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Zhiqiang Mao

Publications and source records attributed to Zhiqiang Mao.

At least 37 records · Page 2Linked to original sources

Spectroscopic evidence of intra-unit-cell charge redistribution in charge-neutral magnetic topological insulator Sb-doped MnBi6Te10

The magnetic topological insulator MnBi$_{6}$Te$_{10}$ has emerged as a promising candidate for realizing the quantum anomalous Hall effect (QAHE), owing to its ability to retain ferromagnetism through precise control of anti-site defects. The next important task for realizing the QAHE is to tune the chemical potential into the energy gap formed by the broken time-reversal symmetry. Here we reveal an intra-unit-cell charge redistribution even when the overall doping suggests a near-charge-neutral condition. By performing time- and angle-resolved photoemission spectroscopy (trARPES) on the optimally 18% Sb-doped MnBi$_{6}$Te$_{10}$, we observe transient surface photovoltage (SPV) effects on both the MnBi$_{2}$Te$_{4}$ and single-Bi$_{2}$Te$_{3}$ terminations. Furthermore, we observe a time-dependent splitting of the band structure indicating multiple SPV shifts with different magnitudes. This observation suggests that adjacent plateaus with nominally the same terminating layer exhibit a strong intra-unit-cell charge redistribution, resulting in spontaneous electrical polarization. This is consistent with static micro-ARPES measurements revealing significant doping deviations from the charge-neutral configuration. Our findings underscore the challenges of engineering the family of Mn-Bi-Te materials to realize QAHE purely through chemical doping. Achieving the desired topological quantum phase requires both a uniform carrier doping and a ferromagnetic ground state. Furthermore, the light-induced polarization within each unit cell of ferromagnetic Mn(Bi$_{0.82}$Sb$_{0.18}$)$_{6}$Te$_{10}$ may open new possibilities for optoelectronic and spintronics.

cond-mat.mes-hall↗

Double-Crucible Vertical Bridgman Technique for Stoichiometry-Controlled Chalcogenide Crystal Growth

Precise stoichiometry control in single-crystal growth is essential for both technological applications and fundamental research. However, conventional growth methods often face challenges such as non-stoichiometry, compositional gradients, and phase impurities, particularly in non-congruent melting systems. Even in congruent melting systems like Bi2Se3, deviations from the ideal stoichiometric composition can lead to significant property degradation, such as excessive bulk conductivity, which limits its topological applications. In this study, we introduce the double-crucible vertical Bridgman (DCVB) method, a novel approach that enhances stoichiometry control through the combined use of continuous source material feeding, traveling-solvent growth, and liquid encapsulation, which suppresses volatile element loss under high pressure. Using Bi2Se3 as a model system, we demonstrate that crystals grown via DCVB exhibit enhanced stoichiometric control, significantly reducing defect density and achieving much lower carrier concentrations compared to those produced by conventional Bridgman techniques. Moreover, the continuous feeding of source material enables the growth of large crystals. This approach presents a promising strategy for synthesizing high-quality, large-scale crystals, particularly for metal chalcogenides and pnictides that exhibit challenging non-congruent melting behaviors.

cond-mat.mtrl-sci↗

Discovery of a Highly Anisotropic Type-II Ferromagnetic Weyl State Exhibiting a 3D Quantum Hall Effect

Topological semimetals, particularly Weyl semimetals (WSMs), are crucial platforms for exploring emergent quantum phenomena due to their unique electronic structures and potential to transition into various topological phases. In this study, we report the discovery of a ferromagnetic (FM) type-II WSM in Mn(Bi1-xSbx)4Te7, which exhibits a remarkable three-dimensional (3D) quantum Hall effect (QHE). By precisely tuning the chemical potential through Sb doping, we obtained samples with the Fermi level near the charge neutrality point for x = ~ 0.27. This was confirmed by spectroscopy measurements (ARPES and STS), and these samples showed strong quantum oscillations along with a key transport signature of a Weyl state - chiral anomaly, and Fermi surface reconstruction driven by FM ordering. Our theoretical analysis indicates that this Weyl state evolves from a parent nodal ring state, where higher-order k-terms split the nodal line into type-II Weyl nodes. The Weyl state exhibits significant anisotropy, characterized by a pronounced reduction in Fermi velocity along the kz-axis, likely accounting for the observed 3D QHE. These results not only highlight the exceptional tunability of the Mn(Bi1-xSbx)4Te7 system, where precise control of the chemical potential and magnetic properties opens access to novel quantum phases, but also advance the understanding of FM WSMs.

cond-mat.mtrl-sci↗

Surface-dominant transport in Weyl semimetal NbAs nanowires for next-generation interconnects

