Large Magneto-Transverse and Longitudinal Thermoelectric Effects in the Magnetic Weyl Semimetal TbPtBi.

Magnetic topological semimetals provide new opportunities for power generation and solid-state cooling based on thermoelectric (TE) effect. The interplay between magnetism and nontrivial band topology prompts the magnetic topological semimetals to yield strong transverse TE effect, while the longitudinal TE performance is usually poor. Herein, it is demonstrated that the magnetic Weyl semimetal TbPtBi has high value for both transverse and longitudinal thermopower with large power factor (PF). At 300 K and 13.5 Tesla, the transverse thermopower and PF reach up to 214 µV K-1 and 35 µW cm-1  K-2 , respectively, which are comparable to those of state-of-the-art TE materials. Combining first-principles calculations, longitudinal magnetoresistance and planar Hall resistance measurements, and two-band model fitting, the large transverse thermopower and PF are attributed to both bipolar effect and large Hall angle. Moreover, the imperfectly compensated charge carriers and large transverse magnetoresistance induce the maximum magneto-longitudinal thermopower of 251 µV K-1 with a PF of 24 µW cm-1  K-2 at 150 K and 13.5 Tesla, which is two times higher than that at zero magnetic field. This work demonstrates the great potential of topological semimetals for TEs and offers a new excellent candidate for magneto-TEs.

Physical realization of topological Roman surface by spin-induced ferroelectric polarization in cubic lattice.

Topology, an important branch of mathematics, is an ideal theoretical tool to describe topological states and phase transitions. Many topological concepts have found their physical entities in real or reciprocal spaces identified by topological invariants, which are usually defined on orientable surfaces, such as torus and sphere. It is natural to investigate the possible physical realization of more intriguing non-orientable surfaces. Herein, we show that the set of spin-induced ferroelectric polarizations in cubic perovskite oxides AMn3Cr4O12 (A = La and Tb) reside on the topological Roman surface-a non-orientable two-dimensional manifold formed by sewing a Möbius strip edge to that of a disc. The induced polarization may travel in a loop along the non-orientable Möbius strip or orientable disc, depending on the spin evolution as controlled by an external magnetic field. Experimentally, the periodicity of polarization can be the same or twice that of the rotating magnetic field, which is consistent with the orientability of the disc and the Möbius strip, respectively. This path-dependent topological magnetoelectric effect presents a way to detect the global geometry of a surface and deepens our understanding of topology in both mathematics and physics.

Atomic-Scale Visualization and Quantification of Configurational Entropy in Relation to Thermal Conductivity: A Proof-of-Principle Study in t-GeSb2Te4.

It remains a daunting task to quantify the configurational entropy of a material from atom-revolved electron microscopy images and correlate the results with the material's lattice thermal conductivity, which strides across statics, dynamics, and thermal transport of crystal lattice over orders of magnitudes in length and time. Here, a proof-of-principle study of atomic-scale visualization and quantification of configurational entropy in relation to thermal conductivity in single crystalline trigonal GeSb2Te4 (aka t-GeSb2Te4) with native atomic site disorder is reported. A concerted effort of large t-GeSb2Te4 single crystal growth, in-lab developed analysis procedure of atomic column intensity, the visualization and quantification of configurational entropy including corresponding modulation, and thermal transport measurements enable an entropic "bottom-up" perspective to the lattice thermal conductivity of t-GeSb2Te4. It is uncovered that the configurational entropy increases phonon scattering and reduces phonon mean free path as well as promotes anharmonicity, thereby giving rise to low lattice thermal conductivity and promising thermoelectric performance. The current study sheds lights on an atomic scale bottom-up configurational entropy design in diverse regimes of structural and functional materials research and applications.

Spin reorientation transition and spin dynamics study of perovskite orthoferrite TmFeO3 detected by electron paramagnetic resonance.

