Field-driven Phase Transition Research Articles

Engineering Plateau Phase Transition in Quantum Anomalous Hall Multilayers.

The plateau phase transition in quantum anomalous Hall (QAH) insulators corresponds to a quantum state wherein a single magnetic domain gives way to multiple domains and then reconverges back to a single magnetic domain. The layer structure of the sample provides an external knob for adjusting the Chern number C of the QAH insulators. Here, we employ molecular beam epitaxy to grow magnetic topological insulator multilayers and realize the magnetic field-driven plateau phase transition between two QAH states with odd Chern number change ΔC. We find that critical exponents extracted for the plateau phase transitions with ΔC = 1 and ΔC = 3 in QAH insulators are nearly identical. We construct a four-layer Chalker-Coddington network model to understand the consistent critical exponents for the plateau phase transitions with ΔC = 1 and ΔC = 3. This work will motivate further investigations into the critical behaviors of plateau phase transitions with different ΔC in QAH insulators.

Giant energy storage and power density negative capacitance superlattices.

Dielectric electrostatic capacitors1, because of their ultrafast charge-discharge, are desirable for high-power energy storage applications. Along with ultrafast operation, on-chip integration can enable miniaturized energy storage devices for emerging autonomous microelectronics and microsystems2-5. Moreover, state-of-the-art miniaturized electrochemical energy storage systems-microsupercapacitors and microbatteries-currently face safety, packaging, materials and microfabrication challenges preventing on-chip technological readiness2,3,6, leaving an opportunity for electrostatic microcapacitors. Here we report record-high electrostatic energy storage density (ESD) and power density, to our knowledge, in HfO2-ZrO2-based thin film microcapacitors integrated into silicon, through a three-pronged approach. First, to increase intrinsic energy storage, atomic-layer-deposited antiferroelectric HfO2-ZrO2 films are engineered near a field-driven ferroelectric phase transition to exhibit amplified charge storage by the negative capacitance effect7-12, which enhances volumetric ESD beyond the best-known back-end-of-the-line-compatible dielectrics (115 J cm-3) (ref. 13). Second, to increase total energy storage, antiferroelectric superlattice engineering14 scales the energy storage performance beyond the conventional thickness limitations of HfO2-ZrO2-based (anti)ferroelectricity15 (100-nm regime). Third, to increase the storage per footprint, the superlattices are conformally integrated into three-dimensional capacitors, which boosts the areal ESD nine times and the areal power density 170 times that of the best-known electrostatic capacitors: 80 mJ cm-2 and 300 kW cm-2, respectively. This simultaneous demonstration of ultrahigh energy density and power density overcomes the traditional capacity-speed trade-off across the electrostatic-electrochemical energy storage hierarchy1,16. Furthermore, the integration of ultrahigh-density and ultrafast-charging thin films within a back-end-of-the-line-compatible process enables monolithic integration of on-chip microcapacitors5, which can unlock substantial energy storage and power delivery performance for electronic microsystems17-19.

Experimental study on coupled caloric effect driven by dual fields in metamagnetic alloy ErCo2

This study presents an experimental investigation of the coupled caloric effect driven by dual-fields in metamagnetic alloy ErCo2 with strong magneto-structural coupling. Magnetic measurements were conducted under different pressures, revealing that the application of hydrostatic pressure stabilizes a small volume of paramagnetism (PM) phase, resulting in a shift of the phase transition temperature towards the low-temperature region. This shift is opposite to the temperature associated with the magnetic field-driven phase transition. As pressure increases, the metamagnetic transition in ErCo2 is suppressed, and the hysteresis disappears. However, the produced cross-coupling caloric effect compensates the decrease in entropy change caused by the disappearance of the metamagnetic transition. As a result, a reversible giant magnetocaloric effect of 46.2 J/(kg·K) without hysteresis is achieved at a pressure of 0.910 GPa. Moreover, we propose that the temperature span of ErCo2 can be significantly widened by optimizing the thermodynamic pathway of the magnetic and pressure fields, overcoming the defect of a narrow temperature range.

