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Identifying air-stable two-dimensional (2D) ferromagnetism with high Curie temperature (Tc) is highly desirable for its potential applications in next-generation spintronics. However, most of the work reported so far mainly focuses on promoting one specific key factor of 2D ferromagnetism (Tc or air stability), rather than comprehensive promotion of both of them. Herein, ultrathin Cr1−xTe crystals grown by chemical vapor deposition (CVD) show thickness-dependent Tc up to 285 K. The out-of-plane ferromagnetic order is well preserved down to atomically thin limit (2.0 nm), as evidenced by anomalous Hall effect observed in non-encapsulated samples. Besides, the CVD-grown Cr1−xTe nanosheets present excellent ambient stability, with no apparent change in surface roughness or electrical transport properties after exposure to air for months. Our work provides an alternative platform for investigation of intrinsic 2D ferromagnetism and development of innovative spintronic devices.

Heteroepitaxy with large lattice mismatch remains a great challenge for high-quality epifilm growth. Although great efforts have been devoted to epifilm growth with an in-plane lattice mismatch, the epitaxy of 2D layered crystals on stepped substrates with a giant out-of-plane lattice mismatch is seldom reported. Here, taking the molecular-beam epitaxy of 2D semiconducting Bi

Magnetic anisotropy is essential for permanent magnets to maintain their magnetization along specific directions. Understanding and controlling the magnetic anisotropy on a single-molecule scale are challenging but of fundamental importance for the future's spintronic technology. Here, by using scanning tunneling microscopy (STM), we demonstrated the ability to control the magnetic anisotropy by tuning the ligand field at the single-molecule level. We constructed a molecular magnetic complex with a single Mn atom and an organic molecule (4,4'-biphenyldicarbonitrile) as a ligand via atomic manipulation. Inelastic tunneling spectra (IETS) show that the Mn complex has much larger axial magnetic anisotropy than individual Mn atoms, and the anisotropy energy can be tuned by the coupling strength of the ligand. With density functional theory calculations, we revealed that the enhanced magnetic anisotropy of Mn arising from the carbonitrile ligand provides a prototype for the engineering of the magnetism of quantum devices.

We exploit a high-performing resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi2 O2 Se nanoplates. Scanning tunneling microscopy combined with first-principle calculations confirms an amorphous Se atomic layer formed on the surface of 2D Bi2 O2 Se exposed to oxygen, which contributes to larger specific surface area and abundant active adsorption sites. Such 2D Bi2 O2 Se oxygen sensors have remarkable oxygen-adsorption induced variations of carrier density/mobility, and exhibit an ultrahigh sensitivity featuring minimum detection limit of 0.25 ppm, long-term stability, high durativity, and wide-range response to concentration up to 400 ppm at room temperature. 2D Bi2 O2 Se arrayed sensors integrated in parallel form are found to possess an oxygen detection minimum of sub-0.25 ppm ascribed to an enhanced signal-to-noise ratio. These advanced sensor characteristics involving ease integration show 2D Bi2 O2 Se is an ideal candidate for trace oxygen detection.

Silicon-based transistors are approaching their physical limits and thus new high-mobility semiconductors are sought to replace silicon in the microelectronics industry. Both bulk materials (such as silicon-germanium and III–V semiconductors) and low-dimensional nanomaterials (such as one-dimensional carbon nanotubes and two-dimensional transition metal dichalcogenides) have been explored, but, unlike silicon, which uses silicon dioxide (SiO2) as its gate dielectric, these materials suffer from the absence of a high-quality native oxide as a dielectric counterpart. This can lead to compatibility problems in practical devices. Here, we show that an atomically thin gate dielectric of bismuth selenite (Bi2SeO5) can be conformally formed via layer-by-layer oxidization of an underlying high-mobility two-dimensional semiconductor, Bi2O2Se. Using this native oxide dielectric, high-performance Bi2O2Se field-effect transistors can be created, as well as inverter circuits that exhibit a large voltage gain (as high as 150). The high dielectric constant (~21) of Bi2SeO5 allows its equivalent oxide thickness to be reduced to 0.9 nm while maintaining a gate leakage lower than thermal SiO2. The Bi2SeO5 can also be selectively etched away by a wet chemical method that leaves the mobility of the underlying Bi2O2Se semiconductor almost unchanged. An atomically thin high-κ gate dielectric of Bi2SeO5 can be formed via layer-by-layer oxidization of an underlying two-dimensional semiconductor, allowing high-performance field-effect transistors and inverters to be fabricated.

