Impurity Spin Research Articles

Quantifying the quantum nature of high-spin YSR excitations in transverse magnetic field.

Excitations of individual and coupled spins on superconductors provide a platform to study quantum spin impurity models as well as a pathway toward realizing topological quantum computing. Here, we characterize, using ultralow temperature scanning tunneling microscopy/spectroscopy, the Yu-Shiba-Rusinov (YSR) states of individual manganese phthalocyanine molecules with high spin on an ultrathin lead film in variable transverse magnetic field. We observe two types of YSR excitations, depending on the adsorption geometry. Using a zero-bandwidth model, we detail the role of the magnetic anisotropy, spin-spin exchange, and Kondo exchange. We illustrate that one molecular type can be treated as an individual spin, whereas the other type is best described by a coupled spin system. Using the field dependence of the YSR excitations combined with modeling, we describe the quantum phase of each excitation type. These results provide an insight into the quantum nature of YSR excitations in magnetic field and a platform to study spin impurity models on superconductors in magnetic field.

Prerelaxation in quantum, classical, and quantum-classical two-impurity models

We numerically study the relaxation dynamics of impurity-host systems, focusing on the presence of long-lived metastable states in the nonequilibrium dynamics after an initial excitation of the impurities. In generic systems, an excited impurity coupled to a large bath at zero temperature is expected to relax and approach its ground state over time. However, certain exceptional cases exhibit metastability, where the system remains in an excited state on timescales largely exceeding the typical relaxation time. We study this phenomenon for three prototypical impurity models: a tight-binding quantum model of independent spinless fermions on a lattice with two stub impurities, a classical-spin Heisenberg model with two weakly coupled classical impurity spins, and a tight-binding quantum model of independent electrons with two classical impurity spins. Through numerical integration of the fundamental equations of motion, we find that all three models exhibit similar qualitative behavior: complete relaxation for nearest-neighbor impurities and incomplete or strongly delayed relaxation for next-nearest-neighbor impurities. The underlying mechanisms leading to this behavior differ between models and include impurity-induced bound states, emergent approximately conserved local observables, and exact cancellation of local and nonlocal dissipation effects. Published by the American Physical Society 2024

Performance of quantum registers in diamond in the presence of spin impurities

Performance of quantum registers in diamond in the presence of spin impurities

Calculation of the Energy Levels for a Quantum Dot Coupled to a Fixed Spin Impurity

Calculation of the Energy Levels for a Quantum Dot Coupled to a Fixed Spin Impurity

Onset of spin entanglement in doped carbon nanotubes studied by EPR.

Nanoscale semiconductors with isolated spin impurities have been touted as promising materials for their potential use at the intersection of quantum, spin, and information technologies. Electron paramagnetic resonance (EPR) studies of spins in semiconducting carbon nanotubes have overwhelmingly focused on spins more strongly localized by sp3-type lattice defects. However, the creation of such impurities is irreversible and requires specific reactions to generate them. Shallow charge impurities, on the other hand, are more readily and widely produced by simple redox chemistry, but have not yet been investigated for their spin properties. Here, we use EPR to study p-doped (6,5) semiconducting single-wall carbon nanotubes (s-SWNTs) and elucidate the role of impurity-impurity interactions in conjunction with exchange and correlation effects for the spin behavior of this material. A quantitative comparison of the EPR signals with phenomenological modeling combined with configuration interaction electronic structure calculations of impurity pairs shows that orbital overlap, combined with exchange and correlation effects, causes the EPR signal to disappear due to spin entanglement for doping levels corresponding to impurity spacings of 14nm (at 30K). This transition is predicted to shift to higher doping levels with increasing temperature and to lower levels with increasing screening, providing an opportunity for improved spin control in doped s-SWNTs.

Differences in Kondo Splitting of Surface Quantum Systems Induced by Two Distinct Magnetic Tips: A Joint Method of DFT and HEOM.

The interactions between a magnetic tip and local spin impurities initiate unconventional Kondo phenomena, such as asymmetric suppression or even splitting of the Kondo peak. However, a lack of realistic theoretical models and comprehensive explanations for this phenomenon persists due to the complexity of the interactions. This research employs a joint method of density functional theory (DFT) and hierarchical equation of motion (HEOM) to simulate and contrast the modulation of the spin state and Kondo behavior in the Fe/Cu(100) system with two distinct magnetic tips. A cobalt tip, possessing a larger magnetic moment, incites greater atomic displacement of the iron atom, more notable alterations in electronic structure, and enhanced charge transfer with the environment compared with the control process utilizing a nickel tip. Furthermore, the Kondo resonance undergoes asymmetric splitting as a result of the ferromagnetic correlation between the iron atom and the magnetic tip. The Co tip's higher spin polarization results in a wider spacing between the splitting peaks. This investigation underscores the precision of the DFT + HEOM approach in predicting complex quantum phenomena and explaining the underlying physical principles. This provides valuable theoretical support for developing more sophisticated quantum regulation experiments.

