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Van der Waals (vdW) magnets have opened a new avenue of novel opportunities covering various interesting phases. Co1/3TaS2-an intercalated metallic vdW antiferromagnet-is one of the latest important additions to the growing list of materials due to its unique triple-Q (3Q) ground state possessing topological characteristics. Careful bulk characterisations have shown the ground state of CoxTaS2 to be a rare 3Q tetrahedral structure for x less than 1/3. The uniqueness of this ground state arises from the dense real-space Berry curvature due to scalar spin chirality, giving rise to a noticeable anomalous Hall effect. In this work, we demonstrate that we can control this topological phase via gating. Using three kinds of CoxTaS2 devices with different Co compositions, we have established that we can cover the whole 3Q topological phase with ionic gating. This work reports a rare demonstration of electrical gating control of layered antiferromagnetic metal. More importantly, our work constitutes one of the first examples of the electrical control of the scalar spin chirality using antiferromagnetic metal., Comment: 19 pages, 4 figures

Identifying the exotic quantum spin liquid phase in Kitaev magnets has garnered great research interests and remains a significant challenge. In experiments, most of the proposed candidate materials exhibit an antiferromagnetic (AFM) order at low temperatures, thus the challenge transforms into the searching for a field-driven disordered phase that is distinct from the partially polarized paramagnetic phase after suppressing the AFM order. Recently, Na$_2$Co$_2$TeO$_6$ has been proposed as one of the prime candidates, where the Kitaev interaction is realized by the high-spin $t^{5}_{2g}e^2_g$ configuration, and spin-orbit entangled $J_{\rm eff} = 1/2$ state in a bond-edge shared honeycomb lattice. In this study, we identify an emergent intermediate disordered phase induced by an external field along the $c$-axis of the honeycomb plane. This phase is characterized through magnetization and magnetocaloric effect experiments in high magnetic fields. To explain the experimental results, we propose an effective spin model with large AFM Kitaev interaction, which yields results in good agreement with both our findings and previously reported data. We determine that the effective $K$-$J$-$\Gamma$-$\Gamma'$ model for Na$_2$Co$_2$TeO$_6$ is nearly dual to that of $\alpha$-RuCl$_3$ under an unitary transformation. Given the insignificant fragility of Na$_2$Co$_2$TeO$_6$ sample, further high-field experiments can be conducted to explore this intermediate-field quantum spin disordered phase., Comment: 12 pages, 8 figures

Van der Waals (vdW) magnets have rapidly emerged as a fertile playground for novel fundamental physics and exciting applications. Despite the impressive developments over the past few years, technical limitations pose a severe challenge to many other potential breakthroughs. High on the list is the lack of suitable experimental tools for studying spin dynamics on atomically thin samples. Here, Raman scattering techniques are employed to observe directly the low-lying magnon (~1 meV) even in bilayer NiPS3. The unique advantage is that it offers excellent energy resolutions far better on low-energy sides than most inelastic neutron spectrometers can offer. More importantly, with appropriate theoretical analysis, the polarization dependence of the Raman scattering by those low-lying magnons also provides otherwise hidden information on the dominant spin-exchange scattering paths for different magnons. By comparing with high-resolution inelastic neutron scattering data, these low-energy Raman modes are confirmed to be indeed of magnon origin. Because of the different scattering mechanisms involved in inelastic neutron and Raman scattering, this new information is fundamental in pinning down the final spin Hamiltonian. This work demonstrates the capability of Raman spectroscopy to probe the genuine two-dimensional spin dynamics in atomically-thin vdW magnets, which can provide novel insights that are obscured in bulk spin dynamics., Comment: 37 pages, 5 figures, supplementary information 11 pages

The functionality of magnetoelectric multiferroics depends on the formation, size, and coupling of their magnetic and electric domains. Knowing the parameters guiding these criteria is a key effort in the emerging field of magnetoelectric domain engineering. Here we show, using a combination of piezoresponse-force microscopy, non-linear optics, and x-ray scattering, that the correlation length setting the size of the ferroelectric domains in the multiferroic hexagonal manganites can be engineered from the micron range down to a few unit cells under the substitution of Mn$^{3+}$ ions with Al$^{3+}$ ions. The magnetoelectric coupling mechanism between the antiferromagnetic Mn$^{3+}$ order and the distortive-ferroelectric order remains intact even at substantial replacement of Mn$^{3+}$ by Al$^{3+}$. Hence, chemical substitution proves to be an effective tool for domain-size engineering in one of the most studied classes of multiferroics., Comment: 10 pages, 8 figures