We report the discovery of a new three-dimensional (3D) topological Dirac semimetal (TDS) material KZnBi, coexisting with a naturally formed superconducting state on the surface under ambient pressure. Using photoemission spectroscopy together with first-principles calculations, a 3D Dirac state with linear band dispersion is identified. The characteristic features of massless Dirac fermions are also confirmed by magnetotransport measurements, exhibiting an extremely small cyclotron mass of m^{*}=0.012 m_{0} and a high Fermi velocity of v_{F}=1.04×10^{6} m/s. Interestingly, superconductivity occurs below 0.85 K on the (001) surface, while the bulk remains nonsuperconducting. The captured linear temperature dependence of the upper critical field suggests the possible non-s-wave character of this surface superconductivity. Our discovery serves a distinctive platform to study the interplay between 3D TDS and the superconductivity.

Research on the anomalous Hall effect (AHE) has been lasting for a century to make clear the underlying physical mechanism. Generally, the AHE appears in magnetic materials, in which the extrinsic process related to scattering effects and intrinsic contribution connected with Berry curvature are crucial. Recently, AHE has been counterintuitively observed in nonmagnetic topological materials and attributed to the existence of Weyl points. However, the Weyl point scenario would lead to unsaturated AHE even in large magnetic fields and contradicts the saturation of AHE in several tesla (T) in experiments. In this work, we investigate the Hall effect of $\mathrm{Zr}{\mathrm{Te}}_{5}$ and $\mathrm{Hf}{\mathrm{Te}}_{5}$ thin flakes in static ultrahigh magnetic fields up to 33 T. We find the AHE saturates to $55\phantom{\rule{0.16em}{0ex}}(70)\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Omega}}}^{\text{}1}\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{\text{}1}$ for $\mathrm{Zr}{\mathrm{Te}}_{5}$ ($\mathrm{Hf}{\mathrm{Te}}_{5}$) thin flakes above $\ensuremath{\sim}10\phantom{\rule{0.16em}{0ex}}\mathrm{T}$. Combining detailed magnetotransport experiments and Berry curvature calculations, we clarify that the splitting of massive Dirac bands without Weyl points can be responsible for AHE in nonmagnetic topological materials $\mathrm{Zr}{\mathrm{Te}}_{5}$ and $\mathrm{Hf}{\mathrm{Te}}_{5}$ thin flakes. This model can identify our thin flake samples to be weak topological insulators and serve as a tool to probe the band structure topology in topological materials.

The air-stable and high-mobility two-dimensional (2D) Bi2O2Se semiconductor has emerged as a promising alternative that is complementary to graphene, MoS2, and black phosphorus for next-generation digital applications. However, the room-temperature residual charge carrier concentration of 2D Bi2O2Se nanoplates synthesized so far is as high as about 1019–1020 cm–3, which results in a poor electrostatic gate control and unsuitable threshold voltage, detrimental to the fabrication of high-performance low-power devices. Here, we first present a facile approach for synthesizing 2D Bi2O2Se single crystals with ultralow carrier concentration of ∼1016 cm–3 and high Hall mobility up to 410 cm2 V–1 s–1 simultaneously at room temperature. With optimized conditions, these high-mobility and low-carrier-concentration 2D Bi2O2Se nanoplates with domain sizes greater than 250 μm and thicknesses down to 4 layers (∼2.5 nm) were readily grown by using Se and Bi2O3 powders as coevaporation sources in a dual heating zone chemi...

${\mathrm{FeSe}}_{0.45}{\mathrm{Te}}_{0.55}$ (FeSeTe) has recently emerged as a promising candidate to host topological superconductivity, with a Dirac surface state and signatures of Majorana bound states in vortex cores. However, correlations strongly renormalize the bands compared to electronic structure calculations, and there is no evidence for the expected bulk band inversion. We present here a comprehensive angle resolved photoemission (ARPES) study of FeSeTe as a function of photon energies ranging from 15--100 eV. We find that although the top of the bulk valence band shows essentially no ${k}_{z}$ dispersion, its normalized intensity exhibits a periodic variation with ${k}_{z}$. We show, using ARPES selection rules, that the intensity oscillation is a signature of band inversion indicating a change in the parity going from $\mathrm{\ensuremath{\Gamma}}$ to $Z$. We also present a simple realistic tight-binding model which gives insight into ARPES observations. Thus we provide direct evidence for a topologically nontrivial bulk band structure that supports protected surface states.