The temperature-dependent spin-reorientation transition (SRT) and spin interaction mechanism of bulk TmFeO3 were studied by the electron paramagnetic resonance (EPR) method. The combined experimental results of magnetic curves and EPR spectra confirmed that there is an antiferromagnetic transition at 85 K with a reentering ferromagnetic state due to the spin-reorientation behavior. In the high-temperature region of T > 90 K, there are three distinct resonance peaks in the EPR spectrum, which indicates the presence of multiple magnetic phases (canted antiferromagnetic, weak ferromagnetic, and paramagnetic phases). In the low-temperature region (T < 85 K), the temperature dependence of the EPR linewidth, effective g-factor, and intensity can be used to infer a strong spin-lattice correlation. Different magnetic interactions such as Fe3+-Fe3+, Fe3+-Tm3+, and Tm3+-Tm3+ lead to a paramagnetic-canted antiferromagnetic phase at T > 85 K, with SRT between 85-65 K and ferromagnetic interaction at the lower temperature, respectively. Above 90 K, we find that the spin relaxation mechanism is determined by the mixture of spin-spin and spin-lattice interactions. Below 85 K, the transverse relaxation rate increases with the decrease in temperature, which is consistent with the weakening of the fluctuating internal field in this temperature region. This EPR detection provides a new method to clarify the strong spin coupling in antiferromagnetic materials.

Mode-Resolved Detection of Magnetization Dynamics Using X-ray Diffractive Ferromagnetic Resonance.

Collective spin excitations of ordered magnetic structures offer great potential for the development of novel spintronic devices. The present approach relies on micromagnetic models to explain the origins of dynamic modes observed by ferromagnetic resonance (FMR) studies, since experimental tools to directly reveal the origins of the complex dynamic behavior are lacking. Here we demonstrate a new approach which combines resonant magnetic X-ray diffraction with FMR, thereby allowing for a reconstruction of the real-space spin dynamics of the system. This new diffractive FMR technique builds on X-ray detected FMR that allows for element-selective dynamic studies, giving unique access to specific wave components of static and dynamic coupling in magnetic heterostructures. In combination with diffraction, FMR is elevated to the level of a modal spectroscopy technique, potentially opening new pathways for the development of spintronic devices.

Measurement of the angle dependence of magnetostriction in pulsed magnetic fields using a piezoelectric strain gauge.

We present a high resolution method for measuring magnetostriction in millisecond pulsed magnetic fields at cryogenic temperatures with a sensitivity of 1.11×10-11/Hz . The sample is bonded to a thin piezoelectric plate such that when the sample's length changes, it strains the piezoelectric and induces a voltage change. This method is more sensitive than a fiber-Bragg grating method. It measures two axes simultaneously instead of one. The gauge is small and versatile, functioning in DC and millisecond pulsed magnetic fields. We demonstrate its use by measuring the magnetostriction of Ca3Co1.03Mn0.97O6 single crystals in pulsed magnetic fields. By comparing our data to new and previously published results from a fiber-Bragg grating magnetostriction setup, we confirm that this method detects magnetostriction effects. We also demonstrate the small size and versatility of this technique by measuring angle dependence with respect to the applied magnetic field in a rotator probe in 65 T millisecond pulsed magnetic fields.

Spin-induced multiferroicity in the binary perovskite manganite Mn2O3.

The ABO3 perovskite oxides exhibit a wide range of interesting physical phenomena remaining in the focus of extensive scientific investigations and various industrial applications. In order to form a perovskite structure, the cations occupying the A and B positions in the lattice, as a rule, should be different. Nevertheless, the unique binary perovskite manganite Mn2O3 containing the same element in both A and B positions can be synthesized under high-pressure high-temperature conditions. Here, we show that this material exhibits magnetically driven ferroelectricity and a pronounced magnetoelectric effect at low temperatures. Neutron powder diffraction revealed two intricate antiferromagnetic structures below 100 K, driven by a strong interplay between spin, charge, and orbital degrees of freedom. The peculiar multiferroicity in the Mn2O3 perovskite is ascribed to a combined effect involving several mechanisms. Our work demonstrates the potential of binary perovskite oxides for creating materials with highly promising electric and magnetic properties.

Observation of Magnetodielectric Effect in a Dysprosium-Based Single-Molecule Magnet.

Materials that possess coupled magnetic and electric properties are of significant interest because of their potential use in next-generation magnetoelectric devices such as digital information storage. To date, the magnetoelectric materials that have been studied in-depth have been limited mainly to inorganic oxides such as perovskite oxides. Molecular materials are a promising alternative because their magnetic and electric elements can be combined together at the molecular level via relatively simple molecular designs. Here, we report the coupling of magnetic and electric properties through a magnetodielectric (MD) effect in a single-crystal sample, which is constructed from dysprosium(III) single-molecule magnets (SMMs). The MD effect originates from intrinsic spin-lattice coupling of the dysprosium(III) ion within the sample. This is the first observation of the MD effect in a SMM-based material, which could pave the way toward the synthesis of advanced materials that combine distinct magnetic and electric properties using molecular chemistry for use in molecular devices with nanoscale size.