Low voltage–driven high-performance thermal switching in antiferroelectric PbZrO 3 thin films

Effective control of heat transfer is vital for energy saving and carbon emission reduction. In contrast to achievements in electrical conduction, active control of heat transfer is much more challenging. Ferroelectrics are promising candidates for thermal switching as a result of their tunable domain structures. However, switching ratios in ferroelectrics are low (<1.2). We report that high-quality antiferroelectric PbZrO 3 epitaxial thin films exhibit high-contrast (>2.2), fast-speed (<150 nanoseconds), and long-lifetime (>10 7 ) thermal switching under a small voltage (<10 V). In situ reciprocal space mapping and atomistic modelings reveal that the field-driven antiferroelectric-ferroelectric phase transition induces a substantial change of primitive cell size, which modulates phonon-phonon scattering phase space drastically and results in high switching ratio. These results advance the concept of thermal transport control in ferroic materials.

High-performance van der Waals antiferroelectric CuCrP2S6-based memristors

Layered thio- and seleno-phosphate ferroelectrics, such as CuInP2S6, are promising building blocks for next-generation nonvolatile memory devices. However, because of the low Curie point, the CuInP2S6-based memory devices suffer from poor thermal stability (<42 °C). Here, exploiting the electric field-driven phase transition in the rarely studied antiferroelectric CuCrP2S6 crystals, we develop a nonvolatile memristor showing a sizable resistive-switching ratio of ~ 1000, high switching endurance up to 20,000 cycles, low cycle-to-cycle variation, and robust thermal stability up to 120 °C. The resistive switching is attributed to the ferroelectric polarization-modulated thermal emission accompanied by the Fowler–Nordheim tunneling across the interfaces. First-principles calculations reveal that the good device performances are associated with the exceptionally strong ferroelectric polarization in CuCrP2S6 crystal. Furthermore, the typical biological synaptic learning rules, such as long-term potentiation/depression and spike amplitude/spike time-dependent plasticity, are also demonstrated. The results highlight the great application potential of van der Waals antiferroelectrics in high-performance synaptic devices for neuromorphic computing.

Evolving energy-storage performances during temperature-induced antiferroelectric P–R phase transition in NaNbO3-based lead-free ceramics

Temperature-driven antiferroelectric (AFE) P to AFE R phase transition in MnO2-doped 0.90NaNbO3-0.10CaTiO3 ceramics was investigated through polarization-field response, energy-storage and charge-discharge properties as well as ex/in-situ multiscale structure characterization. Both room-temperature AFE P and high-temperature AFE R phases show double polarization-electric field hysteresis loops, indicating a reversible field-driven AFE to ferroelectric (FE) phase transition. An abnormal variation of critical fields for the AFE-FE and FE-AFE phase transition and a faster polarization-field response contribute to the reduced polarization hysteresis for both AFE P and R phases but an obviously expanded linear polarization-field response only for AFE R phase, being responsible for a two-time significant enhancement in energy-storage properties from P phase to P–R phase boundary and then to R phase. The variation of unit cell anisotropy and domain morphology with temperature was found to play crucial roles in the modulated field-driven phase transition behavior and polarization-field response on heating.

Possible evidence of Weyl fermion enhanced thermal conductivity under magnetic fields in the antiferromagnetic topological insulator Mn(Bi1−xSbx)2Te4

We report thermal conductivity and Seebeck effect measurements on $\text{Mn}{({\text{Bi}}_{1\ensuremath{-}x}{\text{Sb}}_{x})}_{2}{\text{Te}}_{4}$ (MBST) with $x=0.26$ under applied magnetic fields below $50\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. Our data shows clear indications of the electronic structure transition induced by the antiferromagnetic (AFM) to ferromagnetic (FM) transition driven by applied magnetic field as well as significant positive magnetothermal conductivity in the Weyl semimetal state of MBST. Further, by examining the dependence of magnetothermal conductivity on field orientation for MBST and comparison with the magnetothermal conductivity of ${\text{MnBi}}_{2}{\text{Te}}_{4}$, we see possible evidence of a contribution to thermal conductivity due to Weyl fermions in the FM phase of MBST. From the temperature dependence of the Seebeck coefficient under magnetic fields for MBST, we also observed features consistent with the Fermi surface evolution from a hole pocket in the paramagnetic state to a Fermi surface with coexistence of electron and hole pockets in the FM state. These findings provide further evidence for the field-driven topological phase transition from an AFM topological insulator to a FM Weyl semimetal.