Understanding the nonequilibrium dynamics of photoexcited polarons at the atomic scale is of great importance for improving the performance of photocatalytic and solar-energy materials. Using a pulsed-laser-combined scanning tunneling microscopy and spectroscopy, here we succeeded in resolving the relaxation dynamics of single polarons bound to oxygen vacancies on the surface of a prototypical photocatalyst, rutile TiO_{2}(110). The visible-light excitation of the defect-derived polarons depletes the polaron states and leads to delocalized free electrons in the conduction band, which is further corroborated by ab initio calculations. We found that the trapping time of polarons becomes considerably shorter when the polaron is bound to two surface oxygen vacancies than that to one. In contrast, the lifetime of photogenerated free electrons is insensitive to the atomic-scale distribution of the defects but correlated with the averaged defect density within a nanometer-sized area. Those results shed new light on the photocatalytically active sites at the metal-oxide surface.

We exploit a high-performing resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi

The discovery of topological Weyl semimetals has revealed opportunities to realize several extraordinary physical phenomena in condensed matter physics. Specifically, Weyl semimetals with strong spin-orbit coupling, broken inversion symmetry, and novel spin textures are predicted to exhibit a large spin Hall effect that can efficiently convert the charge current to a spin current. Here, we report a direct experimental observation of large spin Hall and inverse spin Hall effects in the Weyl semimetal WTe2 at room temperature obeying the Onsager reciprocity relation. We demonstrate the detection of a pure spin current generated by the spin Hall phenomenon in WTe2 by making a van der Waals heterostructure with graphene, taking advantage of its long spin coherence length and spin transmission at the heterostructure interface. These experimental findings, well supported by ab initio calculations, show a large charge-spin conversion efficiency in WTe2, which can pave the way for the utilization of spin-orbit-induced phenomena in spintronic memory and logic circuit architectures.

Dual topological materials are unique topological phases that host coexisting surface states of different topological nature on the same or on different material facets. Here, we show that Bi2TeI is a dual topological insulator. It exhibits band inversions at two time reversal symmetry points of the bulk band, which classify it as a weak topological insulator with metallic states on its 'side' surfaces. The mirror symmetry of the crystal structure concurrently classifies it as a topological crystalline insulator. We investigated Bi2TeI spectroscopically to show the existence of both two-dimensional Dirac surface states, which are susceptible to mirror symmetry breaking, and one-dimensional channels that reside along the step edges. Their mutual coexistence on the step edge, where both facets join, is facilitated by momentum and energy segregation. Our observation of a dual topological insulator should stimulate investigations of other dual topology classes with distinct surface manifestations coexisting at their boundaries.

We used screw dislocations as a tool to probe spectroscopically the topological classification of electronic matter in bismuth., The growing diversity of topological classes leads to ambiguity between classes that share similar boundary phenomenology. This is the status of bulk bismuth. Recent studies have classified it as either a strong or a higher-order topological insulator, both of which host helical modes on their boundaries. We resolve the topological classification of bismuth by spectroscopically mapping the response of its boundary modes to a screw-dislocation. We find that the one-dimensional mode, on step-edges, extends over a wide energy range and does not open a gap near the screw-dislocations. This signifies that this mode binds to the screw-dislocation, as expected for a material with nonzero weak indices. We argue that the small energy gap, at the time reversal invariant momentum L, positions bismuth within the critical region of a topological phase transition between a higher-order topological insulator and a strong topological insulator with nonzero weak indices.

