Spin-Lattice Coupled Metamagnetism in Frustrated van der Waals Magnet CrOCl.

The long-range magnetic ordering in frustrated magnetic systems is stabilized by coupling magnetic moments to various degrees of freedom, for example, by enhancing magnetic anisotropy via lattice distortion. Here, the unconventional spin-lattice coupled metamagnetic properties of atomically-thin CrOCl, a van der Waals antiferromagnet with inherent magnetic frustration rooted in the staggered square lattice, are reported. Using temperature- and angle-dependent tunneling magnetoconductance (TMC), in complementary with magnetic torque and first-principles calculations, the antiferromagnetic (AFM)-to-ferrimagnetic (FiM) metamagnetic transitions (MTs) of few-layer CrOCl are revealed to be triggered by collective magnetic moment flipping rather than the established spin-flop mechanism, when external magnetic field (H) enforces a lattice reconstruction interlocked with the five-fold periodicity of the FiM phase. The spin-lattice coupled MTs are manifested by drastic jumps in TMC, which show anomalous upshifts at the transition thresholds and persist much higher above the AFM Néel temperature. While the MTs exhibit distinctive triaxial anisotropy, reflecting divergent magnetocrystalline anisotropy of the c-axis AFM ground state, the resulting FiM phase has an a-c easy plane in which the magnetization axis is freely rotated by H. At the 2D limit, such a field-tunable FiM phase may provide unique opportunities to explore exotic emergent phenomena and novel spintronics devices.

Two-dimensional superconductivity at the surfaces of KTaO3 gated with ionic liquid.

The recent discovery of superconductivity at the interfaces between KTaO3 and EuO (or LaAlO3) gives birth to the second generation of oxide interface superconductors. This superconductivity exhibits a strong dependence on the surface plane of KTaO3, in contrast to the seminal LaAlO3/SrTiO3 interface, and the superconducting transition temperature Tc is enhanced by one order of magnitude. For understanding its nature, a crucial issue arises: Is the formation of oxide interfaces indispensable for the occurrence of superconductivity? Exploiting ionic liquid (IL) gating, we are successful in achieving superconductivity at KTaO3(111) and KTaO3(110) surfaces with Tc up to 2.0 and 1.0 K, respectively. This oxide-IL interface superconductivity provides a clear evidence that the essential physics of KTaO3 interface superconductivity lies in the KTaO3 surfaces doped with electrons. Moreover, the controllability with IL technique paves the way for studying the intrinsic superconductivity in KTaO3.

Commensurate Stacking Phase Transitions in an Intercalated Transition Metal Dichalcogenide.

Intercalation and stacking-order modulation are two active ways in manipulating the interlayer interaction of transition metal dichalcogenides (TMDCs), which lead to a variety of emergent phases and allow for engineering material properties. Herein, the growth of Pb-intercalated TMDCs-Pb(Ta1+x Se2 )2 , the first 124-phase, is reported. Pb(Ta1+x Se2 )2 exhibits a unique two-step first-order structural phase transition at around 230 K. The transitions are solely associated with the stacking degree of freedom, evolving from a high-temperature (high-T) phase with ABC stacking and R3m symmetry to an intermediate phase with AB stacking and P3m1, and finally to a low-temperature (low-T) phase again with R3msymmetry, but with ACB stacking. Each step involves a rigid slide of building blocks by a vector [1/3, 2/3, 0]. Intriguingly, gigantic lattice contractions occur at the transitions on warming. At low-T, bulk superconductivity with Tc  ≈ 1.8 K is observed. The underlying physics of the structural phase transitions are discussed from first-principle calculations. The symmetry analysis reveals topological nodal lines in the band structure. The results demonstrate the possibility of realizing higher-order metal-intercalated phases of TMDCs and advance the knowledge of polymorphic transitions, and may inspire stacking-order engineering in TMDCs and beyond.

Van der Waals Antiferroelectric Magnetic Tunnel Junction: A First-Principles Study of a CrSe2/CuInP2S6/CrSe2 Junction.