Studying antiferromagnetic domains is essential for fundamental physics and potential spintronics applications. Despite its importance, few systematic studies have been performed on van der Waals (vdW) antiferromagnets (AFMs) domains with high spatial resolutions, and direct probing of the N\`eel vectors remains challenging. In this work, we found a multidomain in vdW AFM NiPS3, a material extensively investigated for its exotic magnetic exciton. We employed photoemission electron microscopy combined with the X-ray magnetic linear dichroism (XMLD-PEEM) to image the NiPS3's magnetic structure. The nanometer-spatial resolution of XMLD-PEEM allows us to determine local N\`eel vector orientations and discover thermally fluctuating N\'eel vectors that are independent of the crystal symmetry even at 65 K, well below TN of 155 K. We demonstrate a Ni ions' small in-plane orbital moment anisotropy is responsible for the weak magneto-crystalline anisotropy. The observed multidomain's thermal fluctuations may explain the broadening of magnetic exciton peaks at higher temperatures.

Magnetic-field control of fundamental optical properties is a crucial challenge in the engineering of multifunctional microdevices. Van der Waals (vdW) magnets retaining a magnetic order even in atomically thin layers, offer a promising platform for hosting exotic magneto-optical functionalities owing to their strong spin-charge coupling. Here, we demonstrate that a giant optical anisotropy can be controlled by magnetic fields in the vdW magnet FePS$_3$. The giant linear dichroism ($\sim$11%), observed below $T_{\text{N}}\!\sim\!120$ K, is nearly fully suppressed in a wide energy range from 1.6 to 2.0 eV, following the collapse of the zigzag magnetic order above 40 T. This remarkable phenomenon can be explained as a result of symmetry changes due to the spin order, enabling minority electrons of Fe$^{2+}$ to hop in a honeycomb lattice. The modification of spin-order symmetry by external fields provides a novel route for controllable anisotropic optical micro-devices., Comment: 5 pages, 4 figures

Magnetic van der Waals (vdW) materials have attracted massive attention because of their academic interest and application potential for the past few years. Its main advantage is the intrinsic two-dimensionality, enabling much smaller devices of novel concepts. One particular exciting direction lies in the current-driven spin-orbit torque (SOT). Here, we, for the first time, realize an all vdW three-terminal SOT memory, employing the unique physics principle of gigantic intrinsic SOT of Fe3GeTe2 (FGT) and the well-known industry-adopted tunnelling magnetoresistance (TMR) effect. We designed the device operation procedure and fabricated the FGT/h-BN/FGT vdW heterostructure as a proof of concept. This device exhibits a classical TMR effect and unambiguously demonstrates the conception by precise performance as expected: the magnetic information of the top-FGT is written by current-driven SOT and read out by TMR separately. The writing and reading current paths are physically decoupled, enhancing the design and optimization flexibility substantially and further strengthening the device's endurance naturally. Our work would prompt more expansive use of vdW magnets for spintronic applications., Comment: 26 pages, 7 figures, Accepted by Advanced Electronic Materials

The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS$_3$ under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a $d$-$d$ transition, we reveal a striking change in the coherent magnon's dependence on the pump polarization, indicating two distinct excitation mechanisms. Our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around sub-gap electronic states., Comment: 15 pages, 14 figures

We theoretically investigate the thermal Hall transport of magnon-polarons in a two-dimensional honeycomb antiferromagnetic insulator under the influence of a perpendicular magnetic field, varying in strength. The application of a perpendicular magnetic field induces a magnetic phase transition from the collinear antiferromagnetic phase to the spin-flop phase, leading to a significant alteration in Hall transport across the transition point. In this paper, our focus is on the intrinsic contribution to thermal Hall transport arising from the magnetoelastic interaction. To facilitate experimental verification of our theoretical results, we present the dependence of thermal Hall conductivity on magnetic field strength and temperature., Comment: 10 pages, 6 figures