Photoexcitation is a powerful means in distinguishing different interactions and manipulating the states of matter, especially in charge density wave (CDW) materials. The CDW state of 1

The layered antiferromagnetic MnBi2Te4 films have been proposed to be an intrinsic quantum anomalous Hall (QAH) insulator with a large gap. To realize this proposal, it is crucial to open a magnetic gap of surface states. However, recent experiments have observed gapless surface states, indicating the absence of out-of-plane surface magnetism, and thus the quantized Hall resistance can only be achieved at the magnetic field above 6 T. In this work, we propose to induce out-of-plane surface magnetism of MnBi2Te4 films via the magnetic proximity with magnetic insulator CrI3. Our calculations have revealed a strong exchange bias ~ 40 meV, originating from the long Cr-eg orbital tails that hybridize strongly with Te p-orbitals. By stabilizing surface magnetism, the QAH effect can be realized in the MnBi2Te4/CrI3 heterostructure. Our calculations also demonstrate the high Chern number QAH state can be achieved by controlling external electric gates. Thus, the MnBi2Te4/CrI3 heterostructure provides a promising platform to realize the electrically tunable zero-field QAH effect., 9 Pages including Appendix

Collinear IrMn offers new opportunities for future magnetic memory design as it can be an effective source of spin-orbit torque., Spin-orbit torque (SOT) offers promising approaches to developing energy-efficient memory devices by electric switching of magnetization. Compared to other SOT materials, metallic antiferromagnet (AFM) potentially allows the control of SOT through its magnetic structure. Here, combining the results from neutron diffraction and spin-torque ferromagnetic resonance experiments, we show that the magnetic structure of epitaxially grown L10-IrMn (a collinear AFM) is distinct from the widely presumed bulk one. It consists of twin domains, with the spin axes orienting toward [111] and [−111], respectively. This unconventional magnetic structure is responsible for much larger SOT efficiencies up to 0.60 ± 0.04, compared to 0.083 ± 0.002 for the polycrystalline IrMn. Furthermore, we reveal that this magnetic structure induces a large isotropic bulk contribution and a comparable anisotropic interfacial contribution to the SOT efficiency. Our findings shed light on the critical roles of bulk and interfacial antiferromagnetism to SOT generated by metallic AFM.

The air-stable and high-mobility two-dimensional (2D) Bi

Doping with transition metal elements is an effective method to introduce magnetism in graphene, which could enable future graphene-based spintronic devices. Motivated by the recent experimental observation of a stable single layer iron membrane embedded in graphene perforation, we investigate the electronic and magnetic properties of the Fe-nanostructure-embedded graphene system based on first principles calculations. The results demonstrate that strain could lead to dramatic changes in the magnetic configurations for both small Fe clusters bonded to the edge carbon atoms of graphene perforation and the single layer Fe membrane fully embedded in the graphene layer. For optimal doping, a delicate balance can be achieved, which leads to a half-metallic electronic structure. This work suggests an easy and effective method to introduce and tune the magnetic properties of graphene, which offers a new direction for the development of future graphene-based spintronic devices.

Single-layer transition-metal dichalcogenides (TMDs) such as MoS2 and MoSe2 exhibit unique electronic band structures ideal for hosting many exotic spin-orbital orderings. It has been widely accepted that Rashba spin splitting (RSS) is linearly proportional to the external field in heterostructure interfaces or to the potential gradient in polar materials. Surprisingly, an extraordinary nonlinear dependence of RSS is found in semiconducting TMD monolayers under a gate field. In contrast to small and constant RSS in polar materials, the potential gradient in non-polar TMDs gradually increases with the gate bias, resulting in nonlinear RSS with a Rashba coefficient an order-of-magnitude larger than the linear one. Most strikingly, under a large gate field MoSe2 demonstrates the largest anisotropic spin splitting among all known semiconductors to our knowledge. Based on the k·p model via symmetry analysis, we identify that the third-order contributions are responsible for the large nonlinear Rashba splitting. The gate tunable spin splitting found in semiconducting pristine TMD monolayers promises future spintronics applications in that spin polarized electrons can be generated by external gating in an experimentally accessible way.

