Orbital-Selectivity-Induced Robust Quantum Anomalous Hall Effect in Hund's Metals MgFeP.

Ferromagnetic (FM) states with high Curie temperatures (Tc) and strong spin-orbit coupling (SOC) are indispensable for the long-sought room-temperature quantum anomalous Hall (QAH) effects. Here, we propose a two-dimensional (2D) iron-based monolayer MgFeP that exhibits a notably high FM Tc (about 1525 K) along with exceptional structural stabilities. The unique multiorbital nature in MgFeP, where localized dx2-y2 and dxz/yz orbitals coexist with itinerant dxy and dz2 orbitals, renders the monolayer a Hund's metal and in an orbital-selective Mott phase (OSMP). This OSMP triggers an FM double exchange mechanism, rationalizing the high Tc in the Hund's metal. This material transitions to a QAH insulator upon consideration of the SOC effect. By leveraging orbital selectivity, the QAH band gap can be enlarged by more than two times (to 137 meV). Our findings showcase Hund's metals as a promising material platform for realizing high-performance quantum topological electronic devices.

A new type of stable borophene with flat-band-induced magnetism.

Based on first-principles calculations, we propose a new type of thermally and dynamically stable magnetic borophene (B11) with a tetragonal lattice. The magnetism is found coming from spin polarization of one bonding flat band located at the Fermi level. Despite of the 'anti-molecular' behavior in the monolayer, the interactions between thepzorbitals of the B atoms in the double-octahedron structural unit lead to the formation of the flat bands with localization behaviors. One tight binding model is built to comprehend the magnetic mechanism, which can guide us to tune other nonmagnetic borophene becoming magnetic. Biaxial tensile strain (>2.1%) is found triggering a phase transition from a semimetal to a semiconductor in the B11monolayer. The mechanism is analyzed based on the orbital-resolved crystal field effect. Our work provides a new route for designing and achieving two-dimensional magnetic materials with light elements.

Quantum Spin-Valley Hall Kink States: From Concept to Materials Design.

We propose a general and tunable platform to realize high-density arrays of quantum spin-valley Hall kink (QSVHK) states with spin-valley-momentum locking based on a two-dimensional hexagonal topological insulator. Through the analysis of Berry curvature and topological charge, the QSVHK states are found to be topologically protected by the valley-inversion and time-reversal symmetries. Remarkably, the conductance of QSVHK states remains quantized against both nonmagnetic short- and long-range and magnetic long-range disorder, verified by the Green-function calculations. Based on first-principles results and our fabricated samples, we show that QSVHK states, protected with a gap up to 287 meV, can be realized in bismuthene by alloy engineering, surface functionalization, or electric field, supporting nonvolatile applications of spin-valley filters, valves, and waveguides even at room temperature.

Histamine H1 Receptor Contributes to Vestibular Compensation.

Vestibular compensation is responsible for the spontaneous recovery of postural, locomotor, and oculomotor dysfunctions in patients with peripheral vestibular lesion or posterior circulation stroke. Mechanism investigation of vestibular compensation is of great importance in both facilitating recovery of vestibular function and understanding the postlesion functional plasticity in the adult CNS. Here, we report that postsynaptic histamine H1 receptor contributes greatly to facilitating vestibular compensation. The expression of H1 receptor is restrictedly increased in the ipsilesional rather than contralesional GABAergic projection neurons in the medial vestibular nucleus (MVN), one of the most important centers for vestibular compensation, in unilateral labyrinthectomized male rats. Furthermore, H1 receptor mediates an asymmetric excitation of the commissural GABAergic but not glutamatergic neurons in the ipsilesional MVN, which may help to rebalance bilateral vestibular systems and promote vestibular compensation. Selective blockage of H1 receptor in the MVN significantly retards the recovery of both static and dynamic vestibular symptoms following unilateral labyrinthectomy, and remarkably attenuates the facilitation of betahistine, whose effect has traditionally been attributed to its antagonistic action on the presynaptic H3 receptor, on vestibular compensation. These results reveal a previously unknown role for histamine H1 receptor in vestibular compensation and amelioration of vestibular motor deficits, as well as an involvement of H1 receptor in potential therapeutic effects of betahistine. The findings provide not only a new insight into the postlesion neuronal circuit plasticity and functional recovery in the CNS, but also a novel potential therapeutic target for vestibular disorders.SIGNIFICANCE STATEMENT Vestibular disorders manifest postural imbalance, nystagmus, and vertigo. Vestibular compensation is critical for facilitating recovery from vestibular disorders, and of great importance in understanding the postlesion functional plasticity in the adult CNS. Here, we show that postsynaptic H1 receptor in the medial vestibular nucleus (MVN) contributes greatly to the recovery of both static and dynamic symptoms following unilateral vestibular lesion. H1 receptor selectively mediates the asymmetric activation of commissural inhibitory system in the ipsilesional MVN and actively promotes vestibular compensation. The findings provide not only a new insight into the postlesion neuronal circuit plasticity and functional recovery of CNS, but also a novel potential therapeutic target for promoting vestibular compensation and ameliorating vestibular disorders.