Magnetic field-dependent lattice entropy change in Gd5Ge4

The total entropy change in the first-order magnetic phase transition materials is mainly composed of lattice entropy change (LEC) and magnetic entropy change (MEC). Generally, the MEC is limited by the total angular momentum quantum number, while the LEC is related to the volume change associated with phase transition and it can be easily regulated. Therefore, maximizing LEC is considered as an effective means to improve the refrigeration performance. However, the current research methods only calculate the LEC between two stable phases after phase transition, whereas the LEC during phase transformation is not fully clarified. Here, the mixed Debye temperature (MDT) model and the mixed lattice entropy (MLE) model are proposed based on the two-phase coexistence mechanism for calculating the LEC during the magnetic field-driven phase transition in Gd5Ge4. Both models indicate that the lattice entropy strongly depends on the applied magnetic field during phase transformation. According to the MLE model, which shows better accuracy, a large LEC up to –22.31 Jkg-1K−1 at 25 K can be exerted in Gd5Ge4 by a relatively small magnetic field of 2.5 T. Our proposed theoretical models are helpful for designing high-performance magnetic refrigerants.

Machine-Learning Spectral Indicators of Topology.

Topological materials discovery has emerged as an important frontier in condensed matter physics. While theoretical classification frameworks have been used to identify thousands of candidate topological materials, experimental determination of materials' topology often poses significant technical challenges. X-ray absorption spectroscopy (XAS) is a widely used materials characterization technique sensitive to atoms' local symmetry and chemical bonding, which are intimately linked to band topology by the theory of topological quantum chemistry (TQC). Moreover, as a local structural probe, XAS is known to have high quantitative agreement between experiment and calculation, suggesting that insights from computational spectra can effectively inform experiments. In this work, computed X-ray absorption near-edge structure (XANES) spectra of more than 10000 inorganic materials to train a neural network (NN) classifier that predicts topological class directly from XANES signatures, achieving F1 scores of 89% and 93% for topological and trivial classes, respectively is leveraged. Given the simplicity of the XAS setup and its compatibility with multimodal sample environments, the proposed machine-learning-augmented XAS topological indicator has the potential to discover broader categories of topological materials, such as non-cleavable compounds and amorphous materials, and may further inform field-driven phenomena in situ, such as magnetic field-driven topological phasetransitions.

Cascade of magnetic-field-driven quantum phase transitions in Ce3Pd20Si6

Magnetically hidden order is a hypernym for electronic ordering phenomena that are visible to macroscopic thermodynamic probes but whose microscopic symmetry cannot be revealed with conventional neutron or x-ray diffraction. In a handful of f-electron systems, the ordering of odd-rank multipoles leads to order parameters with a vanishing neutron cross-section. Among them, Ce$_3$Pd$_{20}$Si$_6$ is known for its unique phase diagram exhibiting two distinct multipolar-ordered ground states (phases II and II'), separated by a field-driven quantum phase transition associated with a putative change in the ordered quadrupolar moment from $O_2^0$ to $O_{xy}$. Using torque magnetometry at subkelvin temperatures, here we find another phase transition at higher fields above 12 T, which appears only for low-symmetry magnetic field directions $\mathbf{B} \parallel \langle11L\rangle$ with $1 < L \leq 2$. While the order parameter of this new phase II'' remains unknown, the discovery renders Ce$_3$Pd$_{20}$Si$_6$ a unique material with two field-driven phase transitions between distinct multipolar phases. They are both clearly manifested in the magnetic-field dependence of the field-induced (111) Bragg intensities measured with neutron scattering for $\mathbf{B} \parallel [112]$. We also find from inelastic neutron scattering that the number of nondegenerate collective excitations induced by the magnetic field correlates with the number of phases in the magnetic phase diagram for the same field direction. Furthermore, the magnetic excitation spectrum suggests that the new phase II'' may have a different propagation vector, revealed by the minimum in the dispersion that may represent the Goldstone mode of this hidden-order phase.

