Computational Study on Interlocked-Ferroelectricity-Contributed High-Performance Memristors Based on Two-Dimensional van der Waals Ferroelectric Semiconductors.

In order to realize the prevailing artificial intelligence technology, memristor-implemented in-memory or neuromorphic computing is highly expected to break the bottleneck of von Neumann computers. Although high-performance memristors have been vigorously developed in labs or in industry, systematic computational investigations on memristors are seldom. Hence, it is urgent to provide theoretical or computational support for the exploration of memristor operating mechanisms or the screening of memristor materials. Here, a computational method based on the main input parameters learned from the first-principles calculations was developed to measure resistance switching of two-terminal memristors with sandwiched metal/ferroelectric semiconductor/metal architectures, which strikingly agrees with the experimental measurements. Based on our developed method, the diverse multiterminal memristors were designed to fully exploit the application of interlocked ferroelectricity of a ferroelectric semiconductor and realize their heterosynaptic plasticity, and their heterosynaptic behaviors can still be well described. Our developed method can provide a paradigm for the emulation of ferroelectric memristors and inspire subsequent computational exploration. Furthermore, our study also supplies a device optimization strategy based on the interlocked ferroelectricity and easy processing of two-dimensional van der Waals ferroelectric semiconductors, and our proposed heterosynaptic memristors still await further experimental exploration.

A Superconducting Micro-Magnetometer for Quantum Vortex in Superconducting Nanoflakes.

Superconducting quantum interferometer device (SQUID) plays a key role in understanding electromagnetic properties and emergent phenomena in quantum materials. The technological appeal of SQUID is that its detection accuracy for the electromagnetic signal can precisely reach the quantum level of a single magnetic flux. However, conventional SQUID techniques normally can only be applied to a bulky sample and do not have the capability to probe the magnetic properties of micro-scale samples with small magnetic signals. Herein, it is demonstrated that, based on a specially designed superconducting nano-hole array, the contactless detection of magnetic properties and quantized vortices in micro-sized superconducting nanoflakes is realized. An anomalous hysteresis loop and a suppression of Little-Parks oscillation are observed in the detected magnetoresistance signal, which originates from the disordered distribution of the pinned vortices in Bi2 Sr2 CaCu2 O8+δ . Therefore, the density of pinning centers of the quantized vortices on such micro-sized superconducting samples can be quantitatively evaluated, which is technically inaccessible for conventional SQUID detection. The superconducting micro-magnetometer provides a new approach to exploring mesoscopic electromagnetic phenomena of quantum materials.

High-harmonic generation in Weyl semimetal ß-WP2 crystals.

As a quantum material, Weyl semimetal has a series of electronic-band-structure features, including Weyl points with left and right chirality and corresponding Berry curvature, which have been observed in experiments. These band-structure features also lead to some unique nonlinear properties, especially high-order harmonic generation (HHG) due to the dynamic process of electrons under strong laser excitation, which has remained unexplored previously. Herein, we obtain effective HHG in type-II Weyl semimetal ß-WP2 crystals, where both odd and even orders are observed, with spectra extending into the vacuum ultraviolet region (190 nm, 10th order), even under fairly low femtosecond laser intensity. In-depth studies have interpreted that odd-order harmonics come from the Bloch electron oscillation, while even orders are attributed to Bloch oscillations under the "spike-like" Berry curvature at Weyl points. With crystallographic orientation-dependent HHG spectra, we further quantitatively retrieved the electronic band structure and Berry curvature of ß-WP2. These findings may open the door for exploiting metallic/semimetallic states as solid platforms for deep ultraviolet radiation and offer an all-optical and pragmatic solution to characterize the complicated multiband electronic structure and Berry curvature of quantum topological materials.

Direct Growth of van der Waals Tin Diiodide Monolayers.

Two-dimensional (2D) van der Waals (vdW) materials have garnered considerable attention for their unique properties and potentials in a wide range of fields, which include nano-electronics/optoelectronics, solar energy, and catalysis. Meanwhile, challenges in the approaches toward achieving high-performance devices still inspire the search for new 2D vdW materials with precious properties. In this study, via molecular beam epitaxy, for the first time, the vdW SnI2 monolayer is successfully fabricated with a new structure. Scanning tunneling microscopy/spectroscopy characterization, as corroborated by the density functional theory calculation, indicates that this SnI2 monolayer exhibits a band gap of ≈2.9 eV in the visible purple range, and an indirect- to direct-band gap transition occurs in the SnI2 bilayer. This study provides a new semiconducting 2D material that is promising as a building block in future electronics/optoelectronics.