Ongoing demands for smaller and more energy efficient electronic devices necessitate alternative interconnect materials with lower electrical resistivity at reduced dimensions. Despite the emergence of many promising candidates, synthesizing high quality nanostructures remains a major bottleneck in evaluating their performance. Here, we report the successful synthesis of Weyl semimetal NbAs nanowires via thermomechanical nanomolding, achieving single crystallinity and controlled diameters as small as 40 nm. Our NbAs nanowires exhibit a remarkably low room-temperature resistivity of 9.7 +/- 1.6 microOhm-cm, which is three to four times lower than their bulk counterpart. Theoretical calculations corroborate the experimental observations, attributing this exceptional resistivity reduction to surface dominant conduction with long carrier lifetime at finite temperatures. Further characterization of NbAs nanowires and bulk single crystals reveals high breakdown current density, robust stability, and superior thermal conductivity. Collectively, these properties highlight the strong potential of NbAs nanowires as next-generation interconnects, which can surpass the limitations of current copper-based interconnects. Technologically, our findings present a practical application of topological materials, while scientifically showcasing the fundamental properties uniquely accessible in nanoscale platforms.

cond-mat.mes-hall↗

Beyond-Hubbard pairing in a cuprate ladder

The Hubbard model is believed to capture the essential physics of cuprate superconductors. However, recent theoretical studies suggest that it fails to reproduce a robust and homogeneous superconducting ground state. Here, using resonant inelastic x-ray scattering and density matrix renormalization group calculations, we show that magnetic excitations in the prototypical cuprate ladder Sr$_{14}$Cu$_{24}$O$_{41}$ are inconsistent with those of a simple Hubbard model. The magnetic response of hole carriers, contributing to an emergent branch of spin excitations, is strongly suppressed. This effect is the consequence of d-wave-like pairing, enhanced by nearly an order of magnitude through a large nearest-neighbor attractive interaction. The similarity between cuprate ladders and the two-dimensional compounds suggests that such an enhanced hole pairing may be a universal feature of superconducting cuprates.

cond-mat.str-el↗

Semi-Dirac Fermions in a Topological Metal

Topological semimetals with massless Dirac and Weyl fermions represent the forefront of quantum materials research. In two dimensions (2D), a peculiar class of fermions that are massless in one direction and massive in the perpendicular direction was predicted sixteen years ago. These highly exotic quasiparticles - the semi-Dirac fermions - ignited intense theoretical and experimental interest but remain undetected. Using magneto-optical spectroscopy, we demonstrate the defining feature of semi-Dirac fermions - $B^{2/3}$ scaling of Landau levels - in a prototypical nodal-line metal ZrSiS. In topological metals, including ZrSiS, nodal-lines extend the band degeneracies from isolated points to lines, loops or even chains in the momentum space. With $\textit{ab initio}$ calculations and theoretical modeling, we pinpoint the observed semi-Dirac spectrum to the crossing points of nodal-lines in ZrSiS. Crossing nodal-lines exhibit a continuum absorption spectrum but with singularities that scale as $B^{2/3}$ at the crossing. Our work sheds light on the hidden quasiparticles emerging from the intricate topology of crossing nodal-lines and highlights the potential to explore quantum geometry with linear optical responses.

cond-mat.mtrl-sci↗

Tunneling current-controlled spin states in few-layer van der Waals magnets

Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3 layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3 tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing.

cond-mat.mes-hall↗

Emergence of electric-field-tunable interfacial ferromagnetism in 2D antiferromagnet heterostructures

Van der Waals (vdW) magnet heterostructures have emerged as new platforms to explore exotic magnetic orders and quantum phenomena. Here, we study heterostructures of layered antiferromagnets, CrI3 and CrCl3, with perpendicular and in-plane magnetic anisotropy, respectively. Using magneto-optical Kerr effect microscopy, we demonstrate out-of-plane magnetic order in the CrCl3 layer proximal to CrI3, with ferromagnetic interfacial coupling between the two. Such an interlayer exchange field leads to higher critical temperature than that of either CrI3 or CrCl3 alone. We further demonstrate significant electric-field control of the coercivity, attributed to the naturally broken structural inversion symmetry of the heterostructure allowing unprecedented direct coupling between electric field and interfacial magnetism. These findings illustrate the opportunity to explore exotic magnetic phases and engineer spintronic devices in vdW heterostructures.

cond-mat.mtrl-sci↗

Electrically tunable moiré magnetism in twisted double bilayers of chromium triiodide