Iodine-Catalyzed C-H Amidation and Imination at the 2α-Position of 2,3-Disubstituted Indoles with Chloramine Salts.

A novel iodine-catalyzed amidation and imination at the 2α-position of 2,3-disubstituted indoles in the presence of chloramine salts with high regioselectivity has been achieved. The protocol is applicable to a wide range of substrates to deliver the corresponding 2α-nitrogen-containing indole derivatives. Furthermore, to demonstrate the synthetic value of this established transformation, a concise assembly of the bridged tetracyclic framework of akuammiline alkaloids from the 2α-amidated product has been accomplished in five steps.

Iodine-catalyzed oxidative annulation of 3-cyanoacetylindoles with benzylamines: facile access to 5-(3-indolyl)oxazoles.

An iodine-catalyzed oxidative annulation of 3-cyanoacetylindoles with benzylamines has been developed. This reaction enables the convenient synthesis of a variety of 5-(3-indolyl)oxazoles under mild conditions with broad functional group compatibility.

Large valley polarization in monolayer MoTe2 on a magnetic substrate.

On the basis of valley degree of freedom, there would be immense potential application in valleytronics. Introducing magnetism into triangular or hexagonal lattices is a promising route to realize valley polarization, which is indispensable for applying the valley degree of freedom. In this study, we explored valley polarization by depositing a heterostructure of a MoTe2 monolayer on the (0 0 1) surface of an antiferromagnetic RbMnCl3 substrate. First principles-calculations showed that due to proximity-induced Zeeman effects, the MoTe2 monolayer was drastically magnetized by the topmost Mn layer in the substrate and a very large valley splitting (about 109 meV) was achieved. Using an effective Hamiltonian model, the effect of the competition of the spin-orbit coupling (SOC) and exchange field in the system on the valley polarization was also investigated. The magnitude of the valley splitting was found to be limited by the smaller SOC value and the induced exchange field, providing information on the enhancement of the valley polarization. A device rudiment with an anomalous valley Hall effect is proposed.

Direct 3D Analyses Reveal Barrel-Specific Vascular Distribution and Cross-Barrel Branching in the Mouse Barrel Cortex.

Whether vascular distribution is spatially specific among cortical columns is a fundamental yet controversial question. Here, we have obtained 1-µm resolution 3D datasets that cover the whole mouse barrel cortex by combining Nissl staining with micro-optical sectioning tomography to simultaneously visualize individual cells and blood vessels, including capillaries. Pinpointing layer IV of the posteromedial barrel subfield, direct 3D reconstruction and quantitative analysis showed that (1) penetrating vessels preferentially locate in the interbarrel septa/barrel wall (75.1%) rather than the barrel hollows, (2) the branches of 70% penetrating vessels only reach the neighboring but not always all the neighboring barrels and the other 30% extend beyond the neighboring barrels and may provide cross-barrel blood supply or drainage, (3) the branches of 59.6% penetrating vessels reach all the neighboring barrels, while the rest only reach part of them, and (4) the length density of microvessels in the interbarrel septa/barrel wall is lower than that in the barrel hollows with a ratio of 0.92. These results reveal that the penetrating vessels and microvessels exhibit a barrel-specific organization, whereas the branches of penetrating vessels do not, which suggests a much more complex vascular distribution pattern among cortical columns than previously thought.

Quantum Spin-Quantum Anomalous Hall Insulators and Topological Transitions in Functionalized Sb(111) Monolayers.