Magnetic tunnel junctions (MTJs), ferroelectric/antiferroelectric tunnel junctions (FTJs/AFTJs), and multiferroic tunnel junctions (MFTJs) have recently attracted significant interest for technological applications of nanoscale memory devices. Until now, most of them are based on perovskite oxide heterostructures with a relatively high resistance-area (RA) product and low resistance difference unfavorable for practical applications. The recent discovery of the two-dimensional (2D) van der Waals (vdW) ferroelectric (FE) and magnetic materials has opened a new route to realize tunnel junctions with high performance and atomic-scale dimensions. Here, using first-principles calculations, we propose a new type of 2D tunnel junction: an antiferroelectric magnetic tunnel junction (AFMTJ), which inherits the features of both MTJ and AFTJ. This AFMTJ is composed of monolayer CuInP2S6 (CIPS) sandwiched between 2D magnetic electrodes of CrSe2. The AFTJ with nonmagnetic electrodes of TiSe2 on both sides of CIPS and the asymmetric AFTJ with both CrSe2 and TiSe2 electrodes are also investigated. Based on quantum-mechanical modeling of the electronic transport, sizeable tunneling electroresistance effects and multiple nonvolatile resistance states are demonstrated. More importantly, a remarkably low RA product (less than 0.1 Ω·µm2) makes the proposed vdW AFMTJs superior to the conventional MFTJs in terms of their promising nonvolatile memory applications. Our calculations provide new guidance for the experiment and application of nanoscale memory devices.

Possible Evidence for Berezinskii-Kosterlitz-Thouless Transition in Ba(Fe0.914Co0.086)2As2 Crystals.

In this study, we measure the in-plane transport properties of high-quality Ba(Fe0.914Co0.086)2As2 single crystals. Signatures of vortex unbinding Berezinskii-Kosterlitz-Thouless (BKT) transition are shown from both the conventional approach and the Fisher-Fisher-Huse dynamic scaling analysis, in which a characteristic Nelson-Kosterlitz jump is demonstrated. We also observe a non-Hall transverse signal exactly at the superconducting transition, which is explained in terms of guided motion of unbound vortices.

Discovery of segmented Fermi surface induced by Cooper pair momentum.

A sufficiently large supercurrent can close the energy gap in a superconductor and create gapless quasiparticles through the Doppler shift of quasiparticle energy caused by finite Cooper pair momentum. In this gapless superconducting state, zero-energy quasiparticles reside on a segment of the normal-state Fermi surface, whereas the remaining Fermi surface is still gapped. We use quasiparticle interference to image the field-controlled Fermi surface of bismuth telluride (Bi2Te3) thin films under proximity effect from the superconductor niobium diselenide (NbSe2). A small applied in-plane magnetic field induces a screening supercurrent, which leads to finite-momentum pairing on the topological surface states of Bi2Te3. We identify distinct interference patterns that indicate a gapless superconducting state with a segmented Fermi surface. Our results reveal the strong impact of finite Cooper pair momentum on the quasiparticle spectrum.

Rashba valleys and quantum Hall states in few-layer black arsenic.

Exciting phenomena may emerge in non-centrosymmetric two-dimensional electronic systems when spin-orbit coupling (SOC)1 interplays dynamically with Coulomb interactions2,3, band topology4,5 and external modulating forces6-8. Here we report synergetic effects between SOC and the Stark effect in centrosymmetric few-layer black arsenic, which manifest as particle-hole asymmetric Rashba valley formation and exotic quantum Hall states that are reversibly controlled by electrostatic gating. The unusual findings are rooted in the puckering square lattice of black arsenic, in which heavy 4p orbitals form a Brillouin zone-centred Γ valley with pz symmetry, coexisting with doubly degenerate D valleys of px origin near the time-reversal-invariant momenta of the X points. When a perpendicular electric field breaks the structure inversion symmetry, strong Rashba SOC is activated for the px bands, which produces spin-valley-flavoured D± valleys paired by time-reversal symmetry, whereas Rashba splitting of the Γ valley is constrained by the pz symmetry. Intriguingly, the giant Stark effect shows the same px-orbital selectiveness, collectively shifting the valence band maximum of the D± Rashba valleys to exceed the Γ Rashba top. Such an orchestrating effect allows us to realize gate-tunable Rashba valley manipulations for two-dimensional hole gases, hallmarked by unconventional even-to-odd transitions in quantum Hall states due to the formation of a flavour-dependent Landau level spectrum. For two-dimensional electron gases, the quantization of the Γ Rashba valley is characterized by peculiar density-dependent transitions in the band topology from trivial parabolic pockets to helical Dirac fermions.

Coexistence of Ferroelectricity and Ferromagnetism in One-Dimensional SbN and BiN Nanowires.

Ferroelectricity exists in a variety of three- and two-dimensional materials and is of great significance for the development of electronic devices. However, the presence of ferroelectricity in one-dimensional materials is extremely rare. Here, we predict ferroelectricity in one-dimensional SbN and BiN nanowires. Their polarization strengths are 1 order of magnitude higher than ever reported values in one-dimensional structures. Moreover, we find that spontaneous spin polarization can be generated in SbN and BiN nanowires by moderate hole doping. This is the first time the coexistence of both ferroelectricity and ferromagnetism in a one-dimensional system has been reported. Our finding not only broadens the family of one-dimensional ferroelectric materials but also offers a promising platform for novel electronic and spintronic applications.

