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Quantum magnetism in the frustrated square lattice oxyhalides YbBi 2 IO 4 and YbBi 2 ClO 4

Square-lattice systems offer a direct route for realizing two-dimensional (2D) quantum magnetism with frustration induced by competing interactions. In this work, the square lattice materials YbBi 2 IO 4 and YbBi 2 ClO 4 were investigated using a combination of magnetization and specific-heat measurements on polycrystalline samples. Specific-heat measurements provide evidence for long-range magnetic order below $T$ N = 0.21 K (0.25 K) for YbBi 2 IO 4 (YbBi 2 ClO 4 ). On the other hand, a rather broad maximum is found in the temperature-dependent magnetic susceptibility, located at $T$ max = 0.33 K (0.38 K) in YbBi 2 IO 4 (YbBi 2 ClO 4 ), consistent with the quasi-2D magnetism expected for the large separation between the magnetic layers. Estimation of the magnetic entropy supports the expected Kramers' doublet ground state for Yb 3+ and the observed paramagnetic behavior is consistent with a well-isolated doublet. Roughly two-thirds of the entropy is consumed above $T$ N , due to a combination of the quasi-2D behavior and magnetic frustration. The impact of frustration is examined from the viewpoint of a simplified $J$ 1 -$J$ 2 square lattice model, which is frustrated for antiferromagnetic interactions. Specifically, a high-temperature series expansion analysis of the temperature-dependent specific-heat and magnetization data yields $J$ 2 /$J$ 1 = 0.30 (=0.23) for YbBi 2 IO 4 (YbBi 2 ClO 4 ). In conclusion, this simplified analysis suggests strong frustration that should promote significant quantum fluctuations in these compounds, and thus motivates future work on the static and dynamic magnetic properties of these materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Non-Equilibrium Effects in Quantum Magnets

While most often the state of a material will tend toward an equilibrium determined by its environment, there are many cases of scientific and technological interest where materials are manipulated to be or are found in non-equilibrium configurations. For example, data can be stored in hard drives by deliberately altering the magnetic orientation in a material to store information in non-equilibrium pattern. In this project, the main goals were studies of non-equilibrium properties of quantum magnets using neutron scattering as the primary experimental method. Neutron scattering allows characterization of magnetic correlation lengths sensitive to the presence of defects. It can also be used to distinguish equilibrium from non-equilibrium states via energy transfer rates. Typical bulk state magnetization relaxation times are too short to perform many neutron scattering measurements of interest. To enable the study of non-equilibrium conditions, materials with longer magnetic relaxation times were targeted. CoNb 2 O 6 was used in two experiments related to non-equilibrium physics. In the first, evidence for defects created via the Kibble-Zurek mechanism (KZM) was sought by quenching across a magnetic field-dependent phase transition. Somewhat unexpectedly, clear evidence for KZM-induced defects was absent. Additional measurements of CoNb 2 O 6 were made to better characterize its crystal field and other properties to provide a better theoretical understanding to enable more effective non-equilibrium physics measurements. In another project, LiHo 0.45 Y 0.55 F 4 was used to compare a quantum annealing protocol to a thermal annealing one since magnetic fields can be used to control the thermal fluctuations in LiHo 0.45 Y 0.55 F 4 . In addition, a new pulsed magnet power supply and new techniques were developed suitable for neutron scattering experimental environments to enable faster magnetic field changes for producing non-equilibrium conditions. The power supply developed for this project has wider technological applications in addition to faster magnetic field ramps.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Proximity-magnetized quantum spin Hall insulator: monolayer 1 T’ WTe2/Cr2Ge2Te6

Abstract Van der Waals heterostructures offer great versatility to tailor unique interactions at the atomically flat interfaces between dissimilar layered materials and induce novel physical phenomena. By bringing monolayer 1 T’ WTe 2 , a two-dimensional quantum spin Hall insulator, and few-layer Cr 2 Ge 2 Te 6 , an insulating ferromagnet, into close proximity in an heterostructure, we introduce a ferromagnetic order in the former via the interfacial exchange interaction. The ferromagnetism in WTe 2 manifests in the anomalous Nernst effect, anomalous Hall effect as well as anisotropic magnetoresistance effect. Using local electrodes, we identify separate transport contributions from the metallic edge and insulating bulk. When driven by an AC current, the second harmonic voltage responses closely resemble the anomalous Nernst responses to AC temperature gradient generated by nonlocal heater, which appear as nonreciprocal signals with respect to the induced magnetization orientation. Our results from different electrodes reveal spin-polarized edge states in the magnetized quantum spin Hall insulator.