Non-hydrostatic pressure-dependent structural and transport properties of BiCuSeO and BiCuSO single crystals.

High-pressure experiments usually expect a hydrostatic condition, in which the physical properties of materials can be easily understood by theoretical simulations. Unfortunately, non-hydrostatic effect is inevitable in experiments due to the solidification of the pressure transmitting media under high pressure. Resultantly, non-hydrostaticity affects the accuracy of the experimental data and sometimes even leads to false phenomena. Since the non-hydrostatic effect is extrinsic, it is quite hard to analyze quantitatively. Here, we have conducted high pressure experiments on the layered BiCuXO (X = S and Se) single crystals and quantitatively analyzed their pronounced non-hydrostatic effect by high throughput first-principles calculations and experimental Raman spectra. Our experiments find that the BiCuXO single crystals sustain the tetragonal structure up to 55 GPa (maximum pressure in our experiment). However, their pressure-dependent Raman shift and electric resistance show anomalous behaviors. Through optimization of thousands of crystal structures in the high throughput first-principles calculations, we have obtained the evolution of the lattice constants under external pressures, which clearly substantiates the non-hydrostatical pressure exerted in BiCuXO crystals. Our work indicates that the high throughput first-principles calculations could be a handy method to investigate the non-hydrostatic effect on the structural and electronic properties of materials in high pressure experiments.

Kinetics-Limited Two-Step Growth of van der Waals Puckered Honeycomb Sb Monolayer.

Puckered honeycomb Sb monolayer, the structural analog of black phosphorene, has been recently successfully grown by means of molecular beam epitaxy. However, little is known to date about the growth mechanism for such a puckered honeycomb monolayer. In this study, by using scanning tunneling microscopy in combination with first-principles density functional theory calculations, we unveil that the puckered honeycomb Sb monolayer takes a kinetics-limited two-step growth mode. As the coverage of Sb increases, the Sb atoms first form the distorted hexagonal lattice as the half layer, and then the distorted hexagonal half-layer transforms into the puckered honeycomb lattice as the full layer. These results provide the atomic-scale insight in understanding the growth mechanism of puckered honeycomb monolayer and can be instructive to the direct growth of other monolayers with the same structure.

Tuning the Electronic Structure of an α-Antimonene Monolayer through Interface Engineering.

The interfacial charge transfer from the substrate may influence the electronic structure of the epitaxial van der Waals (vdW) monolayers and, thus, their further technological applications. For instance, the freestanding Sb monolayer in the puckered honeycomb phase (α-antimonene), the structural analogue of black phosphorene, was predicted to be a semiconductor, but the epitaxial one behaves as a gapless semimetal when grown on the Td-WTe2 substrate. Here, we demonstrate that interface engineering can be applied to tune the interfacial charge transfer and, thus, the electron band of the epitaxial monolayer. As a result, the nearly freestanding (semiconducting) α-antimonene monolayer with a band gap of ∼170 meV was successfully obtained on the SnSe substrate. Furthermore, a semiconductor-semimetal crossover is observed in the bilayer α-antimonene. This study paves the way toward modifying the electron structure in two-dimensional vdW materials through interface engineering.

Electrical scattering mechanism evolution in un-doped and halogen-doped Bi2O2Se single crystals.

Recently the layered oxide semiconductor Bi2O2Se was hotly explored for its ultrahigh mobility and ultrafast photo-response whose physical origins need to be further explored or elucidated. Here, we have grown halogen (Cl, Br, I) doped and un-doped Bi2O2Se single crystals by a melt-solidification method. Comparative electrical transport characterizations and detailed data-analysis substantiate that the electron-electron scattering is the major source of resistivity in un-doped Bi2O2Se crystals; however, in halogen-doped Bi2O2Se crystals, electron-electron scattering is only effective at low temperature (<60 K) and subsequently electron-phonon-interaction scattering is dominated to resistivity. Hall measurement and analysis show that electron concentration of halogen-doped Bi2O2Se (∼1020 cm-3) is one-order higher than un-doped one (∼1019 cm-3), but the carrier mobility of halogen-doped Bi2O2Se at 2 K (∼102 cm2 V-1 s-1) is reduced by more than two orders than un-doped ones (∼104 cm2 V-1 s-1). Three kinds of relaxation time (due to the impurity scattering, electron-electron scattering and electron-phonon scattering), calculated by linear-response theory and electron-/phonon-dispersion, are in agreement with experimental results quantitatively. The scattering mechanism evolution from sole electron-electron scattering (un-doped Bi2O2Se) to electron-phonon scattering (doped Bi2O2Se) at high temperature (>60 K) is attributed to the net effect of decreased screened Coulomb-interaction and increased Fermi energy in halogen-doped Bi2O2Se. This work may provide clues of physical origins of superior electrical/photoelectrical properties of Bi2O2Se.

