npj Quantum Materials最新文献

GdTe₃ is a layered antiferromagnet which has attracted attention due to its exceptionally high mobility, distinctive unidirectional incommensurate charge density wave (CDW), superconductivity under pressure, and a cascade of magnetic transitions between 7 and 12 K, with as yet unknown order parameters. Here, we use spin-polarized scanning tunneling microscopy to directly image the charge and magnetic orders in GdTe₃. Below 7 K, we find a striped antiferromagnetic phase with twice the periodicity of the Gd lattice and perpendicular to the CDW. As we heat the sample, we discover a spin density wave with the same periodicity as the CDW between 7 and 12 K; the viability of this phase is supported by our Landau free energy model. Our work reveals the order parameters of the magnetic phases in GdTe₃ and shows how the interplay between charge and spin can generate a cascade of magnetic orders.

Elastocaloric measurements of the ferroquadrupolar/nematic rare-earth intermetallic TmAg₂ are presented. TmAg₂ undergoes a cooperative Jahn-Teller-like ferroquadrupolar phase transition at 5K, in which the Tm³⁺ ion’s local 4f electronic ground state doublet spontaneously splits and develops an electric quadrupole moment which breaks the rotational symmetry of the tetragonal lattice. The elastocaloric effect, which is the temperature change in the sample induced by adiabatic strains the sample experiences, is sensitive to quadrupolar fluctuations in the paranematic phase which couple to the induced strain. We show that elastocaloric measurements of this material reveal a Curie-Weiss like nematic susceptibility with a Weiss temperature of T* ≈ 2.7K, in agreement with previous elastic constant measurements. Furthermore, we establish that a magnetic field along the c-axis acts as an effective transverse field for the quadrupole moments.

Skyrmion lattices (SkL) in centrosymmetric materials typically have a magnetic period on the nanometer-scale, so that the coupling between magnetic superstructures and the underlying crystal lattice cannot be neglected. We reveal the commensurate locking of a SkL to the atomic lattice in Gd₃Ru₄Al₁₂ via high-resolution resonant elastic x-ray scattering (REXS). Weak easy-plane magnetic anisotropy, demonstrated here by a combination of ferromagnetic resonance and REXS, penalizes placing a skyrmion core on a site of the atomic lattice. Under these conditions, a commensurate SkL, locked to the crystal lattice, is stable at finite temperatures – but gives way to a competing incommensurate ground state upon cooling. We discuss the role of Umklapp-terms in the Hamiltonian for the formation of this lattice-locked state, its magnetic space group, and the role of slight discommensurations, or (line) defects in the magnetic texture. We also contrast our findings with the case of SkLs in noncentrosymmetric material platforms.

Ferroelectricity in crystalline hafnium oxide has attracted considerable attention because of its potential application for memory devices. A recent breakthrough involves electric-field-induced crystallization, allowing HfO₂-based materials to avoid high-temperature crystallization, which is unexpected in the back-end-of-line process. However, due to the lack of clarity in understanding the mechanisms during the crystallization process, we aim to employ theoretical methods for simulation, to guide experimental endeavors. In this work, we extended our phase-field model by coupling the crystallization model and time-dependent Ginzburg-Landau equation to analyze the crystalline properties and the polarization evolution of Hf_0.5Zr_0.5O₂ thin film under applying an electric field periodic pulse. Through this approach, we found a wake-up effect during the process of crystallization and a transformation from orthorhombic nano-domains to the stripe domain. Furthermore, we have proposed an innovative artificial neural synapse concept based on the continuous polarization variation under applied electric field pulses. Our research lays the theoretical groundwork for the advancement of electric-field-induced crystallization in the hafnium oxide system.

Owing to geometrical frustration in the kagome lattice, Mn₃Sn displays a 120° in-plane triangular antiferromagnetic order, a manifestation of exchange interaction within the Heisenberg model. Here, we show the formation of a tunable noncoplanar magnetic ground state stabilized by higher-order exchange interactions in electron-doped Mn₃Sn samples. Our density Functional Theory calculations reveal that the higher-order exchange induces a partial out-of-plane alignment of the Mn moments, resulting in a canted magnetic state, further experimentally confirmed by neutron diffraction study along with 60 T magnetic and Hall resistivity measurements. Interestingly, we find a large scalar spin chirality-induced Hall signal depending on the degree of non-coplanarity of the Mn moments. Additionally, we demonstrate simultaneous manipulation of two-component order-parameter in the system, where the two Hall signals can be independently manipulated. The present study explores the quantum phenomena associated with the coexistence of multiple magnetic orders and their prospective use in spintronic devices.