Spontaneous Hall conductivity has recently been reported in the triangular lattice antiferromagnet Co$_{1/3}$TaS$_2$ under a zero magnetic field. This phenomenon originates from the distinctive noncoplanar triple-Q magnetic ground state, possessing uniform real-space Berry curvature characterized by scalar spin chirality. We investigated the physical properties of Co$_{1/3}$TaS$_2$ by judiciously controlling the composition, revealing a drastic change in its bulk properties, even by slight variations in cobalt composition, despite the same crystal structure. For $0.299 < x < 0.325$, Co$_x$TaS$_2$ keeps all the characteristics of the ground state consistent with the previous studies -- two antiferromagnetic phase transitions at $T_{N1}$ and $T_{N2} (< T_{N1})$, a large spontaneous Hall conductivity (${\sigma}_{xy} (H=0)$), and a weak ferromagnetic moment along the c-axis. However, samples with $x > 0.330$ exhibit distinct bulk properties, including the absence of both ${\sigma}_{xy} (H=0)$ and the weak ferromagnetic moment. Our neutron diffraction data reveal that Co$_x$TaS$_2$ with $x > 0.330$ develops coplanar helical magnetic order with $q_{m1} = (1/3, 0, 0)$. This is entirely different from what has been seen in $x < 0.325$, explaining the observed composition dependence., Comment: 15 pages, 4 figures, accepted for publication in Phys. Rev. B

Observations of emergent quantum phases in twisted bilayer graphene prompted a flurry of activities in van-der-Waals (vdW) materials beyond graphene. Most current twisted experiments use a so-called tear-and-stack method using a polymer called PPC. However, despite the clear advantage of the current PPC tear-and-stack method, there are also technical limitations, mainly a limited number of vdW materials that can be studied using this PPC-based method. This technical bottleneck has been preventing further development of the exciting field beyond a few available vdW samples. To overcome this challenge and facilitate future expansion, we developed a new tear-and-stack method using a strongly adhesive polycaprolactone (PCL). With similar angular accuracy, our technology allows fabrication without a capping layer, facilitating surface analysis and ensuring inherently clean interfaces and low operating temperatures. More importantly, it can be applied to many other vdW materials that have remained inaccessible with the PPC-based method. We present our results on twist homostructures made with a wide choice of vdW materials - from two well-studied vdW materials (graphene and MoS$_2$) to the first-ever demonstrations of other vdW materials (NbSe$_2$, NiPS$_3$, and Fe$_3$GeTe$_2$). Therefore, our new technique will help expand $moir\acute{e}$ physics beyond few selected vdW materials and open up more exciting developments., Comment: 26 pages, 4+7 figures, accepted to 2D Materials

Inversion symmetry breaking is critical for many quantum effects and fundamental for spin-orbit torque, which is crucial for next-generation spintronics. Recently, a novel type of gigantic intrinsic spin-orbit torque has been established in the topological van-der-Waals (vdW) magnet iron germanium telluride. However, it remains a puzzle because no clear evidence exists for interlayer inversion symmetry breaking. Here, we report the definitive evidence of broken inversion symmetry in iron germanium telluride directly measured by the second harmonic generation (SHG) technique. Our data show that the crystal symmetry reduces from centrosymmetric P63/mmc to noncentrosymmetric polar P3m1 space group, giving the three-fold SHG pattern with dominant out-of-plane polarization. Additionally, the SHG response evolves from an isotropic pattern to a sharp three-fold symmetry upon increasing Fe deficiency, mainly due to the transition from random defects to ordered Fe vacancies. Such SHG response is robust against temperature, ensuring unaltered crystalline symmetries above and below the ferromagnetic transition temperature. These findings add crucial new information to our understanding of this interesting vdW metal, iron germanium telluride: band topology, intrinsic spin-orbit torque and topological vdW polar metal states., Comment: 32 pages, 9 figures, Accepted by Advanced Materials

The thermal Hall effect in magnetic insulators has been considered a powerful method for examining the topological nature of charge-neutral quasiparticles such as magnons. Yet, unlike the kagome system, the triangular lattice has received less attention for studying the thermal Hall effect because the scalar spin chirality cancels out between adjacent triangles. However, such cancellation cannot be perfect if the triangular lattice is distorted, which could open the possibility of a non-zero thermal Hall effect. Here, we report that the trimerized triangular lattice of multiferroic hexagonal manganite YMnO$_3$ produces a highly unusual thermal Hall effect due to topological spin fluctuations with the additional intricacy of a Dzyaloshinskii-Moriya interaction under an applied magnetic field. We conclude the thermal Hall conductivity arises from the system's topological nature of spin fluctuations. Our theoretical calculations demonstrate that the thermal Hall conductivity is also related in this material to the splitting of the otherwise degenerate two chiralities, left and right, of its 120$^{\circ}$ magnetic structure. Our result is one of the most unusual cases of topological physics due to this broken $Z_2$ symmetry of the chirality in the supposedly paramagnetic state of YMnO$_3$, with strong topological spin fluctuations. These new mechanisms in this important class of materials are crucial in exploring new thermal Hall physics and exotic excitations., Comment: 14 pages, 3 figures; accepted for publication in Nature Communications

