction flat band, with a corresponding reduction of the local density of states at the Fermi level. By mapping the tunneling differential conductance we show that this correlated system exhibits energetically split states that are spatially delocalized throughout the different regions in the moiré unit cell, inconsistent with order originating solely from onsite Coulomb repulsion within strongly-localized orbitals. We have performed self-consistent Hartree-Fock calculations that suggest exchange-driven spontaneous symmetry breaking in the degenerate conduction flat band is the origin of the observed correlated state. Our results provide new insight into the nature of electron-electron interactions in twisted double bilayer graphene and related moiré systems.

cond-mat.str-el↗

arXiv2020

Atomic scale visualization of topological spin textures in the chiral magnet MnGe

Spin polarized scanning tunneling microscopy is used to directly image topological magnetic textures in thin films of MnGe, and to correlate the magnetism with structure probed at the atomic-scale. Our images indicate helical stripe domains, each characterized by a single wavevector Q, and their associated helimagnetic domain walls, in contrast to the 3Q magnetic state seen in the bulk. Combining our surface measurements with micromagnetic modeling, we deduce the three-dimensional orientation of the helical wavevectors and gain detailed understanding of the structure of individual domain walls and their intersections. We find that three helical domains meet in two distinct ways to produce either a "target-like" or a "pi-like" topological spin texture, and correlate these with local strain on the surface. We further show that the target-like texture can be reversibly manipulated through either current/voltage pulsing or applied magnetic field, a promising step toward future applications.

cond-mat.mes-hall↗

arXiv2020

Chemical Migration and Dipole Formation at van der Waals Interfaces between Magnetic Transition Metal Chalcogenides and Topological Insulators

Metal and magnetic overlayers alter the surface of the topological insulator (TI) bismuth selenide (Bi$_2$Se$_3$) through proximity effects but also by changing the composition and chemical structure of the Bi$_2$Se$_3$ sub-surface. The interface between Bi$_2$Se$_3$ and Mn metal or manganese selenide was explored using x-ray photoelectron spectroscopy (XPS) revealing chemical and electronic changes at the interface. Depositing Mn metal on Bi$_2$Se$_3$ without an external source of Se shows unexpected bonding within the Mn layer due to Mn-Se bonding as Se diffuses out of the Bi$_2$Se$_3$ layer into the growing Mn film. The Se out-diffusion is further evidenced by changes in Bi core levels within the Bi$_2$Se$_3$ layers indicating primarily Bi-Bi bonding over Bi-Se bonding. No out-diffusion of Se occurred when excess Se is supplied with Mn, indicating the importance of supplying enough chalcogen atoms with deposited metals. However, Bi$_2$Se$_3$ core level photoelectrons exhibited a rigid chemical shift toward higher binding energy after depositing a monolayer of MnSe$_{2-x}$, indicating a dipole within the overlayer. Stoichiometry calculations indicated that the monolayer forms MnSe preferentially over the transition metal dichalcogenide (TMD) phase MnSe$_2$, providing a consistent picture of the dipole formation in which a plane of Se anions sits above Mn cations. This study shows that chemical diffusion and dipole formation are important for Mn-Bi$_2$Se$_3$ and MnSe$_{2-x}$-Bi$_2$Se$_3$ and should be considered carefully for TMD/TI interfaces more generally.

cond-mat.mtrl-sci↗

arXiv2020

Coherent Growth and Characterization of van der Waals 1T-VSe$_2$ Layers on GaAs(111)B Using Molecular Beam Epitaxy

We report epitaxial growth of vanadium diselenide (VSe$_2$) thin films in the octahedrally-coordinated (1T) structure on GaAs(111)B substrates by molecular beam epitaxy. Film thickness from a single monolayer (ML) up to 30 ML is demonstrated. Structural and chemical studies using by x-ray diffraction, transmission electron microscopy, scanning tunneling microscopy and x-ray photoelectron spectroscopy indicate high quality thin films. Further studies show that monolayer VSe$_2$ films on GaAs are not air-stable and are susceptible to oxidation within a matter of hours, which indicates that a protective capping layer should be employed for device applications. This work demonstrates that VSe$_2$, a candidate van der Waals material for possible spintronic and electronic applications, can be integrated with III-V semiconductors via epitaxial growth for 2D/3D hybrid devices.

cond-mat.mtrl-sci↗

arXiv2020

Magnetic Properties and Electronic Structure of Magnetic Topological Insulator MnBi$_2$Se$_4$

The intrinsic magnetic topological insulators MnBi$_2$X$_4$ (X = Se, Te) are promising candidates in realizing various novel topological states related to symmetry breaking by magnetic order. Although much progress had been made in MnBi$_2$Te$_4$, the study of MnBi$_2$Se$_4$ has been lacking due to the difficulty of material synthesis of the desired trigonal phase. Here, we report the synthesis of multilayer trigonal MnBi$_2$Se$_4$ with alternating-layer molecular beam epitaxy. Atomic-resolution scanning transmission electron microscopy (STEM) and scanning tunneling microscopy (STM) identify a well-ordered multilayer van der Waals (vdW) crystal with septuple-layer base units in agreement with the trigonal structure. Systematic thickness-dependent magnetometry studies illustrate the layered antiferromagnetic ordering as predicted by theory. Angle-resolved photoemission spectroscopy (ARPES) reveals the gapless Dirac-like surface state of MnBi$_2$Se$_4$, which demonstrates that MnBi$_2$Se$_4$ is a topological insulator above the magnetic ordering temperature. These systematic studies show that MnBi$_2$Se$_4$ is a promising candidate for exploring the rich topological phases of layered antiferromagnetic topological insulators.