Moiré superlattices in van der Waals structures can be used to control the electronic properties of the material and lead to emergent correlated and topological phenomena. Its first demonstration in van der Waals magnets exhibited noncollinear states and domain structures with, however, limited manipulation. Here we report electrically tunable moiré magnetism in twisted double bilayers - that is, a bilayer plus a bilayer with a twist angle between them - of layered antiferromagnet CrI3. Using magneto-optical Kerr effect microscopy, we observe the coexistence of antiferromagnetic and ferromagnetic order with nonzero net magnetization - a hallmark of moiré magnetism. Such magnetic state extends over a wide range of twist angles (with transitions at around 0° and above 20°) and exhibits a nonmonotonic temperature dependence. We further demonstrate voltage-assisted magnetic switching. The observed nontrivial magnetic states and unprecedented control by twist angle, temperature and electrical gating are supported by the simulated phase diagram of the moiré magnetism.

cond-mat.mtrl-sci↗

Distinguishing Surface and Bulk Electromagnetism via Their Dynamics in an Intrinsic Magnetic Topological Insulator

The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi2Te4. Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but over-estimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi2Te4. Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics.

cond-mat.str-el↗

Crystallographic Disorder and Strong Magnetic Anisotropy in Dy3.1Pt2.0Sb3.8

We report the crystal growth and characterization of a rare-earth-containing material, Dy3.00(1)Pt2Sb4.48(2). This compound possesses a similar structure to the previously reported Y3Pt4Ge6, but lacks two layers of Pt atoms. Crystallographic disorder was found in Dy3.00(1)Pt2Sb4.48(2). Additionally, the Dy-Dy framework was found to have both square net and triangular lattices. Dy3.00(1)Pt2Sb4.48(2)8 was determined to be antiferromagnetically ordered around ~15 K while a competing antiferromagnetic sublattice also exists at lower temperature. Strong magnetic anisotropy was observed and several metamagnetic transitions were seen in the hysteresis loops. Furthermore, the Curie-Weiss fitting revealed unusually small effective moment of Dy, which is far below the expected value of Dy3+ (10.65 muB). This material might provide a new platform to study the relation between crystallographic disorder and magnetism.

cond-mat.mtrl-sci↗

Structure and lattice excitations of the copper substituted lead oxyapatite Pb$_{9.06(7)}$Cu$_{0.94(6)}$(PO$_{3.92(4)}$)$_{6}$O$_{0.96(3)}$

The copper substituted lead oxyapatite, Pb$_{10-x}$Cu$_{x}$(PO$_{3.92(4)}$)$_{6}$O$_{0.96(3)}$ (x=0.94(6)) was studied using neutron and x-ray diffraction and neutron spectroscopy techniques. The crystal structure of the main phase of our sample, which has come to be colloquially known as LK-99, is verified to possess a hexagonal structure with space group $P 6_{3}/m$, alongside the presence of impurity phases Cu and Cu$_2$S. We determine the primary substitution location of the Cu as the Pb1 ($6h$) site, with a small substitution at the Pb2 ($4f$) site. Consequently, no clear Cu-doping-induced structural distortion was observed in the investigated temperature region between 10~K and 300~K. Specially, we did not observe a reduction of coordinate number at the Pb2 site or a clear tilting of PO$_4$ tetrahedron. Magnetic characterization reveals a diamagnetic signal in the specimen, accompanied by a very weak ferromagnetic component at 2 K. No long-range magnetic order down to 10 K was detected by the neutron diffraction. Inelastic neutron scattering measurements did not show magnetic excitations for energies up to 350 meV. There is no sign of a superconducting resonance in the excitation spectrum of this material. The measured phonon density of states compares well with density functional theory calculations performed for the main LK-99 phase and its impurity phases. Our study may shed some insight into the role of the favored substitution site of copper in the absence of structural distortion and superconductivity in LK-99.

cond-mat.mtrl-sci↗

Ferroelectric Schottky diodes of CuInP$_2$S$_6$ nanosheet

Ferroelectricity in van der Waals (vdW) layered material has attracted a great deal of interest recently. CuInP$_2$S$_6$ (CIPS), the only vdW layered material whose ferroelectricity in the bulk was demonstrated by direct polarization measurements, was shown to remain ferroelectric down to a thickness of a few nanometers. However, its ferroelectric properties have just started to be explored in the context of potential device applications. We report here the preparation and measurements of metal-ferroelectric semiconductor-metal heterostructures using nanosheets of CIPS obtained by mechanical exfoliation. Four bias voltage and polarization dependent resistive states were observed in the current-voltage characteristics, which we attribute to the formation of ferroelectric Schottky diode, along with switching behavior.

cond-mat.mtrl-sci↗

Hidden non-collinear spin-order induced topological surface states

Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report the observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Neel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

cond-mat.str-el↗

Colossal nonreciprocal Hall effect and broadband frequency mixing due to a room temperature nonlinear Hall effect