The unique discovery of magnetic exciton in van der Waals antiferromagnet NiPS3 arises between two quantum many-body states of a Zhang-Rice singlet excited state and a Zhang-Rice triplet ground state. Simultaneously, the spectral width of photoluminescence originating from this exciton is exceedingly narrow as 0.4 meV. These extraordinary properties, including the extreme coherence of the magnetic exciton in NiPS3, beg many questions. We studied doping effects using Ni1-xCdxPS3 using two experimental techniques and theoretical studies. Our experimental results show that the magnetic exciton is drastically suppressed upon a few % Cd doping. All these happen while the width of the exciton only gradually increases, and the antiferromagnetic ground state is robust. These results highlight the lattice uniformity's hidden importance as a prerequisite for coherent magnetic exciton. Finally, an exciting scenario emerges: the broken charge transfer forbids the otherwise uniform formation of the coherent magnetic exciton in (Ni,Cd)PS3., Comment: 40 pages, 4 main figures, 13 supporting figures, accepted by Nano Letters

Fe3GeTe2 (FGT), a ferromagnetic van der Waals topological nodal line semimetal, has recently been studied. Using first-principles calculations and symmetry analysis, we investigate the effect of a uniaxial tensile strain on the nodal line and the resultant intrinsic anomalous Hall effect (AHE). Our results reveal their robustness to the in-plane strain. Moreover, the intrinsic AHE remains robust even for artificial adjustment of the atomic positions introduced to break the crystalline symmetries of FGT. When the spin-orbit coupling is absent, the nodal line degeneracy remains intact as long as the inversion symmetry or the two-fold screw symmetry is maintained, which reveal that the nodal line may emerge much more easily than previously predicted. This strong robustness is surprising and disagrees with the previous experimental report [Y. Wang et al., Adv. Mater. 32, 2004533 (2020)], which reports that a uniaxial strain of less than 1 % of the in-plane lattice constant can double the anomalous Hall resistance. This discrepancy implies that the present understanding of the AHE in FGT is incomplete. The possible origins of this discrepancy are discussed., Comment: 7 pages, 3 figures

The Kitaev model, a honeycomb network of spins with bond-dependent anisotropic interactions, is a rare example of having a quantum spin liquid ground state. Although most Kitaev model candidate materials eventually order magnetically due to inevitable non-Kitaev terms, their bond-dependent anisotropy manifests in unusual spin dynamics. It has recently been suggested that bond-dependent anisotropy can stabilise novel magnetic phases and exotic spin dynamics on the geometrically frustrated triangular lattice. However, few materials have been identified with simultaneous geometric frustration and bond-dependent anisotropy. Here, we report a frustrated triangular lattice with bond-dependent anisotropy in the cobalt-based triangular van der Waals antiferromagnet CoI2. Its momentum and energy-resolved spin dynamics exhibit substantial magnon breakdown and complex level repulsion, as measured by inelastic neutron scattering. A thorough examination of excitations in both the paramagnetic and magnetically ordered states reveals that the bond-dependent anisotropy is the origin of the spiral order and the magnon breakdown found in CoI2. Our result paves the way toward a new research direction for the Kitaev model with geometrical frustration., Comment: 13 pages, 4 figures, Nature Physics

Two-dimensional (2D) Heisenberg honeycomb ferromagnets are expected to have interesting topological magnon effects as their magnon dispersion can have Dirac points. The Dirac points are gapped with finite second nearest neighbor Dzyaloshinskii-Moriya interaction, providing nontrivial Berry curvature with finite magnon Hall effect. Yet, it is unknown how the topological properties are affected by magnon damping. We report the thermal Hall effect in Cr$_2$Ge$_2$Te$_6$, an insulating 2D honeycomb ferromagnet with a large Dirac magnon gap and significant magnon damping. Interestingly, the thermal Hall conductivity in Cr$_2$Ge$_2$Te$_6$ shows the coexisting phonon and magnon contributions. Using an empirical two-component model, we successfully estimate the magnon contribution separate from the phonon part, revealing that the magnon Hall conductivity was 20 times smaller than the theoretical calculation. Finally, we suggest that such considerable suppression in the magnon Hall conductivity is due to the magnon damping effect in Cr$_2$Ge$_2$Te$_6$., Comment: 15 pages, 3 figures. Accepted for publication in Phys. Rev. B