Two-dimensional (2D) heterostructures composed of transition-metal dichalcogenide atomic layers are the new frontier for novel optoelectronic and photovoltaic device applications. Some key properties that make these materials appealing, yet are not well understood, are ultrafast hole/electron dynamics, interlayer energy transfer and the formation of interlayer hot excitons. Here, we study photoexcited electron/hole dynamics in a representative heterostructure, the MoS2/WSe2 interface, which exhibits type II band alignment. Employing time-dependent density functional theory in the time domain, we observe ultrafast charge dynamics with lifetimes of tens to hundreds of femtoseconds. Most importantly, we report the discovery of an interfacial pathway in 2D heterostructures for the relaxation of photoexcited hot electrons through interlayer hopping, which is significantly faster than intralayer relaxation. This finding is of particular importance for understanding many experimentally observed photoinduced proc...

Semiconductors are essential materials that affect our everyday life in the modern world. Two-dimensional semiconductors with high mobility and moderate bandgap are particularly attractive today because of their potential application in fast, low-power, and ultrasmall/thin electronic devices. We investigate the electronic structures of a new layered air-stable oxide semiconductor, Bi

We introduce a class of two-dimensional (2D) materials that possess coexisting ferroelectric and topologically insulating orders. Such ferroelectric topological insulators (FETIs) occur in noncentrosymmetric atomic layer structures with strong spin-orbit coupling (SOC). We showcase a prototype 2D FETI in an atomically thin bismuth layer functionalized by CH2OH, which exhibits a large ferroelectric polarization that is switchable by a ligand molecule rotation mechanism and a strong SOC that drives a band inversion leading to the topologically insulating state. An external electric field that switches the ferroelectric polarization also tunes the spin texture in the underlying atomic lattice. Moreover, the functionalized bismuth layer exhibits an additional quantum order driven by the valley splitting at the K and K′ points in the Brillouin zone stemming from the symmetry breaking and strong SOC in the system, resulting in a remarkable state of matter with the simultaneous presence of the quantum spin Hall and quantum valley Hall effect. These phenomena are predicted to exist in other similarly constructed 2D FETIs, thereby offering a unique quantum material platform for discovering novel physics and exploring innovative applications.

Some two-dimensional liquid systems are theoretically predicted to have an anomalous phase transition due to unique intermolecular interactions, for example the first-order transition between two-dimensional high-density water and low-density amorphous ice. However, it has never been experimentally observed, to the best of our knowledge. Here we report an entropy-driven phase transition between a high-density liquid crystal and low-density crystalline solid, directly observed by scanning tunneling microscope in carbon monoxide adsorbed on Cu(111). Combined with first principle calculations, we find that repulsive dipole–dipole interactions between carbon monoxide molecules lead to unconventional thermodynamics. This finding of unconventional thermodynamics in two-dimensional carbon monoxide not only provides a platform to study the fundamental principles of anomalous phase transitions in two-dimensional liquids at the atomic scale, but may also help to design and develop more efficient copper-based catalysis., Intermolecular interactions have a crucial role in the adsorption of molecules on a surface, however their role in promoting phase transitions is less well known. Here, the authors report an abnormal phase transition between a high-density liquid crystal and low-density solid in the case of carbon monoxide on Cu(111), driven by intermolecular interactions and entropy.

Photoexcitation is a powerful means in distinguishing different interactions and manipulating the states of matter, especially in complex quantum systems. As a well-known charge density wave (CDW) material, 1T-TaS2 has been widely studied experimentally thanks to its intriguing photoexcited responses. However, the microscopic atomic dynamics and underlying mechanism are still under debate. Here, we demonstrate photoexcitation induced ultrafast dynamics in 1T-TaS2 using time-dependent density functional theory molecular dynamics. We discover a novel collective mode induced by photodoping, which is significantly different from thermally-induced phonon mode in TaS2. In addition, our finding validates nonthermal melting of CDW induced at low light intensities, supporting that conventional hot electron model is inadequate to explain photoinduced dynamics. Our results provide a deep insight on coherent electron and lattice quantum dynamics during the formation and excitation of CDW in 1T-TaS2., Comment: 5 figures