Predicting magnetic ordering in kagome compounds offers the possibility of harnessing topological or flat-band physical properties through tuning of the magnetism. Here, we examine the magnetic interactions and phases of ErMn₆Sn₆ which belongs to a family of RMn₆Sn₆, R = Sc, Y, Gd–Lu, compounds with magnetic kagome Mn layers, triangular R layers, and signatures of topological properties. Using results from single-crystal neutron diffraction and mean-field analysis, we find that ErMn₆Sn₆ sits close to the critical boundary separating the spiral-magnetic and ferrimagnetic ordered states typical for non-magnetic versus magnetic R layers, respectively. Finding interlayer magnetic interactions and easy-plane Mn magnetic anisotropy consistent with other members of the family, we predict the existence of a number of temperature and field dependent collinear, noncollinear, and noncoplanar magnetic phases. We show that thermal fluctuations of the Er magnetic moment, which act to weaken the Mn-Er interlayer magnetic interaction and quench the Er magnetic anisotropy, dictate magnetic phase stability. Our results provide a starting point and outline a multitude of possibilities for studying the behavior of Dirac fermions in RMn₆Sn₆ compounds with control of the Mn spin orientation and real-space spin chirality.

Electrons in metals can show a giant anomalous Hall effect (AHE) when interacting with characteristic spin texture. The AHE has been discussed in terms of scalar-spin-chirality (SSC) in long-range-ordered noncollinear spin textures typified by Skyrmion. The SSC becomes effective even in the paramagnetic state with thermal fluctuations, but the resultant AHE has been limited to be very small. Here, we report the observation of large AHE caused by the spin fluctuation near the devil’s staircase transition in a collinear antiferromagnetic metal SrCo₆O₁₁. The AHE is prominent near and above the transition temperature at moderate magnetic fields, where the anomalous Hall angle becomes the highest level among known oxide collinear ferromagnets/antiferromagnets (>2%). Furthermore, the anomalous Hall conductivity is quadratically scaled to the conductivity. These results imply that the thermally induced solitonic spin defects inherent to the devil’s staircase transition promote SSC-induced skew scattering.

We use elastic and inelastic neutron scattering (INS) to study the antiferromagnetic (AF) phase transitions and spin excitations in the two-dimensional (2D) zig-zag antiferromagnet FePSe₃. By determining the magnetic order parameter across the AF phase transition, we conclude that the AF phase transition in FePSe₃ is first-order in nature. In addition, our INS measurements reveal that the spin waves in the AF ordered state have a large easy-axis magnetic anisotropy gap, consistent with an Ising Hamiltonian, and possible biquadratic magnetic exchange interactions. On warming across T_N, we find that dispersive spin excitations associated with three-fold rotational symmetric AF fluctuations change into FM spin fluctuations above T_N. These results suggest that the first-order AF phase transition in FePSe₃ may arise from the competition between C₃ symmetric AF and C₁ symmetric FM spin fluctuations around T_N, in place of a conventional second-order AF phase transition.

Motivated by the recent observation of superconductivity with T_c ~ 80 K in pressurized La₃Ni₂O₇¹, we explore the structural and electronic properties of A₃Ni₂O₇ bilayer nickelates (A = La-Lu, Y, Sc) as a function of pressure (0–150 GPa) from first principles including a Coulomb repulsion term. At ~ 20 GPa, we observe an orthorhombic-to-tetragonal transition in La₃Ni₂O₇ at variance with x-ray diffraction data, which points to so-far unresolved complexities at the onset of superconductivity, e.g., charge doping by variations in the oxygen stoichiometry. We compile a structural phase diagram that establishes chemical and external pressure as distinct and counteracting control parameters. We find unexpected correlations between T_c and the in-plane Ni-O-Ni bond angles for La₃Ni₂O₇. Moreover, two structural phases with significant c⁺ octahedral rotations and in-plane bond disproportionations are uncovered for A = Nd-Lu, Y, Sc that exhibit a pressure-driven electronic reconstruction in the Ni e_g manifold. By disentangling the involvement of basal versus apical oxygen states at the Fermi surface, we identify Tb₃Ni₂O₇ as an interesting candidate for superconductivity at ambient pressure. These results suggest a profound tunability of the structural and electronic phases in this novel materials class and are key for a fundamental understanding of the superconductivity mechanism.

Atomic-scale spin entity in a two-dimensional topological insulator lays the foundation to manufacture magnetic topological materials with single atomic thickness. Here, we have successfully fabricated Fe monomer, dimer and trimer doped in the monolayer stanene/Cu(111) through a low-temperature growth and systematically investigated Kondo effect by combining scanning tunneling microscopy/spectroscopy (STM/STS) with density functional theory (DFT) and numerical renormalization group (NRG) method. Given high spatial and energy resolution, tunneling conductance (dI/dU) spectra have resolved zero-bias Kondo resonance and resultant magnetic-field-dependent Zeeman splitting, yielding an effective spin S_eff = 3/2 with an easy-plane magnetic anisotropy on the self-assembled Fe atomic dopants. Reduced Kondo temperature along with attenuated Kondo intensity from Fe monomer to trimer have been further identified as a manifestation of Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction between Sn-separated Fe atoms. Such magnetic Fe atom assembly in turn constitutes important cornerstones for tailoring topological band structures and developing magnetic phase transition in the single-atom-layer stanene.