Nonreciprocal (NR) charge transport in quantum materials has attracted enormous interest since it offers an avenue to investigate quantum symmetry related physics and holds many prospective applications such as rectification and photodetection over a wide range of frequencies. The NR transport reported to date occurs along the longitudinal direction with the NR resistance limited to a few percent of the ohmic resistance. Here we report a transverse nonreciprocal transport phenomenon with divergent nonreciprocity - colossal NR Hall effect. This is revealed in direct current (DC) measurements on the microscale Hall devices made of the Pt wires deposited by focused ion beam (FIB) on Si substrates and the Weyl semimetal NbP with FIB-deposited Pt electrodes at 0 magnetic field. When a DC is applied along the x-axis of the devices Ix, it generates a voltage along the y-axis Vy near room temperature, with Vy quadratically scaling with Ix. The transverse resistance, which shows a sign reversal upon switching the current direction, results from a colossal extrinsic nonlinear Hall effect (NLHE) rooted in the disorder scatterings in the Pt wires. While NbP was not found to show NLHE, the NLHE generated in the Pt electrodes can be transmitted to the NbP Hall devices, which yields a surprisingly large nonlinear anomalous Hall effect in NbP with the Hall angle (${Θ_H}$) far exceeding the record value of the anomalous Hall angle of magnetic conductors at room temperature. Furthermore, we find such a strong NLHE can lead to broadband frequency mixing, with the frequency spectrum of the Hall voltage including 2nd-harmonic generation, sum & difference frequency generations, and other multiple wave mixing components. These results not only demonstrate the concept of the NRHE for the first time but also pave the way for exploring NLHE's applications in Thz communication, imaging, and energy harvesting.

cond-mat.mes-hall↗

Coupling Between Magnetic and Transport Properties in Magnetic Layered Material Mn2-xZnxSb

We synthesized single crystals for Mn2-xZnxSb and studied their magnetic and electronic transport properties. This material system displays rich magnetic phase tunable with temperature and Zn composition. In addition, two groups of distinct magnetic and electronic properties, separated by a critical Zn composition of x = 0.6, are discovered. The Zn-less samples are metallic and characterized by a resistivity jump at the magnetic ordering temperature, while the Zn-rich samples lose metallicity and show a metal-to-insulator transition-like feature tunable by magnetic field. Our findings establish Mn2-xZnxSb as a promising material platform that offers opportunities to study how the coupling of spin, charge, and lattice degrees of freedom governs interesting transport properties in 2D magnets, which is currently a topic of broad interest.

cond-mat.mtrl-sci↗

Pressure tunable quantum anomalous Hall states in a topological antiferromagnet

Mechanical modulation of the lattice parameter can modify the electronic structure and manipulate the magnetic coupling of a material without introducing impurities. Inspired by success in pressure-controlled magnetism, we investigate the effect of hydrostatic pressure on quantized Chern states in the antiferromagnetic topological insulator MnBi2Te4, using transport as a probe. We show that pressure can enhance the robustness of quantum anomalous Hall (QAH) phases that are otherwise delicate in 7SL MnBi2Te4 and in the spin-flop (SF) state of 8SL MnBi2Te4. We explain our findings using a coupled Dirac cone model of MnBi2Te4, which identifies stronger hybridization between van der Waals layers as the driver of topological states. We further demonstrate that moderate pressures readily available in laboratory systems can provide reversible control of magnetic and topological phases. Our results reveal a strong connection between the mechanical engineering of band topology and magnetism.

cond-mat.mes-hall↗

A simplified method characterizing magnetic ordering modulated photo-thermoelectric response in noncentrosymmetric semimetal Ca3Ru2O7

Photo-Thermoelectric (PTE) response is usually one of the main working mechanisms for photodetectors. However, as another fast and easier way to measure thermoelectric characteristics of materials, it can also reveal important physics such as electric-phonon coupling, electron-electron correlation, etc. Recently, the spin entropy related to magnetic order transition which contributes to thermoelectric power is attracting more and more attention. Here, we demonstrate the PTE response can be reshaped when Ca3Ru2O7 undergoes meta-magnetic phase (MMP) transition driven by both temperature and magnetic field. Firstly, a sign change is observed crossing TS = 48 K and the linear polarization angle dependent PTE current maximizes along a-axis above TS while maximizes along b-axis below TS, which indicates that the antiferromagnetic spin order contributes to such spatial anisotropy. Secondly, in the temperature range of around 40 ~ 50 K, the PTE current is found to be sharply suppressed when external magnetic field is applied in plane along a-axis but is only gradually suppressed when applied field is along b-axis which gives out two critical fields. We attribute such suppression of PTE current under magnetic field to the suppression of the spin entropy in the phase transition between the antiferromagnetic state and the MMP state and the H-T phase diagrams of Ca3Ru2O7 is redrawn accordingly. Compared to previously work which trying to understand the magnetic phase transition in Ca3Ru2O7, such as neutron scattering, specific heat, and other advanced transport measurements, our work provides a more convenient yet efficient method, which may also find applications in other correlated spin materials in general.

cond-mat.str-el↗