Synthesis, structure, and electronic properties of the Li11RbGd4Te6O30 single crystal.

Materials with spin dimers have attracted much attention in the last several decades because they could provide a playground to embody simple quantum spin models. For example, the Bose-Einstein condensation of magnons has been observed in TlCuCl3 with anti-ferromagnetic Cu2Cl6 dimers. In this work, we have synthesized a new kind of single-crystal Li11RbGd4Te6O30 with Gd2O15 dimers. This material belongs to the rhombohedral system with the lattice parameters: a = b = c = 16.0948 Å and α = ß = γ = 33.74°. First-principles calculations indicate that Li11RbGd4Te6O30 is a wide-bandgap (about 4.5 eV) semiconductor. But unlike many other well studied quantum dimer magnets with an anti-ferromagnetic ground state, the Gd2O14 dimers in Li11RbGd4Te6O30 show ferromagnetic intra-dimer exchange interactions according to our calculations. Our work provides a new material which could possibly extend the studies of the spin dimers.

Anomalous transport and magnetic properties induced by slight Cu valence alternation in layered oxytelluride BiCuTeO.

In this paper, we report on the transport and magnetic properties of layered oxytelluride BiCuTeO polycrystals with slight mixed valence of Cu. The temperature-dependent electrical resistivity reveals degenerate semiconductor behavior (similar to metals). Under the action of an external magnetic field, the BiCuTeO polycrystal sample exhibits unsaturated magnetic resistance (MR) of about 8% at 2 K and 9 Tesla. The Hall resistivities show nonlinear behavior, suggesting the coexistence of both electrons and holes in the sample. When the temperature is decreased to around 110 K, the dominant carriers are changed from electrons to holes from the viewpoint of electrical transport, which is supported by the calculated temperature-dependent Fermi energy. Meanwhile, at low temperatures (<100 K), the impurity magnetic moment formed by a small amount of positive divalent copper exhibits short-range magnetism (a spin-glass-like feature), which gives rise to a narrow magnetic hysteresis loop. Our work may benefit in-depth understanding of physical properties of BiCuTeO-based materials.

Infrared and Raman spectra of Bi2O2X and Bi2OX2 (X = S, Se, and Te) studied from first principles calculations.

The bismuth oxychalcogenide compounds contain many different kinds of materials, such as Bi2O2X and Bi2OX2 (X = S, Se, and Te). These materials have different but similar layered crystal structures and exhibit various interesting physical properties. Here, we have theoretically investigated their Raman and infrared spectra by first principles calculations based on density functional theory. It is found that in Bi2O2Se the calculated frequency of the A1g Raman active mode is in good agreement with the experimental measurements while the other three modes are ambiguous or not observed yet. The Raman and infrared spectra of other materials are also presented and need further confirmation. Our work provides the structural fingerprints of these materials, which could be helpful in identifying the crystal structures in future experiments.

Van der Waals Heteroepitaxial Growth of Monolayer Sb in a Puckered Honeycomb Structure.

Atomically thin 2D crystals have gained tremendous attention owing to their potential impact on future electronics technologies, as well as the exotic phenomena emerging in these materials. Monolayers of α-phase Sb (α-antimonene), which shares the same puckered structure as black phosphorous, are predicted to be stable with precious properties. However, the experimental realization still remains challenging. Here, high-quality monolayerα-antimonene is successfully grown, with the thickness finely controlled. The α-antimonene exhibits great stability upon exposure to air. Combining scanning tunneling microscopy, density functional theory calculations, and transport measurements, it is found that the electron band crossing the Fermi level exhibits a linear dispersion with a fairly small effective mass, and thus a good electrical conductivity. All of these properties make the α-antimonene promising for future electronic applications.