36 MATERIALS SCIENCE↗

Floquet engineering of Kitaev quantum magnets

Abstract In recent years, there has been an intense search for materials realizing the Kitaev quantum spin liquid model. A number of edge-shared compounds with strong spin-orbit coupling, such as RuCl 3 and iridates, have been proposed to realize this model. Nevertheless, an effective spin Hamiltonian derived from the microscopic model relevant to these compounds generally contains terms that are antagonistic toward the quantum spin liquid. This is consistent with the fact that the zero magnetic field ground state of these materials is generally magnetically ordered. It is a pressing issue to identify protocols to drive the system to the limit of the Kitaev quantum spin model. In this work, we propose Floquet engineering of these Kitaev quantum magnets by coupling materials to a circularly polarized laser. We demonstrate that all the magnetic interactions can be tuned in situ by the amplitude and frequency of the laser, hence providing a route to stabilize the Kitaev quantum spin liquid phase.

36 MATERIALS SCIENCE↗

Revealing room temperature ferromagnetism in exfoliated Fe 5 GeTe 2 flakes with quantum magnetic imaging

Van der Waals (vdW) material Fe 5 GeTe 2 , with its long-range ferromagnetic ordering near room temperature, has significant potential to become an enabling platform for implementing novel spintronic and quantum devices. To pave the way for applications, it is crucial to determine the magnetic properties when the thickness of Fe 5 GeTe 2 reaches the few-layers regime. However, this is highly challenging due to the need for a characterization technique that is local, highly sensitive, artifact-free, and operational with minimal fabrication. Prior studies have indicated that Curie temperature T C can reach up to close to room temperature for exfoliated Fe 5 GeTe 2 flakes, as measured via electrical transport; there is a need to validate these results with a measurement that reveals magnetism more directly. Here, we investigate the magnetic properties of exfoliated thin flakes of vdW magnet Fe 5 GeTe 2 via quantum magnetic imaging technique based on nitrogen vacancy centers in diamond. Through imaging the stray fields, we confirm room-temperature magnetic order in Fe 5 GeTe 2 thin flakes with thickness down to 7 units cell. The stray field patterns and their response to magnetizing fields with different polarities is consistent with previously reported perpendicular easy-axis anisotropy. Furthermore, we perform imaging at different temperatures and determine the Curie temperature of the flakes at ≈300 K. These results provide the basis for realizing a room-temperature monolayer ferromagnet with Fe 5 GeTe 2 . This work also demonstrates that the imaging technique enables rapid screening of multiple flakes simultaneously as well as time-resolved imaging for monitoring time-dependent magnetic behaviors, thereby paving the way towards high throughput characterization of potential two-dimensional (2D) magnets near room temperature and providing critical insights into the evolution of domain behaviors in 2D magnets due to degradation.

2D magnet↗

Light-wave control of correlated materials using quantum magnetism during time-periodic modulation of coherent transport

Light–wave quantum electronics utilizes the oscillating carrier wave to control electronic properties with intense laser pulses. Without direct light–spin interactions, however, magnetic properties can only be indirectly affected by the light electric field, mostly at later times. A grand challenge is how to establish a universal principle for quantum control of charge and spin fluctuations, which can allow for faster-than-THz clock rates. Using quantum kinetic equations for the density matrix describing non–equilibrium states of Hubbard quasiparticles, here we show that time–periodic modulation of electronic hopping during few cycles of carrier–wave oscillations can dynamically steer an antiferromagnetic insulating state into a metalic state with transient magnetization. While nonlinearities associated with quasi-stationary Floquet states have been achieved before, magneto–electronics based on quasiparticle acceleration by time–periodic multi–cycle fields and quantum femtosecond/attosecond magnetism via strongly–coupled charge–spin quantum excitations represents an alternative way of controlling magnetic moments in sync with quantum transport.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Magnetoelectronic phenomena due to quantum magnetization fluctuations