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin-lattice coupling in a vdW antiferromagnet FePS$_{3}$ that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS$_{3}$ selectively couples to the trigonal distortions through partially filled t$_{2g}$ orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin-lattice coupling in FePS$_3$, but also establish phase-resolved CPS as a tool to investigate hidden interactions., Comment: 6 pages, 4 figures

The triangular lattice antiferromagnet (TLAF) has been the standard paradigm of frustrated magnetism for several decades. The most common magnetic ordering in insulating TLAFs is the 120 structure. However, a new triple-Q chiral ordering can emerge in metallic TLAFs, representing the short wavelength limit of magnetic skyrmion crystals. We report the metallic TLAF Co1/3TaS2 as the first example of tetrahedral triple-Q magnetic ordering with the associated topological Hall effect (non-zero {\sigma}_{xy}(H=0)). We also present a theoretical framework that describes the emergence of this magnetic ground state, which is further supported by the electronic structure measured by angle-resolved photoemission spectroscopy. Additionally, our measurements of the inelastic neutron scattering cross section are consistent with the calculated dynamical structure factor of the tetrahedral triple-Q state., Comment: 23 pages, 4 figures, SI not included. Accepted for publication in Nature Communications

We report a comprehensive spin wave analysis of the semiconducting honeycomb van der Waal antiferromagnet NiPS$_3$. Using single crystal inelastic neutron scattering, we map out the full Brillouin zone and fit the observed modes to a spin wave model with rigorously defined uncertainty. We find that the third neighbor exchange $J_3$ dominates the Hamiltonian, a feature which we fully account for by ab-initio density functional theory calculations. We also quantify the degree to which the three-fold rotation symmetry is broken and account for the $Q=0$ excitations observed in other measurements, yielding a spin exchange model which is consistent across multiple experimental probes. We also identify a strongly reduced static ordered moment and reduced low-energy intensity relative to the linear spin wave calculations, signaling unexplained features in the magnetism which requires going beyond the linear spin wave approximation., Comment: 7 pages, 8 figures; 8 pages and 10 additional figures of appendices

The spin waves in single crystals of the layered van der Waals antiferromagnet CoPS$_3$ have been measured using inelastic neutron scattering. The data show four distinct spin wave branches with large ($\gtrsim 14$ meV) energy gaps at the Brillouin zone center indicating significant anisotropy. The data were modelled using linear spin wave theory derived from a Heisenberg Hamiltonian. Exchange interactions up to the third nearest-neighbour in the layered planes were required to fit the data with ferromagnetic $J_1 = -1.37$ meV between first neighbours, antiferromagnetic $J_3 = 3.0$ meV between third neighbours, and a very small $J_2 = 0.09$ meV between second neighbours. A biaxial single-ion anisotropy was required, with a collinear term $D^x = -0.77$ meV for the axis parallel to the aligned moment direction and a coplanar term $D^z=6.07$ meV for an axis approximately normal to the layered crystal planes., Comment: 11 pages, 6 figures, 3 tables

Van der Waals (vdW) magnets are an ideal platform for tailoring two-dimensional (2D) magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. We used X-ray photoemission electron microscopy to address the electronic and magnetic properties of the vdW antiferromagnet FePS3 down to the monolayer. Our experiments reveal a giant out-of-plane magnetic anisotropy of 22 meV per Fe ion, accompanied by unquenched magnetic orbital moments. Moreover, our calculations suggest that the Ising magnetism in FePS3 is a visible manifestation of spin-orbit entanglement of the Fe 3d electron system.