Superconductivity in Potassium-Intercalated T d-WTe2.

To realize a topological superconductor is one of the most attracting topics because of its great potential in quantum computation. In this study, we successfully intercalate potassium (K) into the van der Waals gap of type II Weyl semimetal WTe2 and discover the superconducting state in K xWTe2 through both electrical transport and scanning tunneling spectroscopy measurements. The superconductivity exhibits an evident anisotropic behavior. Moreover, we also uncover the coexistence of superconductivity and the positive magnetoresistance state. Structural analysis substantiates the negligible lattice expansion induced by the intercalation, therefore suggesting K-intercalated WTe2 still hosts the topological nontrivial state. These results indicate that the K-intercalated WTe2 may be a promising candidate to explore the topological superconductor.

Preparation, Structure Evolution, and Metal-Insulator Transition of Na xRhO2 Crystals (0.25 ≤ x ≤ 1).

The triangular lattice Na xRhO2 contains a 4d Rh element with large spin-orbit coupling, and the electron-electron correlation effect is expected to have some novel physical properties. Here we report NaRhO2 crystal growth by Na2CO3 vapor growth and a series of Na xRhO2 (0.25 ≤ x ≤ 1) crystals prepared using the chemical desodiation method. Na xRhO2 reveals a layer structure with the space group R3̅ m, and the lattice parameter a evolves from 3.09 to 3.03 Å and c from 15.54 to 15.62 Å when x decreases from 1.0 to 0.2. Decreasing potassium concentration leads to a contraction of the RhO6 octahedral layers, which may be attributed to a higher covalency of Rh-O bonds. More important, the metal-insulator transition in Na xRhO2 was observed in resistivity along the ab plane. The conducting mechanism of Na xRhO2 is strongly dependent on x. Two-dimensional variable range hopping (VRH) mechanisms (0.67 ≤ x ≤ 1) and metallic behaviors (0.42 and 0.47) are observed in temperature-dependent resistivity. The origin of this metal-insulator transition was discussed on the basis of the Ioffe-Regel criterion. Our work demonstrates the strong correlation between sodium concentration and physical properties of Na xRhO2.

Nematic superconducting state in iron pnictide superconductors.

Nematic order often breaks the tetragonal symmetry of iron-based superconductors. It arises from regular structural transition or electronic instability in the normal phase. Here, we report the observation of a nematic superconducting state, by measuring the angular dependence of the in-plane and out-of-plane magnetoresistivity of Ba0.5K0.5Fe2As2 single crystals. We find large twofold oscillations in the vicinity of the superconducting transition, when the direction of applied magnetic field is rotated within the basal plane. To avoid the influences from sample geometry or current flow direction, the sample was designed as Corbino-shape for in-plane and mesa-shape for out-of-plane measurements. Theoretical analysis shows that the nematic superconductivity arises from the weak mixture of the quasi-degenerate s-wave and d-wave components of the superconducting condensate, most probably induced by a weak anisotropy of stresses inherent to single crystals.

The Microstructural Characterization of Multiferroic LaFeO3-YMnO3 Multilayers Grown on (001)- and (111)-SrTiO3 Substrates by Transmission Electron Microscopy.

The microstructure of multiferroic LaFeO3-YMnO3 (LFO-YMO) multilayers grown on (001)- and (111)-SrTiO3 substrates is characterized by the transmission electron microscopy (TEM). Detailed TEM characterization reveals that LFO-YMO multilayers grown on both substrates have clear layer-by-layer morphology and distinct chemical-composition layered structure. The most notable feature is that LFO-YMO multilayers grown on (001)-SrTiO3 substrate have three types of domains, while those on (111)-SrTiO3 have only one. The multi-/twin- domain structure can be qualitatively explained by the lattice mismatch in this system. The details of the domain structure of LFO-YMO multilayers are crucial to understanding their magnetic properties.

Composition and temperature-dependent phase transition in miscible Mo1-xWxTe2 single crystals.