Anisotropic gapping of topological Weyl rings in the charge-density-wave superconductor InxTaSe2.

Topological materials and topological phases have recently become a hot topic in condensed matter physics. In this work, we report an In-intercalated transition-metal dichalcogenide InxTaSe2 (named 112 system), a topological nodal-line semimetal in the presence of both charge density wave (CDW) and superconductivity. In the x = 0.58 sample, the 2×3 commensurate CDW (CCDW) and the 2×2 CCDW are observed below 116 and 77 K, respectively. Consistent with theoretical calculations, the spin-orbital coupling gives rise to two twofold-degenerate nodal rings (Weyl rings) connected by drumhead surface states, confirmed by angle-resolved photoemission spectroscopy. Our results suggest that the 2×2 CCDW ordering gaps out one Weyl ring in accordance with the CDW band folding, while the other Weyl ring remains gapless with intact surface states. In addition, superconductivity emerges at 0.91 K, with the upper critical field deviating from the s-wave behavior at low temperature, implying possibly unconventional superconductivity. Therefore, we think this type of the 112 system may possess abundant physical states and offer a platform to investigate the interplay between CDW, nontrivial band topology and superconductivity.

Tunable Topological Energy Bands in 2D Dialkali-Metal Monoxides.

2D materials with nontrivial energy bands are highly desirable for exploring various topological phases of matter, as low dimensionality opens unprecedented opportunities for manipulating the quantum states. Here, it is reported that monolayer (ML) dialkali-metal monoxides, in the well-known 2H-MoS2 type lattice, host multiple symmetry-protected topological phases with emergent fermions, which can be effectively tuned by strain engineering. Based on first-principles calculations, it is found that in the equilibrium state, ML Na2O is a 2D double Weyl semimetal, while ML K2O is a 2D pseudospin-1 metal. These exotic topological states exhibit a range of fascinating effects, including universal optical absorbance, super Klein tunneling, and super collimation effect. By introducing biaxial or uniaxial strain, a series of quantum phase transitions between 2D double Weyl semimetal, 2D Dirac semimetal, 2D pseudospin-1 metal, and semiconductor phases can be realized. The results suggest monolayer dialkali-metal monoxides as a promising platform to explore fascinating physical phenomena associated with novel 2D emergent fermions.

Ferroelectric control of single-molecule magnetism in 2D limit.

The electric control of magnetic properties based on magnetoelectric effect is crucial for the development of future data storage devices. Here, based on first-principles calculations, a strong magnetoelectric effect is proposed to effectively switch on/off the magnetic states as well as alter the in-plane/perpendicular easy axes of metal-phthalocyanine molecules (MPc) by reversing the electric polarization of the underlying two-dimensional (2D) ferroelectric α-In2Se3 substrate with the application of an external electric field. The mechanism originates from the different hybridization between the molecule and the ferroelectric substrate in which the different electronic states of surface Se layer play a dominant role. Moreover, the magnetic moments and magnetic anisotropy energies (MAE) of OsPc/In2Se3 can be further largely enhanced by a functionalized atom atop the OsPc molecule. The I-OsPc/In2Se3 system possesses large MAE up to 30 meV at both polarization directions, which is sufficient for room-temperature applications. These findings provide a feasible scheme to realize ferroelectric control of magnetic states in 2D limit, which have great potential for applications in nanoscale electronics and spintronics.

Heavy fermion quantum criticality at dilute carrier limit in CeNi2-δ(As1-xPx)2.

We study the quantum phase transitions in the nickel pnctides, CeNi2-δ(As1-xPx)2 (δ ≈ 0.07-0.22) polycrystalline samples. This series displays the distinct heavy fermion behavior in the rarely studied parameter regime of dilute carrier limit. We systematically investigate the magnetization, specific heat and electrical transport down to low temperatures. Upon increasing the P-content, the antiferromagnetic order of the Ce-4f moment is suppressed continuously and vanishes at xc ~ 0.55. At this doping, the temperature dependences of the specific heat and longitudinal resistivity display non-Fermi liquid behavior. Both the residual resistivity ρ0 and the Sommerfeld coefficient γ0 are sharply peaked around xc. When the P-content reaches close to 100%, we observe a clear low-temperature crossover into the Fermi liquid regime. In contrast to what happens in the parent compound x = 0.0 as a function of pressure, we find a surprising result that the non-Fermi liquid behavior persists over a nonzero range of doping concentration, xc < x < 0.9. In this doping range, at the lowest measured temperatures, the temperature dependence of the specific-heat coefficient is logarithmically divergent and that of the electrical resistivity is linear. We discuss the properties of CeNi2-δ(As1-xPx)2 in comparison with those of its 1111 counterpart, CeNi(As1-xPx)O. Our results indicate a non-Fermi liquid phase in the global phase diagram of heavy fermion metals.