Mimicking Synaptic Plasticity and Neural Network Using Memtranstors.

Artificial synaptic devices that mimic the functions of biological synapses have drawn enormous interest because of their potential in developing brain-inspired computing. Current studies are focusing on memristive devices in which the change of the conductance state is used to emulate synaptic behaviors. Here, a new type of artificial synaptic devices based on the memtranstor is demonstrated, which is a fundamental circuit memelement in addition to the memristor, memcapacitor, and meminductor. The state of transtance (presented by the magnetoelectric voltage) in memtranstors acting as the synaptic weight can be tuned continuously with a large number of nonvolatile levels by engineering the applied voltage pulses. Synaptic behaviors including the long-term potentiation, long-term depression, and spiking-time-dependent plasticity are implemented in memtranstors made of Ni/0.7Pb(Mg1/3 Nb2/3 )O3 -0.3PbTiO3 /Ni multiferroic heterostructures. Simulations reveal the capability of pattern learning in a memtranstor network. The work elucidates the promise of memtranstors as artificial synaptic devices with low energy consumption.

Realization of Large Electric Polarization and Strong Magnetoelectric Coupling in BiMn3 Cr4 O12.

Magnetoelectric multiferroics have received much attention in the past decade due to their interesting physics and promising multifunctional performance. For practical applications, simultaneous large ferroelectric polarization and strong magnetoelectric coupling are preferred. However, these two properties have not been found to be compatible in the single-phase multiferroic materials discovered as yet. Here, it is shown that superior multiferroic properties exist in the A-site ordered perovskite BiMn3 Cr4 O12 synthesized under high-pressure and high-temperature conditions. The compound experiences a ferroelectric phase transition ascribed to the 6s2 lone-pair effects of Bi3+ at around 135 K, and a long-range antiferromagnetic order related to the Cr3+ spins around 125 K, leading to the presence of a type-I multiferroic phase with huge electric polarization. On further cooling to 48 K, a type-II multiferroic phase induced by the special spin structure composed of both Mn- and Cr-sublattices emerges, accompanied by considerable magnetoelectric coupling. BiMn3 Cr4 O12 thus provides a rare example of joint multiferroicity, where two different types of multiferroic phases develop subsequently so that both large polarization and significant magnetoelectric effect are achieved in a single-phase multiferroic material.

Giant magnetoelectric effects achieved by tuning spin cone symmetry in Y-type hexaferrites.

Multiferroics materials, which exhibit coupled magnetic and ferroelectric properties, have attracted tremendous research interest because of their potential in constructing next-generation multifunctional devices. The application of single-phase multiferroics is currently limited by their usually small magnetoelectric effects. Here, we report the realization of giant magnetoelectric effects in a Y-type hexaferrite Ba0.4Sr1.6Mg2Fe12O22 single crystal, which exhibits record-breaking direct and converse magnetoelectric coefficients and a large electric-field-reversed magnetization. We have uncovered the origin of the giant magnetoelectric effects by a systematic study in the Ba2-x Sr x Mg2Fe12O22 family with magnetization, ferroelectricity and neutron diffraction measurements. With the transverse spin cone symmetry restricted to be two-fold, the one-step sharp magnetization reversal is realized and giant magnetoelectric coefficients are achieved. Our study reveals that tuning magnetic symmetry is an effective route to enhance the magnetoelectric effects also in multiferroic hexaferrites.Control of the electrical properties of materials by means of magnetic fields or vice versa may facilitate next-generation spintronic devices, but is still limited by their intrinsically weak magnetoelectric effect. Here, the authors report the existence of an enhanced magnetoelectric effect in a Y-type hexaferrite, and reveal its underlining mechanism.

Electrochemical-reaction-induced synaptic plasticity in MoOx-based solid state electrochemical cells.