The Wiedemann-Franz (WF) law links the ratio of electronic charge and heat conductivity to fundamental constants. It has been tested in numerous solids, but the extent of its relevance to the anomalous transverse transport, which represents the topological nature of the wave function, remains an open question. Here we present a study of anomalous transverse response in the noncollinear antiferromagnet Mn$_{3}$Ge extended from room temperature down to sub-Kelvin temperature and find that the anomalous Lorenz ratio remains close to the Sommerfeld value up to 100 K, but not above. The finite-temperature violation of the WF correlation is caused by a mismatch between the thermal and electrical summations of the Berry curvature, rather than the inelastic scattering as observed in ordinary metals. This interpretation is backed by our theoretical calculations, which reveals a competition between the temperature and the Berry curvature distribution. The accuracy of the experiment is supported by the verification of the Bridgman relation between the anomalous Ettingshausen and Nernst effects. Our results identify the anomalous Lorenz ratio as an extremely sensitive probe of Berry spectrum near the chemical potential., Comment: 9 pages,6 figures, Supplemental Material included

Combining first principles investigations and scanning tunneling microscopy, we identify that the presumable van der Waals packed multilayered silicene sheets spontaneously transform into a diamond-structure bulk Si film due to strong interlayer couplings. In contrast to drastic surface reconstruction on conventional Si(111), multilayered silicene prepared by bottom-up epitaxy on Ag(111) exhibits a nearly ideal flat surface with only weak buckling. Without invoking Ag surfactants, √3 × √3 honeycomb patterns emerge thanks to dynamic fluctuation of mirror-symmetric rhombic phases, similar to monolayered silicene [Chen et al., Phys. Rev. Lett., 2013, 110, 085504]. The weak relaxation enables novel surface states with a Dirac linear dispersion.

We report on a Kondo effect on Co/Sb(111) mediating topological protection of the surface states against local magnetic perturbations. A sharp scanning tunneling spectroscopic peak near the Fermi energy is interpreted as a fingerprint of the Kondo resonance with a high Kondo temperature of about 200 K. Density function theory calculations reveal that the protruding Co adatoms are responsible for the Kondo peak, while the Co atoms underneath present as nonmagnetic impurities. By identifying the quasiparticle interference wavevectors, we demonstrate that only scattering channels related to backscattering confinements are observed for surfaces with and without the Co adsorption. It suggests that the Kondo effect suppresses the backscattering of the topological surface states and may help to expand the functionality of magnetically coupled topological materials for spintronics applications.

Dual topological materials are unique topological phases that host coexisting surface states of different topological nature on the same or on different material facets. Here, we show that Bi

The magnetoelectric (ME) effect originating from the effective coupling between electric field and magnetism is an exciting frontier in nanoscale science such as magnetic tunneling junction (MTJ), ferroelectric/piezoelectric heterojunctions etc. The realization of switchable ME effect under external electric field in d0 semiconducting materials of single composition is needed especially for all-silicon spintronics applications because of its natural compatibility with current industry. We employ density functional theory (DFT) to reveal that the pristine Si(111)-3×3 R30° (Si3 hereafter) reconstructed surfaces of thin films with a thickness smaller than eleven bilayers support a sizeable linear ME effect with switchable direction of magnetic moment under external electric field. This is achieved through the interlayer exchange coupling effect in the antiferromagnetic regime, where the spin-up and spin-down magnetized density is located on opposite surfaces of Si3 thin films. The obtained coefficient for the linear ME effect can be four times larger than that of ferromagnetic Fe films, which fail to have the reversal switching capabilities. The larger ME effect originates from the spin-dependent screening of the spin-polarized Dirac fermion. The prediction will promote the realization of well-controlled and switchable data storage in all-silicon electronics.

Light‐induced interlayer ultrafast charge transfer in 2D heterostructures provides a new platform for optoelectronic and photovoltaic applications. The charge separation process is generally hypothesized to be dependent on the interlayer stackings and interactions, however, the quantitative characteristic and detailed mechanism remain elusive. Here, a systematical study on the interlayer charge transfer in model MoS2/WS2 bilayer system with variable stacking configurations by time‐dependent density functional theory methods is demonstrated. The results show that the slight change of interlayer geometry can significantly modulate the charge transfer time from 100 fs to 1 ps scale. Detailed analysis further reveals that the transfer rate in MoS2/WS2 bilayers is governed by the electronic coupling between specific interlayer states, rather than the interlayer distances, and follows a universal dependence on the state‐coupling strength. The results establish the interlayer stacking as an effective freedom to control ultrafast charge transfer dynamics in 2D heterostructures and facilitate their future applications in optoelectronics and light harvesting.