Transition metal dichalcogenides (TMDs) WTe2 and MoTe2 with orthorhombic Td phase, being potential candidates as type-II Weyl semimetals, are attracted much attention recently. Here we synthesized a series of miscible Mo1-xWxTe2 single crystals by bromine vapor transport method. Composition-dependent X-ray diffraction and Raman spectroscopy, as well as composition and temperature-dependent resistivity prove that the tunable crystal structure (from hexagonal (2H), monoclinic (ß) to orthorhombic (Td) phase) can be realized by increasing W content in Mo1-xWxTe2. Simultaneously the electrical property gradually evolves from semiconductor to semimetal behavior. Temperature-dependent Raman spectroscopy proves that temperature also can induce the structural phase transition from ß to Td phase in Mo1-xWxTe2 crystals. Based on aforementioned characterizations, we map out the temperature and composition dependent phase diagram of Mo1-xWxTe2 system. In addition, a series of electrical parameters, such as carrier type, carrier concentration and mobility, have also been presented. This work offers a scheme to accurately control structural phase in Mo1-xWxTe2 system, which can be used to explore type-II Weyl semimetal, as well as temperature/composition controlled topological phase transition therein.

Experimental Observation of Anisotropic Adler-Bell-Jackiw Anomaly in Type-II Weyl Semimetal WTe_{1.98} Crystals at the Quasiclassical Regime.

The asymmetric electron dispersion in type-II Weyl semimetal theoretically hosts anisotropic transport properties. Here, we observe the significant anisotropic Adler-Bell-Jackiw (ABJ) anomaly in the Fermi-level delicately adjusted WTe_{1.98} crystals. Quantitatively, C_{W}, a coefficient representing the intensity of the ABJ anomaly along the a and b axis of WTe_{1.98} are 0.030 and 0.051 T^{-2} at 2 K, respectively. We found that the temperature-sensitive ABJ anomaly is attributed to a topological phase transition from a type-II Weyl semimetal to a trivial semimetal, which is verified by a first-principles calculation using experimentally determined lattice parameters at different temperatures. Theoretical electrical transport study reveals that the observation of an anisotropic ABJ along both the a and b axes in WTe_{1.98} is attributed to electrical transport in the quasiclassical regime. Our work may suggest that electron-doped WTe_{2} is an ideal playground to explore the novel properties in type-II Weyl semimetals.

Transcutaneous electrical acupoint stimulation as an adjunct therapy for obsessive-compulsive disorder: A randomized controlled study.

BACKGROUND: Transcutaneous electrical acupoint stimulation (TEAS) is thought to have potential to treat obsessive-compulsive disorder (OCD). OBJECTIVE: The purpose of this study was to determine whether adding TEAS to cognitive behavioral therapy (CBT) and clomipramine would improve the efficacy of these conventional treatments in OCD. METHODS: In this randomized controlled trial, 360 OCD patients were assigned to receive TEAS combined with CBT plus clomipramine (Group A, n = 120), TEAS combined with CBT plus placebo (Group B, n = 120), and simulated (placebo) TEAS combined with CBT plus clomipramine (Group C, n = 120) for 12 weeks. The primary outcome was measured using the Yale-Brown Obsessive-Compulsive Scale (Y-BOCS). RESULTS: OCD symptoms in all patients reduced over time, however Groups A and B had a significantly greater reduction in Y-BOCS total score and the subscale for obsession and compulsion between week 2 and week 12 compared to Group C. Groups A and B had similar scores on these measures. Both groups had significantly higher rates of clinical response than Group C (88.3% and 81.7% vs. 67.5%, respectively, p < 0.001); and higher rates of remission (30.0% and 22.5% vs. 9.2%, respectively, p < 0.001). Group B experienced fewer adverse events than the other two groups. CONCLUSIONS: TEAS enhances the efficacy of conventional OCD interventions and avoids the adverse effects associated with conventional pharmacological treatment. It can be considered as an effective adjunct intervention for OCD.

Experimental Observation of Topological Edge States at the Surface Step Edge of the Topological Insulator ZrTe_{5}.

We report an atomic-scale characterization of ZrTe_{5} by using scanning tunneling microscopy. We observe a bulk band gap of ∼80 meV with topological edge states at the step edge and, thus, demonstrate that ZrTe_{5} is a two-dimensional topological insulator. We also find that an applied magnetic field induces an energetic splitting of the topological edge states, which can be attributed to a strong link between the topological edge states and bulk topology. The relatively large band gap makes ZrTe_{5} a potential candidate for future fundamental studies and device applications.