Solid state electrochemical cells with synaptic functions have important applications in building smart-terminal networks. Here, the essential synaptic functions including potentiation and depression of synaptic weight, transition from short- to long-term plasticity, spike-rate-dependent plasticity, and spike-timing-dependent plasticity behavior were successfully realized in an Ag/MoOx/fluorine-doped tin oxide (FTO) cell with continual resistance switching. The synaptic plasticity underlying these functions was controlled by tuning the excitatory post-synaptic current (EPSC) decay, which is determined by the applied voltage pulse number, width, frequency, and intervals between the pre- and post-spikes. The physical mechanism of the artificial synapse operation is attributed to the interfacial electrochemical reaction processes of the MoOx films with the adsorbed water, where protons generated by water decomposition under an electric field diffused into the MoOx films and intercalated into the lattice, leading to the short- and long-term retention of cell resistance, respectively. These results indicate the possibility of achieving advanced artificial synapses with solid state electrochemical cells and will contribute to the development of smart-terminal networking systems.

A multilevel nonvolatile magnetoelectric memory.

The coexistence and coupling between magnetization and electric polarization in multiferroic materials provide extra degrees of freedom for creating next-generation memory devices. A variety of concepts of multiferroic or magnetoelectric memories have been proposed and explored in the past decade. Here we propose a new principle to realize a multilevel nonvolatile memory based on the multiple states of the magnetoelectric coefficient (α) of multiferroics. Because the states of α depends on the relative orientation between magnetization and polarization, one can reach different levels of α by controlling the ratio of up and down ferroelectric domains with external electric fields. Our experiments in a device made of the PMN-PT/Terfenol-D multiferroic heterostructure confirm that the states of α can be well controlled between positive and negative by applying selective electric fields. Consequently, two-level, four-level, and eight-level nonvolatile memory devices are demonstrated at room temperature. This kind of multilevel magnetoelectric memory retains all the advantages of ferroelectric random access memory but overcomes the drawback of destructive reading of polarization. In contrast, the reading of α is nondestructive and highly efficient in a parallel way, with an independent reading coil shared by all the memory cells.

Uniaxial ferroelectric quantum criticality in multiferroic hexaferrites BaFe12O19 and SrFe12O19.

BaFe12O19 is a popular M-type hexaferrite with a Néel temperature of 720 K and is of enormous commercial value ($3 billion/year). It is an incipient ferroelectric with an expected ferroelectric phase transition extrapolated to lie at 6 K but suppressed due to quantum fluctuations. The theory of quantum criticality for such uniaxial ferroelectrics predicts that the temperature dependence of the electric susceptibility χ diverges as 1/T(3), in contrast to the 1/T(2) dependence found in pseudo-cubic materials such as SrTiO3 or KTaO3. In this paper we present evidence of the susceptibility varying as 1/T(3), i.e. with a critical exponent γ = 3. In general γ = (d + z - 2)/z, where the dynamical exponent for a ferroelectric z = 1 and the dimension is increased by 1 from deff = 3 + z to deff = 4 + z due to the effect of long-range dipole interactions in uniaxial as opposed to multiaxial ferroelectrics. The electric susceptibility of the incipient ferroelectric SrFe12O19, which is slightly further from the quantum phase transition is also found to vary as 1/T(3).

Moisture effects on the electrochemical reaction and resistance switching at Ag/molybdenum oxide interfaces.

An important potential application of solid state electrochemical reactions is in redox-based resistive switching memory devices. Based on the fundamental switching mechanisms, the memory has been classified into two modes, electrochemical metallization memory (ECM) and valence change memory (VCM). In this work, we have investigated a solid state electrochemical cell with a simple Ag/MoO3-x/fluorine-doped tin oxide (FTO) sandwich structure, which shows a normal ECM switching mode after an electroforming process. While in the lower voltage sweep range, the switching behavior changes to VCM-like mode with the opposite switching polarity to the ECM mode. By current-voltage measurements under different ambient atmospheres and X-ray photoemission spectroscopy analysis, electrochemical anodic passivation of the Ag electrode and valence change of molybdenum ions during resistance switching have been demonstrated. The crucial role of moisture adsorption in the switching mode transition has been clarified based on the Pourbaix diagram for the Ag-H2O system for the first time. These results provide a fundamental insight into the resistance switching mechanism model in solid state electrochemical cells.

Quantum electric-dipole liquid on a triangular lattice.