Magnetic and transport properties of low-carrier-density Kondo semimetal CeSbTe.

Single crystals of CeSbTe with a ZrSiS-type structure were synthesized using vapor transport method. The stoichiometry is deviated from the nominal composition, which may cause some disorder in this compound. The physical properties were characterized by measuring the magnetic susceptibility, electrical resistivity, Hall resistivity and specific heat. One antiferromagnetic (AFM) transition related to Ce3+ ions was found at [Formula: see text] K, and a field-induced metamagnetic transition was observed below [Formula: see text]. The moderately enhanced Sommerfeld coefficient [Formula: see text] mJ mol-1 · K-2 and the estimated Kondo temperature [Formula: see text] K, indicate that CeSbTe is a moderately correlated AFM Kondo lattice compound with crystalline electric field effect. The carrier concentration of CeSbTe derived from the Hall coefficient is in the order of 1021 cm-3, lower than most Kondo metals, which indicates that CeSbTe is a low-carrier-density Kondo semimetal.

Dialkali-Metal Monochalcogenide Semiconductors with High Mobility and Tunable Magnetism.

The discovery of archetypal two-dimensional (2D) materials provides enormous opportunities in both fundamental breakthroughs and device applications, as evident by the research booming in graphene, transition-metal chalcogenides, and black phosphorus. Here, we report a new, large family of semiconducting dialkali-metal monochalcogenides (DMMCs) with an inherent A2X monolayer (ML) structure, in which two alkali sub-MLs form hexagonal close packing and sandwich the triangular chalcogen atomic plane. Such a unique lattice leads to extraordinary physical properties, such as good dynamical and thermal stability, visible to near-infrared energy gap, and high electron mobility. Most strikingly, DMMC MLs host extended van Hove singularities near the valence band (VB) edge, readily accessible by moderate hole doping within 1.0 × 1013 cm-2. Upon critical doping, DMMC MLs undergo spontaneous ferromagnetic transition when the top VBs become fully spin-polarized by strong exchange interactions. Such 2D gate tunable magnetism are promising for exploring novel device concepts in spintronics, electronics and optoelectronics.

Superconductivity in a misfit layered compound (SnSe)1.16(NbSe2).

The large size single crystals of (SnSe)1.16(NbSe2) misfit layered compound were grown and superconductivity with T c of 3.4 K was first discovered in this system. Powder x-ray diffraction and high resolution transmission electron microscopy clearly display the misfit feature between SnSe and NbSe2 subsystems. The Sommerfeld coefficient γ inferred from specific-heat measurements is 16.73 mJ mol-1 K-2, slightly larger than the usual misfit compounds. The normalized specific heat jump [Formula: see text] is about 0.98, and the electron-phonon coupling constant [Formula: see text] is estimated to be 0.80. The estimated value of the in-plane upper critical magnetic field, [Formula: see text](0), is about 7.82 T, exceeding the Pauli paramagnetic limit slightly. Both the specific-heat and H c2 data suggest that (SnSe)1.16(NbSe2) is a multi-band superconductor.

Pressure induced superconductivity bordering a charge-density-wave state in NbTe4 with strong spin-orbit coupling.

Transition-metal chalcogenides host various phases of matter, such as charge-density wave (CDW), superconductors, and topological insulators or semimetals. Superconductivity and its competition with CDW in low-dimensional compounds have attracted much interest and stimulated considerable research. Here we report pressure induced superconductivity in a strong spin-orbit (SO) coupled quasi-one-dimensional (1D) transition-metal chalcogenide NbTe4, which is a CDW material under ambient pressure. With increasing pressure, the CDW transition temperature is gradually suppressed, and superconducting transition, which is fingerprinted by a steep resistivity drop, emerges at pressures above 12.4 GPa. Under pressure p = 69 GPa, zero resistance is detected with a transition temperature T c = 2.2 K and an upper critical field µ0Hc2 = 2 T. We also find large magnetoresistance (MR) up to 102% at low temperatures, which is a distinct feature differentiating NbTe4 from other conventional CDW materials.

Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal.