The goal of the project was to identify techniques to study magnetoelectronic phenomena such as spin transfer (ST) that stem from the quantum-mechanical nature of magnetization, and utilize them to characterize these quantum phenomena. The first such technique, electronic measurements based on the dependence of resistance on the population of spin-wave quanta (magnons) in a magnetic nanostructure, was shown by detailed measurements to be significantly influenced by the current-driven generation of a highly nonequilibrium phonon distribution by electrical current. This previously unrecognized phenomenon adds to the understanding of current-induced heating phenomena, qualitatively changes the methodology of analysis of current-induced heating common in scientific studies and engineering of current-carrying nanostructures. It benefits the public by providing a new direction for mitigation of Joule heating effects in electronic devices. The project also included quantum simulations of current-induced effects in magnetic nanostructures, which revealed that linear momentum and energy conservation are important for ST. Only angular momentum conservation was previously believed to be important. This finding is important for the fundamental understanding of ST, and for the design of efficient magnetoelectronic devices taking advantage of these conservation laws. Simulations also showed that non-classical ST is dominant in antiferromagnets, which will transform the understanding of ST in these systems. Finally, experimental studies of spin-transfer in ultrathin transition metal films revealed very large non-classical effects which were traced to the quantum origins of magnetism associated in the studied systems with the formation of an orbital liquid state. These findings i) transform the understanding of "conventional" transition-metal magnetism, ii) open a new field of studies in magnetism and a new method for the electronic control of magnetic properties and magnetism itself, and iii) provide a new approach to the development of efficient magnetoelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Witnessing entanglement in quantum magnets using neutron scattering

We demonstrate how quantum entanglement can be directly witnessed in the quasi-1D Heisenberg antiferromagnet KCuF 3 . We apply three entanglement witnesses—one tangle, two tangle, and quantum Fisher information—to its inelastic neutron spectrum and compare with spectra simulated by finite-temperature density matrix renormalization group (DMRG) and classical Monte Carlo methods. We find that each witness provides direct access to entanglement. Of these, quantum Fisher information is the most robust experimentally and indicates the presence of at least bipartite entanglement up to at least 50 K, corresponding to around 10% of the spinon zone-boundary energy. We apply quantum Fisher information to higher spin-S Heisenberg chains and show theoretically that the witnessable entanglement gets suppressed to lower temperatures as the quantum number increases. Finally, we outline how these results can be applied to higher dimensional quantum materials to witness and quantify entanglement.

1-dimensional systems↗

Spinon excitations and spin correlations in the one-dimensional quantum magnet β -VOSO 4 probed by Raman spectroscopy

Fractionalized excitations such as spinons and anyons have emerged as a central theme in condensed matter physics with broad implications for superconductivity, quantum statistics, and quantum computation. The nearly ideal one-dimensional S = 1/2 system β-VOSO 4 without long-range order down to 85 mK provides a promising platform to experimentally explore such fractionalized excitations. Here, we employ Raman spectroscopy to probe magnetic excitations and the evolution of spin correlations in β-VOSO 4 . Spinon signatures are found along the chain direction, evidenced by a broad, gapless scattering continuum at low temperatures. The temperature dependence of the spinon spectral weight aligns considerably with numerical density matrix renormalization group calculations. By comparing the experimental spinon spectral weight with calculated results and evaluating the associated quantum Fisher information (QFI) therefrom, we observe a steep increase in QFI upon cooling, indicating rapidly growing correlation lengths. Our study showcases QFI as a probe of spin correlations in quantum magnets.

Wulferding, Dirk [Sejong Univ., Seoul (Korea, Repu↗

Quantifying and Controlling Entanglement in the Quantum Magnet Cs 2 CoCl 4

The lack of methods to experimentally detect and quantify entanglement in quantum matter impedes our ability to identify materials hosting highly entangled phases, such as quantum spin liquids. We thus investigate the feasibility of using inelastic neutron scattering (INS) to implement a model-independent measurement protocol for entanglement based on three entanglement witnesses: one-tangle, two-tangle, and quantum Fisher information (QFI). We perform high-resolution INS measurements on Cs 2 CoCl 4 , a close realization of the S = 1/2 transverse-field XXZ spin chain, where we can control entanglement using the magnetic field, and compare with density-matrix renormalization group calculations for validation. The three witnesses allow us to infer entanglement properties and make deductions about the quantum state in the material. Overall, we find QFI to be a particularly robust experimental probe of entanglement, whereas the one and two-tangles require more careful analysis. Our results lay the foundation for a general entanglement detection protocol for quantum spin systems.