Interlayer magnetophononic coupling in MnBi2Te4

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise ‘forbidden’ by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

Magnon condensation in dimerized antiferromagnets with spin-orbit coupling

Bose-Einstein condensation (BEC) of triplet excitations triggered by a magnetic field, sometimes called magnon BEC, in dimerized antiferromagnets gives rise to a long-range antiferromagnetic order in the plane perpendicular to the applied magnetic field. To explore the effects of spin-orbit coupling on magnon condensation, we study a spin model on a distorted honeycomb lattice with dimerized Heisenberg exchange ($J$ terms) and uniform off-diagonal exchange ($\Gamma'$ terms) interactions. Via variational Monte Carlo calculations and spin-wave theory, we find that an out-of-plane magnetic field can induce different types of long-range magnetic orders, no matter if the ground state is a non-magnetic dimerized state or an ordered N\'{e}el state. Furthermore, the critical properties of field-driven phase transitions in the presence of spin-orbit couplings, as illustrated from spin-wave spectrum and interpreted by effective field theory, can be different from the conventional magnon BEC. Our study is helpful to understand the rich phases of spin-orbit coupled antiferromagnets induced by magnetic fields.

Frustrated magnetism of spin- 12 Heisenberg diamond and octahedral chains as a statistical mechanical monomer-dimer problem

It is evidenced that effective lattice-gas models of hard-core monomers and dimers afford a proper description of low-temperature features of spin-$\frac{1}{2}$ Heisenberg diamond and octahedral chains. In addition to monomeric particles assigned within the localized-magnon theory to bound one- and two-magnon eigenstates, the effective monomer-dimer lattice-gas model includes dimeric particles assigned to a singlet-tetramer (singlet-hexamer) state as a cornerstone of dimer-tetramer (tetramer-hexamer) ground state of a spin-$\frac{1}{2}$ Heisenberg diamond (octahedral) chain. The feasibility of the effective description is confirmed through the exact diagonalization and finite-temperature Lanczos methods. Both quantum spin chains display rich ground-state phase diagrams including discontinuous as well as continuous field-driven phase transitions, whereby the specific heat shows in vicinity of the former phase transitions an extraordinary low-temperature peak coming from a highly degenerate manifold of low-lying excitations.

Magnetic field driven phase transitions in EuTiO3

The influence of an external static magnetic field (up to 480 mT) on the structural properties of EuTiO3 (ETO) polycrystalline samples was examined by powder XRD at the Elettra synchrotron facilities in the temperature range 100–300 K. While the cubic to tetragonal structural phase transition temperature in this magnetic field range remains almost unaffected, significant lattice effects appear at two characteristic temperatures (∼200 K and ∼250 K), which become more pronounced at a critical threshold field. At ∼200 K a change in the sign of magnetostriction is detected attributed to a modification of the local magnetic properties from intrinsic ferromagnetism to intrinsic antiferromagnetism. These data are a clear indication that strong spin–lattice interactions govern also the high temperature phase of ETO and trigger the appearance of magnetic domain formation and phase transitions.

Ferroelectric switching in GeTe through rotation of lone-pair electrons by Electric field-driven phase transition

Germanium telluride (GeTe), which has long been used in phase-change devices, has very unique structural characteristics. While atomic movement and related bond-order switching have been believed to determine the ferroelectric characteristics of this compound, structural changes accompanying ferroelectric switching have not been examined. In this study, using transmission electron microscopy and Raman spectroscopy, we directly observed the atomic movement and the related change in the local structure of GeTe during ferroelectric switching under an applied E-field. The crystal symmetry of GeTe could be alternated between two phases (R3m (rhombohedral) and Cm (monoclinic)) by changing the compound's polarization direction, indicating that the ferroelectric switching behavior of GeTe can be controlled. This observation suggests that ferroelectric switching of GeTe may originate from the phase transition between R3m and Cm through the formation of a morphotropic phase boundary (MPB). Since these two phases can generate MPBs with similar energies, the rotation of lone-pair direction during the phase transition can effectively change the polarization direction. The exotic phenomenon of ferroelectric switching, which involves changes in the chemical bonds, can be predicted on the basis of the role of several dopants through DFT calculations.