Kitaev physics has recently attracted attention in condensed matter for its anticipated novel quantum spin liquid state. The thermal transport measurement is crucial for probing the novel features of charge-neutral quasiparticles. In this letter, we report a significant thermal Hall effect in $Na_2Co_2TeO_6$ (NCTO), a Kitaev quantum spin liquid candidate, when the magnetic field is applied along the out-of-plane direction of the honeycomb plane. The thermal conductivity ($\kappa_{xx}$) and thermal Hall conductivity ($\kappa_{xy}$) in NCTO reveal distinct magnetic field dependences below and above the Neel temperature ($T_N$) of 27 K. For $T>T_N$, $\kappa_{xx}$ has a monotonic decrease in the field dependence, while $\kappa_{xy}$ persists up to $T^*$ = 150 K. On the other hand, both $\kappa_{xx}$ and $\kappa_{xy}$ exhibit complex field dependence for $T

Strong periodic driving with light offers the potential to coherently manipulate the properties of quantum materials on ultrafast timescales. Recently, strategies have emerged to drastically alter electronic and magnetic properties by optically inducing non-trivial band topologies, emergent spin interactions and even superconductivity. However, the prospects and methods of coherently engineering optical properties on demand are far less understood. Here we demonstrate coherent control and giant modulation of optical nonlinearity in a van der Waals layered magnetic insulator, manganese phosphorus trisulfide (MnPS$_3$). By driving far off-resonance from the lowest on-site manganese $d$-$d$ transition, we observe a coherent on-off switching of its optical second harmonic generation efficiency on the timescale of 100 femtoseconds with no measurable dissipation. At driving electric fields of the order of 10$^9$ volts per metre, the on-off ratio exceeds 10, which is limited only by the sample damage threshold. Floquet theory calculations based on a single-ion model of MnPS$_3$ are able to reproduce the measured driving field amplitude and polarization dependence of the effect. Our approach can be applied to a broad range of insulating materials and could lead to dynamically designed nonlinear optical elements., Comment: 5 pages main text, 4 figures, 22 pages supplementary information

The coupling between phonon and magnon is ubiquitous in magnetic materials and plays a crucial role in many aspects of magnetic properties, most notably in spintronics. Yet, this academically and technologically interesting problem still poses a severe challenge to a general understanding of the issue in certain materials. We report that Ni3TeO6 exhibits clear evidence of significant magnon-phonon coupling in both longitudinal thermal conductivity ($\kappa_{xx}$) and thermal Hall coefficient ($\kappa_{xy}$). The Debye-Callaway model, a phenomenological description for phonon heat conduction, can explain the measured magnetic field dependence of $\kappa_{xx}(H)$: phonon scattering from spin fluctuation in the paramagnetic phase and additional scattering due to magnon-phonon coupling in the collinear antiferromagnetic phase. We further suggest that a similar approach could be applied to understand the finite $\kappa_{xy}$ values in $Ni_3TeO_6$., Comment: 20 pages, 5 figures, 1 table. Accepted for publication as a Regular Article in Physical Review B

In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character. Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra. Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS3. These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the N\'eel temperature and become accessible with magnetic order. By launching this phonon and spectrally tracking its amplitude, we establish the electronic origin of bound states as localized d-d excitations. Our data directly yield electron-phonon coupling strength which exceeds the highest known value in 2D systems. These results demonstrate NiPS3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets.

Combining magnetism with band topology provides various novel phases that are otherwise impossible. Among several cases, noncollinear metallic antiferromagnets can reveal particularly rich topological physics due to their diverse magnetic ground states. However, there are only a few experimental studies due to the lack of suitable materials, especially with triangular lattice antiferromagnets. Here, we report that metallic triangular antiferromagnet Co1/3TaS2 exhibits a substantial anomalous Hall effect (AHE) related to its noncollinear magnetic order. Our first-principles calculations found that hourglass Weyl fermions from the non-symmorphic symmetry trigger AHE. We further show that AHE in Co1/3TaS2 can be characterized by the toroidal moment, a vortex-like multipole component that arises from a combination of chiral lattice and geometrical frustration. Finally, the unusual field-tunability of the toroidal moment puts Co1/3TaS2 as a rare example of a noncollinear metallic antiferromagnet filled with interesting magnetic and topological properties., Comment: 20 pages, 4 figures, Accepted for publication in npj Quantum Materials