Electronic and topological behaviors of Sb(111) monolayers decorated with H and certain magnetic atoms are investigated by using ab initio methods. The drastic exchange field induced by the magnetic atoms, together with strong spin-orbit coupling (SOC) of Sb atoms, generates one new category of valley polarized topological insulators, called quantum spin-quantum anomalous Hall (QSQAH) insulators in the monolayer, with a band gap up to 53 meV. The strong SOC is closely related to Sb px and py orbitals, instead of pz orbitals in usual two-dimensional (2D) materials. Topological transitions from quantum anomalous Hall states to QSQAH states and then to time-reversal-symmetry-broken quantum spin Hall states are achieved by tuning the SOC strength. The behind mechanism is revealed. Our work is helpful for future valleytronic and spintronic applications in 2D materials.

Nanoparticle Superlattices as Efficient Bifunctional Electrocatalysts for Water Splitting.

The solar-driven water splitting process is highly attractive for alternative energy utilization, while developing efficient, earth-abundant, bifunctional catalysts for both oxygen evolution reaction and hydrogen evolution reaction has remained as a major challenge. Herein, we develop an ordered CoMnO@CN superlattice structure as an efficient bifunctional water-splitting electrocatalyst, in which uniform Co-Mn oxide (CoMnO) nanoparticles are coated with a thin, continuous nitrogen-doped carbon (CN) framework. The CoMnO nanoparticles enable optimized OER activity with effective electronic structure configuration, and the CN framework serves as an excellent HER catalyst. Importantly, the ordered superlattice structure is beneficial for enhanced reactive sites, efficient charge transfer, and structural stability. This bifunctional superlattice catalyst manifests optimized current densities and electrochemical stability in overall water splitting, outperforming most of the previously reported single- or bifunctional electrocatalysts. Combining with a silicon photovoltaic cell, this CoMnO@CN superlattice bifunctional catalyst enables unassisted solar water splitting continuously for ∼5 days with a solar-to-hydrogen conversion efficiency of ∼8.0%. Our discovery suggests that these transition metal oxide-based superlattices may serve as a unique structure modality for efficient bifunctional water splitting electrocatalysts with scale-up potentials.

3D BrainCV: simultaneous visualization and analysis of cells and capillaries in a whole mouse brain with one-micron voxel resolution.

Systematic cellular and vascular configurations are essential for understanding fundamental brain anatomy and metabolism. We demonstrated a 3D brainwide cellular and vascular (called 3D BrainCV) visualization and quantitative protocol for a whole mouse brain. We developed a modified Nissl staining method that quickly labeled the cells and blood vessels simultaneously in an entire mouse brain. Terabytes 3D datasets of the whole mouse brains, with unprecedented details of both individual cells and blood vessels, including capillaries, were simultaneously imaged at 1-µm voxel resolution using micro-optical sectioning tomography (MOST). For quantitative analysis, we proposed an automatic image-processing pipeline to perform brainwide vectorization and analysis of cells and blood vessels. Six representative brain regions from the cortex to the deep, including FrA, M1, PMBSF, V1, striatum, and amygdala, and six parameters, including cell number density, vascular length density, fractional vascular volume, distance from the cells to the nearest microvessel, microvascular length density, and fractional microvascular volume, had been quantitatively analyzed. The results showed that the proximity of cells to blood vessels was linearly correlated with vascular length density, rather than the cell number density. The 3D BrainCV made overall snapshots of the detailed picture of the whole brain architecture, which could be beneficial for the state comparison of the developing and diseased brain.

Reversible chemical tuning of charge carriers for enhanced photoelectrochemical conversion and probing of living cells.

A facile, solution method for reversible tuning of oxygen vacancies inside TiO2 nanowires, in which the reducing treatment of TiO2 by NaBH4 leads to 2.4-fold increase of photocurrent density, compared to pristine TiO2 nanowires, is reported. Subsequent oxidizing treatment using KMnO4 or annealing in air can reset the photocurrent density to the original values. The incident photo-to-current conversion efficiency measurement exhibits that the reduced TiO2 nanowires present both enhanced photoactivity in both UV and visible regions. Density functional theory calculations reveal that the oxygen vacancies in the reduced TiO2 cause defect states in the band structure and result in enhanced carrier density and conductivity. In addition, the enhanced solar energy-driven photoelectrochemical conversion allows real-time, sensitive chemical probing of living cells that are directly grown on the TiO2 nanowire photoanodes. As proofs-of-concept, after functionalized with horseradish peroxidase (HRP) on the surface, the reduced TiO2 NWs demonstrate sensitive, real-time monitoring of the H2O2 levels in several distinctive living cell lines, with the lowest detectable H2O2 concentration of 7.7 nM. This reversible tuning of oxygen vacancies suggests a facile means for transition metal oxides, with enhanced photoconversion activity and electrochemical sensitivity.