1-dimensional spin chains↗

Transitions, Dynamics, and Driven States in Quantum Magnets (Final Report Revised)

Transitions into unusual electronic, optical, and magnetic states at the absolute zero of temperature display special properties that teach us about fundamental quantum mechanics and also underlie important technologies. These so-called quantum phase transitions intertwine the static and dynamical responses of the materials changing state. They are extremely sensitive to the effects of disorder and etch in high relief the role of quantum fluctuations. There are ample questions remaining about the character of such transitions and the nature of the competing quantum states. There are also opportunities to drive quantum materials out of equilibrium, with the possibility of new types of correlated and coherent order, and new ways to access the dynamical evolution of ground and excited states. We have investigated how the order develops in time and space, and the nature of the final configurations. We are able to compare and contrast classical and quantum excitations in our experimental system of choice, and thereby can trace the relative speed by which the system settles into its lowest-energy ground state. This comparison of quantum and classical annealing protocols lies at the heart of strategies for harnessing the power of quantum computers dedicated to optimization problems. A combination of magnetic susceptibility measurements at finite frequency where the magnetic spins are queried by an external ac field, dc magnetometry measurements that characterize the macroscopic strength of magnetic order and its resistance to change, noise measurements that reveal the microscopic fluctuations of the spins as they prepare to change state, and microwave spectroscopy to look at the response of both the electronic and nuclear degrees of freedom, have been performed as functions of temperature, magnetic field, frequency, excitation amplitude, magnetic spin concentration, and disorder. This combination of probes addresses issues of stability over time, overlap between spin states, the ability of the spins to respond independently or coherently, and the promise of control on the nanometer length scale. The research reported here provides insights into fundamental quantum physics. It also addresses the question of how best to use complex systems, such as magnetic solids, to stably process quantum information.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Inductance meets memory in a quantum magnet

Orbital degrees of freedom offer a largely untapped route to emergent dynamical phenomena in correlated quantum materials. However, it remains unclear whether collective orbital states can intrinsically generate both reactive and memory functionalities in a bulk system. Here we show that in the ferrimagnet Mn₃Si₂Te₆, nonequilibrium reconfiguration of chiral orbital currents produces both emergent inductance and nonvolatile memristance as intrinsic properties of a single crystal. At low frequency and under a magnetic field along the c axis, coherent orbital-current domains generate robust clockwise inductive I-V loops. At higher frequency and low field, current-driven first-order reconfiguration leads to incomplete reversal and metastable trapping, producing an intrinsic electromotive force and a finite remanent voltage at zero current. These results establish orbital currents as a class of quantum state variables that encode both reactive and memory functionalities, opening routes toward intrinsically reconfigurable and energy-efficient electronic systems.

Cao, Tristan [University of Colorado, Boulder]↗

Robust Kagome Electronic Structure in Topological Quantum Magnets XMn 6 Sn 6 (X = Dy, Tb, Gd, Y)

Crystal geometry can greatly influence the emergent properties of quantum materials. As an example, the kagome lattice is an ideal platform to study the rich interplay between topology, magnetism, and electronic correlation. In this work, combining high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structure of XMn 6 Sn 6 (X=Dy,Tb,Gd,Y) family compounds. Here, we observe the Dirac fermion and the flat band arising from the magnetic kagome lattice of Mn atoms. Interestingly, the flat band locates in the same energy region in all compounds studied, regardless of their different magnetic ground states and 4f electronic configurations. These observations suggest a robust Mn magnetic kagome lattice across the XMn 6 Sn 6 family, thus providing an ideal platform for the search for, and investigation of, new emergent phenomena in magnetic topological materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Structural tweaking of 2D quantum magnetism

Here, a combination of tunnelling spectroscopy, magnetotransport, electron diffraction and ab initio calculations have revealed that picometre-scale lattice distortions reverse magnetic anisotropy and enhance magnetic frustration in atomically thin ruthenium trichloride — a key step towards realizing a quantum spin liquid in the two-dimensional limit.