How particular bonds form in quantum materials has been a long-standing puzzle. Two key concepts dealing with charge degrees of freedom are dimerization (forming metal-metal bonds) and charge ordering (CO). Since the 1930s, these two concepts have been frequently invoked to explain numerous exciting quantum materials, typically insulators. Here we report dimerization and CO within the dimers coexisting in metallic NaRu$_2$O$_4$. By combining high-resolution x-ray diffraction studies and theoretical calculations, we demonstrate that this unique phenomenon occurs through a new type of bonding, which we call Z-type ordering. The low-temperature superstructure has strong dimerization in legs of zigzag ladders, with short dimers in legs connected by short zigzag bonds, forming Z-shape clusters: simultaneously, site-centered charge ordering also appears. Our results demonstrate the yet unknown flexibility of quantum materials with the intricate interplay among orbital, charge, and lattice degrees of freedom., Comment: 37 pages, 9 figures, 4 tables

Matter-light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, we report that the broken inversion symmetry of multiferroicity can act as an external knob enabling the magnetic exciton in van der Waals antiferromagnet NiI2. We further discover that this magnetic exciton arises from a transition between Zhang-Rice-triplet and Zhang-Rice-singlet's fundamentally quantum entangled states. This quantum entanglement produces an ultra-sharp optical exciton peak at 1.384 eV with a 5 meV linewidth. Our work demonstrates that NiI2 is two-dimensional magnetically ordered with an intrinsically quantum entangled ground state., Comment: 26 pages, 10 figures. Accepted for publication in Advanced Materials

We report unidirectional charge transport in a $\mathrm{NbSe_2}$ noncentrosymmetric superconductor, which is exchange-coupled with a $\mathrm{CrPS_4}$ van der Waals layered antiferromagnetic insulator. The $\mathrm{NbSe_2/CrPS_4}$ bilayer device exhibits bias-dependent superconducting critical-current variations of up to $16\%$, with the magnetochiral anisotropy reaching $\sim 10^5\mathrm{\ T^{-1}A^{-1}}$. Furthermore, the $\mathrm{CrPS_4/NbSe_2/CrPS_4}$ spin-valve structure exhibits the superconducting diode effect with critical-current variations of up to $40\%$. We also utilize the magnetic proximity effect to induce switching in the superconducting state of the spin-valve structure. It exhibits an infinite magnetoresistance ratio depending on the field sweep direction and magnetization configuration. Our result demonstrates a novel route for enhancing the nonreciprocal response in the weak external field regime ($<50\mathrm{\ mT}$) by exploiting the magnetic proximity effect., Comment: 25 pages, 3 figures, 2 supplemental figures

Ferromagnetism in two-dimensional materials presents a promising platform for the development of ultrathin spintronic devices with advanced functionalities. Recently discovered ferromagnetic van der Waals crystals such as CrI$_{3}$, readily isolated two-dimensional crystals, are highly tunable through external fields or structural modifications. However, there remains a challenge because of material instability under air exposure. Here, we report the observation of an air stable and layer dependent ferromagnetic (FM) van der Waals crystal, CrPS$_{4}$, using magneto-optic Kerr effect microscopy. In contrast to the antiferromagnetic (AFM) bulk, the FM out-of-plane spin orientation is found in the monolayer crystal. Furthermore, alternating AFM and FM properties observed in even and odd layers suggest robust antiferromagnetic exchange interactions between layers. The observed ferromagnetism in these crystals remains resilient even after the air exposure of about a day, providing possibilities for the practical applications of van der Waals spintronics., Comment: 22 pages, 5 figures

In this paper, we present a 5.8 GHz radio-frequency (RF) wireless power transfer (WPT) system that consists of 64 transmit antennas and 16 receive antennas. Unlike the inductive or resonant coupling-based near-field WPT, RF WPT has a great advantage in powering low-power internet of things (IoT) devices with its capability of long-range wireless power transfer. We also propose a beam scanning algorithm that can effectively transfer the power no matter whether the receiver is located in the radiative near-field zone or far-field zone. The proposed beam scanning algorithm is verified with a real-life WPT testbed implemented by ourselves. By experiments, we confirm that the implemented 5.8 GHz RF WPT system is able to transfer 3.67 mW at a distance of 25 meters with the proposed beam scanning algorithm. Moreover, the results show that the proposed algorithm can effectively cover radiative near-field region differently from the conventional scanning schemes which are designed under the assumption of the far-field WPT.