Geometric frustration and quantum fluctuations may prohibit the formation of long-range ordering even at the lowest temperature, and therefore liquid-like ground states could be expected. A good example is the quantum spin liquid in frustrated magnets. Geometric frustration and quantum fluctuations can happen beyond magnetic systems. Here we propose that quantum electric-dipole liquids, analogues of quantum spin liquids, could emerge in frustrated dielectrics where antiferroelectrically coupled electric dipoles reside on a triangular lattice. The quantum paraelectric hexaferrite BaFe12O19 with geometric frustration represents a promising candidate for the proposed electric-dipole liquid. We present a series of experimental lines of evidence, including dielectric permittivity, heat capacity and thermal conductivity measured down to 66 mK, to reveal the existence of an unusual liquid-like quantum phase in BaFe12O19, characterized by itinerant low-energy excitations with a small gap. The possible quantum liquids of electric dipoles in frustrated dielectrics open up a fresh playground for fundamental physics.

Observation of Magnetoelectric Multiferroicity in a Cubic Perovskite System: LaMn(3)Cr(4)O(12).

Magnetoelectric multiferroicity is not expected to occur in a cubic perovskite system because of the high structural symmetry. By versatile measurements in magnetization, dielectric constant, electric polarization, neutron and x-ray diffraction, Raman scattering, as well as theoretical calculations, we reveal that the A-site ordered perovskite LaMn(3)Cr(4)O(12) with cubic symmetry is a novel spin-driven multiferroic system with strong magnetoelectric coupling effects. When a magnetic field is applied in parallel (perpendicular) to an electric field, the ferroelectric polarization can be enhanced (suppressed) significantly. The unique multiferroic phenomenon observed in this cubic perovskite cannot be understood by conventional spin-driven microscopic mechanisms. Instead, a nontrivial effect involving the interactions between two magnetic sublattices is likely to play a crucial role.

Nonvolatile electric-field control of magnetization in a Y-type hexaferrite.

The magnetoelectric effects in multiferroic materials enable the mutual control of electric polarization by a magnetic field and magnetization by an electric field. Nonvolatile electric-field control of magnetization is extremely important for information storage applications, but has been rarely realized in single-phase multiferroic materials. Here we demonstrate the prominent direct and converse magnetoelectric effects in the Y-type hexaferrite BaSrCoZnFe11AlO22 single crystal. The electric polarization due to conical magnetic structure can be totally reversed by a small magnetic field, giving rise to large magnetoelectric coefficients of 6000 and 4000 ps/m at 100 and 200 K, respectively. The ab-plane magnetization can be controlled by electric fields with a large hysteresis, leading to nonvolatile change of magnetization. In addition, the reversal of magnetization by electric fields is also realized at 200 K. These diverse magnetoelectric effects with large coefficients highlight the promise of hexaferrites as potential multiferroic materials.

Cross coupling between electric and magnetic orders in a multiferroic metal-organic framework.

The coexistence of both electric and magnetic orders in some metal-organic frameworks (MOFs) has yielded a new class of multiferroics beyond inorganic materials. However, the coupling between two orders in multiferroic MOFs has not been convincingly verified yet. Here we present clear experimental evidences of cross coupling between electric and magnetic orders in a multiferroic MOF [(CH3)2NH2]Fe(HCOO)3 with a perovskite structure. The dielelectric constant exhibit a hump just at the magnetic ordering temperature TN. Moreover, both the direct (magnetic field control of dielectric properties) and converse (electric field control of magnetization) magnetoelectric effects have been observed in the multiferroic state. This work opens up new insights on the origin of ferroelectricity in MOFs and highlights their promise as magnetoelectric multiferroics.

Quantum tunneling of magnetization in a metal-organic framework.

Resonant quantum tunneling of magnetization has been observed in a hybrid metal-organic framework where an intrinsic magnetic phase separation leads to the coexistence of long-range canted antiferromagnetic order and isolated single-ion quantum magnets. This unusual magnetic phenomenon is well interpreted based on a selective long-distance superexchange model in which the exchange interaction between transition metal ions through an organic linker depends on the position of hydrogen bonds. Our work not only extends the resonant quantum tunneling of magnetization to a new class of materials but also evokes the important role of hydrogen bonding in organic magnetism.