cond-mat.mtrl-sci↗

arXiv2018

Transport Spectroscopy of Sublattice-Resolved Resonant Scattering in Hydrogen-Doped Bilayer Graphene

We report the experimental observation of sublattice-resolved resonant scattering in bilayer graphene by performing simultaneous cryogenic atomic hydrogen doping and electron transport measurements in ultrahigh vacuum. This allows us to monitor the hydrogen adsorption on the different sublattices of bilayer graphene without atomic-scale microscopy. Specifically, we detect two distinct resonant scattering peaks in the gate-dependent resistance, which evolve as a function of atomic hydrogen dosage. Theoretical calculations show that one of the peaks originates from resonant scattering by hydrogen adatoms on the α-sublattice (dimer site) while the other originates from hydrogen adatoms on the \b{eta}-sublattice (non-dimer site), thereby enabling a method for characterizing the relative sublattice occupancy via transport measurements. Utilizing this new capability, we investigate the adsorption and thermal desorption of hydrogen adatoms via controlled annealing and conclude that hydrogen adsorption on the \b{eta}-sublattice is energetically favored. Through site-selective desorption from the α-sublattice, we realize hydrogen doping with adatoms primarily on a single sublattice, which is highly desired for generating ferromagnetism.

cond-mat.mes-hall↗

arXiv2018

Importance of Paramagnetic Background Subtraction for Determining the Magnetic Moment in Epitaxially Grown Monolayer and Few-Layer van der Waals Magnets

Due to the atomically thin nature of monolayer and few-layer van der Waals magnets, the undesired background signal from the substrate can have significant contribution when characterizing their magnetic properties. This brings challenges in accurately determining the magnitude of the magnetic moment of the epitaxially grown van der Waals magnets on bulk substrates. In this paper, we discuss the impact of the background subtraction method for accurately determining the magnetic moments in such systems. Using the recently reported intrinsic two-dimensional (2D) van der Waals ferromagnet MnSe${_2}$ as an example, we show that a normal diamagnetic background subtraction method in analyzing the bulk magnetometry measurement will result in an unexpectedly large magnetic moment (greater than ~10 μ${_B}$ per formula unit). Through our systematic growth study, we identify an additional paramagnetic signal due to unintentional Mn doping of the substrate. To extract the correct magnetic moment, a paramagnetic background should also be considered. This yields a total magnetic moment of ~4 μ${_B}$ per formula unit in monolayer MnSe${_2}$, which is in close agreement to the theoretically predicted value.

cond-mat.mtrl-sci↗

arXiv2018

Probing Tunneling Spin Injection into Graphene via Bias Dependence

The bias dependence of spin injection in graphene lateral spin valves is systematically studied to determine the factors affecting the tunneling spin injection efficiency. Three types of junctions are investigated, including MgO and hexagonal boron nitride (hBN) tunnel barriers and direct contacts. A DC bias current applied to the injector electrode induces a strong nonlinear bias dependence of the nonlocal spin signal for both MgO and hBN tunnel barriers. Furthermore, this signal reverses its sign at a negative DC bias for both kinds of tunnel barriers. The analysis of the bias dependence for injector electrodes with a wide range of contact resistances suggests that the sign reversal correlates with bias voltage rather than current. We consider different mechanisms for nonlinear bias dependence and conclude that the energy-dependent spin-polarized electronic structure of the ferromagnetic electrodes, rather than the electrical field-induced spin drift effect or spin filtering effect of the tunnel barrier, is the most likely explanation of the experimental observations.

cond-mat.mes-hall↗

arXiv2018

Strong and Tunable Spin Lifetime Anisotropy in Dual-Gated Bilayer Graphene

We report the discovery of a strong and tunable spin lifetime anisotropy with excellent spin lifetimes up to 7.8 ns in dual-gated bilayer graphene. Remarkably, this realizes the manipulation of spins in graphene by electrically-controlled spin-orbit fields, which is unexpected due to graphene's weak intrinsic spin-orbit coupling. We utilize both the in-plane magnetic field Hanle precession and oblique Hanle precession measurements to directly compare the lifetimes of out-of-plane vs. in-plane spins. We find that near the charge neutrality point, the application of a perpendicular electric field opens a band gap and generates an out-of-plane spin-orbit field that stabilizes out-of-plane spins against spin relaxation, leading to a large spin lifetime anisotropy. This intriguing behavior occurs because of the unique spin-valley coupled band structure of bilayer graphene. Our results demonstrate the potential for highly tunable spintronic devices based on dual-gated 2D materials.

cond-mat.mes-hall↗

arXiv2018

Topological Dirac Semimetal Na3Bi Films in the Ultrathin Limit via Alternating Layer Molecular Beam Epitaxy

Ultrathin films of Na3Bi on insulating substrates are desired for opening a bulk band gap and generating the quantum spin Hall effect from a topological Dirac semimetal, though continuous films in the few nanometer regime have been difficult to realize. Here, we utilize alternating layer molecular beam epitaxy (MBE) to achieve uniform and continuous single crystal films of Na3Bi(0001) on insulating Al2O3(0001) substrates and demonstrate electrical transport on films with 3.8 nm thickness (4 unit cells). The high material quality is confirmed through in situ reflection high-energy electron diffraction (RHEED), scanning tunneling microscopy (STM), x-ray diffraction (XRD), and x-ray photoelectron spectroscopy (XPS). In addition, these films are employed as seed layers for subsequent growth by codeposition, leading to atomic layer-by-layer growth as indicated by RHEED intensity oscillations. These material advances facilitate the pursuit of quantum phenomena in thin films of Dirac semimetals.

cond-mat.mtrl-sci↗