Spin-dependent thermoelectronic transport of a single molecule magnet Mn(dmit)2.

We investigate spin-dependent thermoelectronic transport properties of a single molecule magnet Mn(dmit)2 sandwiched between two Au electrodes using first-principles density functional theory combined with nonequilibrium Green's function method. By applying a temperature difference between the two Au electrodes, spin-up and spin-down currents flowing in opposite directions can be induced due to asymmetric distribution of the spin-up and spin-down transmission spectra around the Fermi level. A pure spin current and 100% spin polarization are achieved by tuning back-gate voltage to the system. The spin caloritronics of the molecule with a perpendicular conformation is also explored, where the spin-down current is blocked strongly. These results suggest that Mn(dmit)2 is a promising material for spin caloritronic applications.

Quantum valley Hall states and topological transitions in Pt(Ni, Pd)-decorated silicene: a first-principles study.

The electronic states and topological behaviors of Pt(Ni, Pd)-decorated silicene are investigated by using an ab-initio method. All the three kinds of the adatoms prefer hollow sites of the silicene, guaranteeing the Dirac cones unbroken. The Pt(Ni, Pd)-decorated silicene systems all present quantum valley Hall (QVH) states with the gap opened exactly at the Fermi level. The gaps of the QVH states can be increased substantially by applying a positive electric field. Very fascinating phase transitions from QVH to quantum spin Hall (QSH) and then to QVH again are achieved in the Pt/Ni-decorated silicene when a negative electric field is applied. The QSH state in the Pd case with a negative electric field is, however, quenched because of relatively larger Rashba spin-orbit coupling (SOC) than the intrinsic SOC in the system. Our findings may be useful for the applications of silicene-based devices in valleytronics and spintronics.

Continuously tracing brain-wide long-distance axonal projections in mice at a one-micron voxel resolution.

Revealing neural circuit mechanisms is critical for understanding brain functions. Significant progress in dissecting neural connections has been made using optical imaging with fluorescence labels, especially in dissecting local connections. However, acquiring and tracing brain-wide, long-distance neural circuits at the neurite level remains a substantial challenge. Here, we describe a whole-brain approach to systematically obtaining continuous neuronal pathways in a fluorescent protein transgenic mouse at a one-micron voxel resolution. This goal is achieved by combining a novel resin-embedding method for maintaining fluorescence, an automated fluorescence micro-optical sectioning tomography system for long-term stable imaging, and a digital reconstruction-registration-annotation pipeline for tracing the axonal pathways in the mouse brain. With the unprecedented ability to image a whole mouse brain at a one-micron voxel resolution, the long-distance pathways were traced minutely and without interruption for the first time. With advancing labeling techniques, our method is believed to open an avenue to exploring both local and long-distance neural circuits that are related to brain functions and brain diseases down to the neurite level.

Strain-induced orbital polarization and multiple phase transitions in Ba2MnWO6 from first principles.

Electronic structures of double perovskite Ba2MnWO6 with epitaxial strain are explored by using methods based on density functional theory. An in-plane compressive strain is found not only resulting in a semiconductor-metal transition (SMT), but also altering the magnetic structures, from different kinds of antiferromagnetic to ferromagnetic orders. Orbital polarization and different orbital occupancies of Mn d(z(2)) and d(x(2)-y(2)) states, induced by the epitaxial strain, are employed to understand the SMT. The rich magnetic phase transitions are rationalized by a magnetic stabilization mechanism. Our results show that many technological applications may be carried out in the material with the control of epitaxial strain.

Large-band-gap non-Dirac quantum spin Hall states and strong Rashba effect in functionalized thallene films.