Magnetite (Fe3O4) is of fundamental importance as the original magnetic material and also for the Verwey transition near T_V = 125 K, below which a complex lattice distortion and electron orders occur. The Verwey transition is suppressed by strain or chemical doping effects giving rise to well-documented first and second-order regimes, but the origin of the order change is unclear. Here, we show that slow oxidation of monodisperse Fe3O4 nanoparticles leads to an intriguing variation of the Verwey transition that elucidates the doping effects. Exposure to various fixed oxygen pressures at ambient temperature leads to an initial drop to TV minima as low as 70 K after 45-75 days, followed by recovery to a constant value of 95 K after 160 days that persists in all experiments for aging times up to 1070 days. A physical model based on both doping and doping-gradient effects accounts quantitatively for this evolution and demonstrates that the persistent 95 K value corresponds to the lower limit for homogenously doped magnetite and hence for the first order regime. In comparison, further suppression down to 70 K results from inhomogeneous strains that characterize the second-order region. This work demonstrates that slow reactions of nanoparticles can give exquisite control and separation of homogenous and inhomogeneous doping or strain effects on an nm scale and offers opportunities for similar insights into complex electronic and magnetic phase transitions in other materials., Comment: 24 pages, 13 figures, 2 tables, the manuscript is accepted for publishing at Nature Communications

Robust multi-level spin memory with the ability to write information electrically is a long-sought capability in spintronics, with great promise for applications. Here we achieve nonvolatile and highly energy-efficient magnetization switching in a single-material device formed of van-der-Waals topological ferromagnet Fe3GeTe2, whose magnetic information can be readily controlled by a tiny current. Furthermore, the switching current density and power dissipation are about 400 and 4000 times smaller than those of the existing spin-orbit-torque magnetic random access memory based on conventional magnet/heavy-metal systems. Most importantly, we also demonstrate multi-level states, switched by electrical current, which can dramatically enhance the information capacity density and reduce computing costs. Thus, our observations combine both high energy efficiency and large information capacity density in one device, showcasing the potential applications of the emerging field of van-der-Waals magnets in the field of spin memory and spintronics., Comment: Accepted by Advanced Functional Materials; 28 pages, 5 main figures, 4 supporting figures

Controlling magnetic states by a small current is essential for the next-generation of energy-efficient spintronic devices. However, it invariably requires considerable energy to change a magnetic ground state of intrinsically quantum nature governed by fundamental Hamiltonian, once stabilized below a phase transition temperature. We report that surprisingly an in-plane current can tune the magnetic state of nm-thin van der Waals ferromagnet Fe3GeTe2 from a hard magnetic state to a soft magnetic state. It is the direct demonstration of the current-induced substantial reduction of the coercive field. This surprising finding is possible because the in-plane current produces a highly unusual type of gigantic spin-orbit torque for Fe3GeTe2. And we further demonstrate a working model of a new nonvolatile magnetic memory based on the principle of our discovery in Fe3GeTe2, controlled by a tiny current. Our findings open up a new window of exciting opportunities for magnetic van der Waals materials with potentially huge impacts on the future development of spintronic and magnetic memory., Comment: 61 pages, 4 main figures, 14 supporting figures

The realization of Kitaev's honeycomb magnetic model in real materials has become one of the most pursued topics in condensed matter physics and materials science. If found, it is expected to host exotic quantum phases of matter and offers potential realizations of fault$-$tolerant quantum computations. Over the past years, much effort was made on 4d$-$ or 5d$-$ heavy transition metal compounds because of their intrinsic strong spin$-$orbit coupling. But more recently, there have been growing shreds of evidence that the Kitaev model could also be realized in 3d$-$transition metal systems with much weaker spin$-$orbit coupling. This review intends to serve as a guide to this fast$-$developing field focusing on systems with d$^7$ transition metal occupation. It overviews the current theoretical and experimental progress on realizing the Kitaev model in those systems. We examine the recent experimental observations of candidate materials with Co$^{2+}$ ions: e.g., CoPS$_3$, Na$_3$Co$_2$SbO$_6$, and Na$_2$Co$_2$TeO$_6$, followed by a brief review of theoretical backgrounds. We conclude this article by comparing experimental observations with density functional theory (DFT) calculations. We stress the importance of inter$-t_{2g}$ hopping channels and Hund's coupling in the realization of Kitaev interactions in Co$-$based compounds, which has been overlooked in previous studies. This review suggests future directions in the search for Kitaev physics in 3d cobalt compounds and beyond., Comment: 45 pages, 13 figures, accepted as Topical Review in Journal of Physics: Condensed Matter

Collective excitations of bound electron-hole pairs -- known as excitons -- are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS$_3$ by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and the long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism., Comment: 24 pages, 23 figures