Evidence for the Fulde\u2013Ferrell\u2013Larkin\u2013Ovchinnikov state in bulk NbS2

We present measurements of the magnetic torque, specific heat and thermal expansion of the bulk transition metal dichalcogenide (TMD) superconductor NbS2 in high magnetic fields, with its layer structure aligned strictly parallel to the field using a piezo rotary positioner. The upper critical field of superconducting TMDs in the 2D form is known to be dramatically enhanced by a special form of Ising spin orbit coupling. This Ising superconductivity is very robust to the Pauli paramagnetic effect and can therefore exist beyond the Pauli limit for superconductivity. We find that superconductivity beyond the Pauli limit still exists in bulk single crystals of NbS2 for a precisely parallel field alignment. However, the comparison of our upper critical field transition line with numerical simulations rather points to the development of a Fulde-Ferrell-Larkin-Ovchinnikov state above the Pauli limit as a cause. This is also consistent with the observation of a magnetic field driven phase transition in the thermodynamic quantities within the superconducting state near the Pauli limit.

Two Phases Inside the Bose Condensation Dome of Yb_{2}Si_{2}O_{7}.

Recent experimental data on Bose-Einstein condensation of magnons in the spin-gap compound Yb_{2}Si_{2}O_{7} revealed an asymmetric Bose-Einstein condensation dome [G. Hester et al., Phys. Rev. Lett. 123, 027201 (2019)PRLTAO0031-900710.1103/PhysRevLett.123.027201]. We examine modifications to the Heisenberg model on a breathing honeycomb lattice, showing that this physics can be explained by competing anisotropic perturbations. We employ a gamut of analytical and numerical techniques to show that the anisotropy yields a field driven phase transition from a state with broken Ising symmetry to a phase that breaks no symmetries and crosses over to the polarized limit.

In situ heating studies on temperature-induced phase transitions in epitaxial Hf0.5Zr0.5O2/La0.67Sr0.33MnO3 heterostructures

Hafnia-based thin films exhibit unconventional ferroelectricity. These materials also show rich polymorphism, and thus temperature and field-driven phase transitions, as well as oxygen migration. In a bigger context of exploring the synergy between ferroelectricity and diffusion-based structural phenomena, here we study temperature-dependent phase transitions in epitaxial Hf0.5Zr0.5O2(HZO)/La0.67Sr0.33MnO3 (LSMO, bottom electrode) heterostructures. We report topotactic phase transitions and their clear pathways in both LSMO and HZO layers upon heating under vacuum, using in situ scanning transmission electron microscopy (STEM). Specifically, we directly image oxygen and cationic columns using integrated differential phase contrast STEM and follow their evolution with temperature. We also perform in situ high temperature x-ray diffraction in air and show that the LSMO layer undergoes reversible thermal expansion and contraction when heated up to 850 °C, whereas HZO undergoes strain relaxation beyond 750 °C without any reversible phase transition. Our results provide a comprehensive and direct understanding of temperature-dependent structure, defect, and property correlations in these systems.

Pressure and inversion symmetry breaking field-driven first-order phase transition and formation of Dirac circle in perovskites

Through model Hamiltonian studies and first-principle electronic structure calculations, we have examined the effect of inversion symmetry breaking (ISB) field and hydrostatic pressure on the band topology of halide perovskites by taking MAPbI$_3$ as a prototype. Our study shows that while hydrostatic pressure induces normal to topological insulator continuous phase transition, the ISB field makes it first order. The pressure smoothly reduces the normal bandgap, and without ISB, the system achieves a gapless state before it produces a non-trivial bandgap with inverted characters. The ISB field does not stabilize the gapless state, and therefore, the discontinuity in the bandgap with pressure gives rise to the first-order transition. Furthermore, in the non-trivial phase, the ISB field forms an invariant surface Dirac circle in the neighbourhood of TRIM, which is first of its kind. The circle is formed due to interpenetration of Dirac cones resembling the band topology of AA-stacked bilayer graphene.

Topological defect states in mesoscopic superconducting squares with spin correlations

In the framework of the microscopic Bogoliubov-de Gennes theory, we study the topological defect states in mesoscopic superconducting square systems with spin correlations. The dominant spin-triplet -wave pairing symmetry of order parameters can be realized by choosing appropriate band parameters. At zero external magnetic field, the single-domain-wall state tends to emerge as the ground state of the system. When the magnetic field is applied, there exist field-driven phase transitions among three types of (anti)vortex patterns for the vortex-free ground state. With increasing field, a large number of coreless single-skyrmionic states with different topological charges can appear as the ground states. In particular, a novel chiral domain-wall ground state carrying fractional total flux quanta can take place, accompanied by an unclosed half-quantum-vortex chain in the phase difference profile. Several unique metastable states are also revealed in the strong flux range in the present system.