The quantum spin Hall state materials have recently attracted much attention owing to their potential applications in the design of spintronic devices. Based on density functional theory calculations and crystal field theory, we study electronic structures and topological properties of functionalized thallene films. Two different hydrogenation styles (Tl2H and Tl2H2) are considered, which can drastically vary the electronic and topological behaviors of the thallene. Due to the C3v symmetry of the two systems, the px and py orbitals at the Γ point have the non-Dirac band degeneracy. With spin-orbit coupling (SOC), topological nontrivial band gaps can be generated, giving rise to non-Dirac quantum spin Hall states in the two thallium hydride films. The nontrivial band gap for the monolayer Tl2H is very large (855 meV) due to the large on-site SOC of Tl px and py orbitals. The band gap in Tl2H2 is, however, small due to the band inversion between the Tl px/y and pz orbitals. It is worth noting that both the Tl2H and Tl2H2 monolayers exhibit strong Rashba spin splitting effects, especially for the monolayer Tl2H2 (αR = 2.52 eVÅ), rationalized well by the breaking of the structural inversion symmetry. The Rashba effect can be tuned sensitively by applying biaxial strain and external electric fields. Our findings provide an ideal platform for fabricating room-temperature spintronic and topological electronic devices.

Modification on Flower Defects and Electronic Properties of Epitaxial Graphene by Erbium.

Manipulating the topological defects and electronic properties of graphene has been a subject of great interest. In this work, we have investigated the influence of Er predeposition on flower defects and electronic band structures of epitaxial graphene on SiC. It is shown that Er atoms grown on the SiC substrate actually work as an activator to induce flower defect formation with a density of 1.52 × 1012 cm-2 during the graphitization process when the Er coverage is 1.6 ML, about 5 times as much as that of pristine graphene. First-principles calculations demonstrate that Er greatly decreases the formation energy of the flower defect. We have discussed Er promoting effects on flower defect formation as well as its formation mechanism. Scanning tunneling microscopy (STM) and Raman and X-ray photoelectron spectroscopy (XPS) have been utilized to reveal the Er doping effect and its modification to electronic structures of graphene. N-doping enhancement and band gap opening can be observed by using angle-resolved photoemission spectroscopy (ARPES). With Er coverage increasing from 0 to 1.6 ML, the Dirac point energy decreases from -0.34 to -0.37 eV and the band gap gradually increases from 320 to 360 meV. The opening of the band gap is attributed to the synergistic effect of substitution doping of Er atoms and high-density flower defects.

Improving electronic transport of zigzag graphene nanoribbons by ordered doping of B or N atoms.

Using an ab initio method, we explored electronic structures and transport properties of zigzag graphene nanoribbons (ZGNRs) with ordered doping of B or N atoms. We find B or N atoms doping can increase significantly the conductance of the ZGNRs with an even number of zigzag chains due to additional conducting channels being induced and the breakdown of parity limitation. The higher the doping concentration, the larger the current amplification factor obtained. For the nanojunctions with one row B (or N) atoms, the current amplification factor can be larger when the doping position is near to the center, while for the junction with two rows, the trend is subtle due to the interactions between the two rows of B (or N) atoms. Negative differential resistive phenomena are found for the case of B doping at low concentrations and the case for N doping. The conductance of the ZGNR with odd numbers of zigzag chains can also be increased by doping of B or N atoms. More interestingly, the B or N doping can almost completely remove the even-odd effect on electronic transport of the ZGNRs. Our studies provide avenues to drastically improve the electronic transport of ZGNRs, helpful for graphene applications.

Anisotropy-induced phase transitions in an intrinsic half-Chern insulator Ni2I2.

One crucial target of research on spintronics is to achieve flexibly tunable and highly efficient spin-polarized electronic current. In this work, by using first-principles calculations and topological characterization theories, we propose an intrinsic half-Chern insulator (HCI) in a Ni2I2 monolayer, which possesses 100% spin-polarized topologically nontrivial edge states, distinct from ordinary Chern insulators. Its band gap is formed due to the lifting of the double degeneracy of non-Dirac bands composed of Ni dxz/dyz orbitals. The HCI becomes a half semiconductor (HS) or a combined state of a half metal (HM) and an HCI if biaxial strain is applied. The phase transition is found to be associated with the unique anisotropy of the bands, originating from the diverse orbital distributions and the opposite moving in energy of Ni dxy and dxz/dyz bands under the strain. Our findings demonstrate that the monolayer Ni2I2 is a unique Chern insulator with ideal spintronic properties, supporting versatile applications in spintronic devices with very high spin polarization and extremely low-power dissipation.