We report a new quasi-one-dimensional compound KMn6Bi5 composed of parallel nanowires crystallizing in a monoclinic space group C2/ m with a = 22.994(2) Å, b = 4.6128(3) Å, c = 13.3830(13) Å and ß = 124.578(6)°. The nanowires are infinite [Mn6Bi5]- columns each of which is composed of a nanotube of Bi atoms acting as the cladding with a nanorod of Mn atoms located in the central axis of the nanotubes. The nanorods of Mn atoms inside the Bi cladding are stabilized by Mn-Mn bonding and are defined by distorted Mn-centered cluster icosahedra of Mn13 sharing their vertices along the b axis. The [Mn6Bi5]- nanowires are linked with weak internanowire Bi-Bi bonds and charge balanced with K+ ions. The [Mn6Bi5]- nanowires were directly imaged by high-resolution transmission electron microscopy and scanning transmission electron microscopy. Magnetic susceptibility studies show one-dimensional characteristics with an antiferromagnetic transition at ∼75 K and a small average effective magnetic moment (1.56 µB/Mn for H ∥ b and 1.37 µB/Mn for H ⊥ b) of Mn from Curie-Weiss fits above 150 K. Specific heat measurements reveal an electronic specific heat coefficient γ of 6.5(2) mJ K-2(mol-Mn)-1 and a small magnetic entropy change Δ Smag ≈ 1.6 J K-1 (mol-Mn)-1 across the antiferromagnetic transition. In contrast to a metallic resistivity along the column, the resistivity perpendicular to the column shows a change from a semiconducting behavior at high temperatures to a metallic one at low temperatures, indicating an incoherent-to-coherent crossover of the intercolumn tunneling of electrons.

Superconductivity in tantalum self-intercalated 4Ha-Ta1.03Se2.

TaSe2 has several different polytypes and abundant physical properties, such as superconductivity and charge density waves (CDW), which have been investigated in the past few decades. However, there has been no report on the physical properties of the 4Ha polytype up to now. Here we report the crystal growth and discovery of superconductivity in the tantalum self-intercalated 4Ha-Ta1.03Se2 single crystal with a superconducting transition onset temperature of [Formula: see text] K, which is the first observation of superconductivity in the 4Ha polytype of TaSe2. A slightly suppressed CDW transition is found around 106 K. A large [Formula: see text] value of about 4.48 is found when a magnetic field is applied in the ab-plane, which probably results from the enhanced spin-orbit coupling. Special stacking faults are observed, which further enhance the anisotropy. Although the density of states at the Fermi level is lower than that of other polytypes, T c remains the same, indicating that the stack mode of the 4Ha polytype may be beneficial to superconductivity in TaSe2.

Defects controlled hole doping and multivalley transport in SnSe single crystals.

SnSe is a promising thermoelectric material with record-breaking figure of merit. However, to date a comprehensive understanding of the electronic structure and most critically, the self-hole-doping mechanism in SnSe is still absent. Here we report the highly anisotropic electronic structure of SnSe investigated by angle-resolved photoemission spectroscopy, in which a unique pudding-mould-shaped valence band with quasi-linear energy dispersion is revealed. We prove that p-type doping in SnSe is extrinsically controlled by local phase segregation of SnSe2 microdomains via interfacial charge transferring. The multivalley nature of the pudding-mould band is manifested in quantum transport by crystallographic axis-dependent weak localisation and exotic non-saturating negative magnetoresistance. Strikingly, quantum oscillations also reveal 3D Fermi surface with unusual interlayer coupling strength in p-SnSe, in which individual monolayers are interwoven by peculiar point dislocation defects. Our results suggest that defect engineering may provide versatile routes in improving the thermoelectric performance of the SnSe family.

Coexistence of Topological Edge State and Superconductivity in Bismuth Ultrathin Film.

Ultrathin freestanding bismuth film is theoretically predicted to be one kind of two-dimensional topological insulators. Experimentally, the topological nature of bismuth strongly depends on the situations of the Bi films. Film thickness and interaction with the substrate often change the topological properties of Bi films. Using angle-resolved photoemission spectroscopy, scanning tunneling microscopy or spectroscopy and first-principle calculation, the properties of Bi(111) ultrathin film grown on the NbSe2 superconducting substrate have been studied. We find the band structures of the ultrathin film is quasi-freestanding, and one-dimensional edge state exists on Bi(111) film as thin as three bilayers. Superconductivity is also detected on different layers of the film and the pairing potential exhibits an exponential decay with the layer thicknesses. Thus, the topological edge state can coexist with superconductivity, which makes the system a promising platform for exploring Majorana Fermions.