36 MATERIALS SCIENCE↗

Universal spin dynamics in infinite-temperature one-dimensional quantum magnets

Here, we address the nature of spin dynamics in various integrable and non-integrable, isotropic and anisotropic quantum spin-$S$ chains, beyond the paradigmatic $S=1/2$ Heisenberg model. In particular, we investigate the algebraic long-time decay $\propto t^{-1/z}$ of the spin-spin correlation function at infinite temperature, using state-of-the-art simulations based on tensor network methods. We identify three universal regimes for the spin transport, independent of the exact microscopic model: (i) superdiffusive with $z=3/2$, as in the Kardar-Parisi-Zhang universality class, when the model is integrable with extra symmetries such as spin isotropy that drive the Drude weight to zero, (ii) ballistic with $z=1$ when the model is integrable with a finite Drude weight, and (iii) diffusive with $z=2$ with easy-axis anisotropy or without integrability, at variance with previous observations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Defect-induced displacement of topological surface state in quantum magnet MnBi2Te4

The topological magnet MnBi2⁢Te4 (MBT), with gapped topological surface state, is an attractive platform for realizing quantum anomalous Hall and axion insulator states. However, the experimentally observed surface state gaps fail to meet theoretical predictions, although the exact mechanism behind the gap suppression has been debated. Recent theoretical studies suggest that intrinsic antisite defects push the topological surface state away from the MBT surface, closing its gap and making it less accessible to scanning probe experiments. Here, we report on the local effect of defects on the MBT surface states and demonstrate that high defect concentrations lead to a displacement of the surface states well into the MBT crystal, validating the theorized mechanism. The local and global influence of antisite defects on the topological surface states are studied with samples of varying defect densities by combining scanning tunneling microscopy, angle-resolved photoemission spectroscopy, and density functional theory. Our findings identify a combination of increased defect density and reduced defect spacing as the primary factors underlying the displacement of the surface states and suppression of surface gap, guiding further development of topological quantum materials.

Lupke, Felix [Carnegie Mellon University (CMU)]↗

Materializing rival ground states in the barlowite family of kagome magnets: quantum spin liquid, spin ordered, and valence bond crystal states

The spin- 1 2 kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu 4 (OH) 6 FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin- 1 2 kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of distorted and undistorted kagome triangles, for which numerical simulations predict a pinwheel va- lence bond crystal (VBC) state instead of a quantum spin liquid (QSL). The presence of interlayer spins eventually leads to an interesting pinwheel q=0 magnetic order. Partially Zn-substituted bar- lowite (Cu 3.44 Zn 0.56 (OH) 6 FBr) has an ideal kagome lattice and shows QSL behavior, indicating a surprising robustness of the QSL against interlayer impurities. The magnetic susceptibility is simi- lar to that of herbertsmithite, even though the Cu 2+ impurities are above the percolation threshold for the interlayer lattice and they couple more strongly to the nearest kagome moment. This system is a unique playground displaying QSL, VBC, and spin order, furthering our understanding of these highly competitive quantum states.

36 MATERIALS SCIENCE↗

A pyroxene-based quantum magnet with multiple magnetization plateaus

Pyroxenes (AMX 2 O 6 ) consisting of infinite one-dimensional edge-sharing MO 6 chains and bridging XO 4 tetrahedra are fertile ground for finding quantum materials. Thus, here, we have studied calcium cobalt germanate (CaCoGe 2 O 6 ) and calcium cobalt silicate (CaCoSi 2 O 6 ) crystals in depth. Heat capacity data show that the spins in both compounds are dominantly Ising-like, even after being manipulated by high magnetic fields. On cooling below the Néel temperatures, a sharp field–induced transition in magnetization is observed for CaCoGe 2 O 6 , while multiple magnetization plateaus beneath the full saturation moment are spotted for CaCoSi 2 O 6 . Our analysis shows that these contrasting behaviors potentially arise from the different electron configurations of germanium and silicon, in which the 3d orbitals are filled in the former but empty in the latter, enabling electron hopping. Thus, silicate tetrahedra can aid the interchain superexchange pathway between cobalt(II) ion centers, while germanate ones tend to block it during magnetization.

Science & Technology - Other Topics↗