Concurrence of directional Kondo transport and incommensurate magnetic order in the layered material AgCrSe2

In this work, we report on the concurrent emergence of the directional Kondo behavior and incommensurate magnetic ordering in a layered material. We employ temperature- and magnetic field-dependent resistivity measurements, susceptibility measurements, and high resolution wavelength X-ray diffraction spectroscopy to study the electronic properties of AgCrSe2. Impurity Kondo behavior with a characteristic temperature of TK = 32 K is identified through quantitative analysis of the in-plane resistivity, substantiated by magneto-transport measurements. The excellent agreement between our experimental data and the Schlottmann’s scaling theory allows us to determine the impurity spin as S = 3/2. Furthermore, we discuss the origin of the Kondo behavior and its relation to the material’s antiferromagnetic transition. Our study uncovers a rare phenomenon—the equivalence of the Néel temperature and the Kondo temperature—paving the way for further investigations into the intricate interplay between impurity physics and magnetic phenomena in quantum materials, with potential applications in advanced electronic and magnetic devices.

Quantum spin driven Yu-Shiba-Rusinov multiplets and fermion-parity-preserving phase transition in K3C60

Magnetic impurities in superconductors are of increasing interest due to emergent Yu-Shiba-Rusinov (YSR) states and Majorana zero modes for fault-tolerant quantum computation. However, a direct relationship between the YSR multiple states and magnetic anisotropy splitting of quantum impurity spins remains poorly characterized. By using scanning tunneling microscopy, we systematically resolve individual transition-metal (Fe, Cr, and Ni) impurities induced YSR multiplets as well as their Zeeman effects in the K3C60 superconductor. The YSR multiplets show identical d orbital-like wave functions that are symmetry-mismatched to the threefold K3C60(1 1 1) host surface, breaking point-group symmetries of the spatial distribution of YSR bound states in real space. Remarkably, we identify an unprecedented fermion-parity-preserving quantum phase transition between ground states with opposite signs of the uniaxial magnetic anisotropy that can be manipulated by an external magnetic field. These findings can be readily understood in terms of anisotropy splitting of quantum impurity spins, and thus elucidate the intricate interplay between the magnetic anisotropy and YSR multiplets.

Exploring anisotropic phases and spin transport in perovskite heterostructures: Insights into 3d/5d interfaces for antiferromagnetic spintronics

Transition metal oxides (TMOs) demonstrate a broad spectrum of properties encompassing electronic correlations, anisotropic transport, magnetism, and optical behavior. The anisotropy arises from both intrinsic crystal symmetry and extrinsic factors like epitaxial strain and structural asymmetry at TMO interfaces. Weiss and Neel's work has elucidated anisotropic magnetic behavior in antiferromagnetic (AFM) materials. AFM TMOs exhibit unique magnetotransport behavior, including weak antilocalization (WAL) and anisotropic magnetoresistance (AMR). Understanding the magnetic structure and band topology in AFM perovskites and their interfaces enables the tailored design of materials for spintronics and energy conversion. In few interfaces lacking inversion symmetry, Rashba spin–orbit coupling (SOC) induces WAL, a quantum correction in conductivity in a two-dimensional electronic system. Electron accumulation and charge transfer across 3d, 5d transition metal-based perovskite interfaces affect WAL and AMR, as observed in 3d/3d and 3d/5d AFM heterostructures, respectively. Advancements in spintronics rely on exploring spin-dependent transport anisotropy. This review focuses on various scattering mechanisms, categorized as extrinsic and intrinsic, in anisotropic transport, particularly in 3d/5d AFM superlattices. The WAL scattering mechanism depends on both intrinsic factors related to Rashba SOC-induced band topology and extrinsic sources like spin impurities and lattice ions. Moreover, the investigation into AMR mechanisms involves the application of impurity-based extrinsic scattering models, which are aligned with the Rashba and Dresselhauss models on Fermi surfaces. This exploration specifically targets the interface of two-band insulators, exemplified by LaAlO3/SrTiO3 and LaVO3/KTaO3. Furthermore, this model achieves comprehensive coverage, extending its applicability to 3d/5d AFM heterostructures like LaMnO3/SrIrO3 and CaMnO3/CaIrO3. Additionally, the intrinsic scattering mechanism tied to Berry phase effects related to band topology is studied, focusing on the CaMnO3/CaIrO3 superlattice. Despite manipulation challenges stemming from reduced stray fields, AFM materials show potential in interface physics and applications within the realm of spintronics.

Kondo screening cloud scaling: impurity entanglement and magnetization

The screening of an impurity spin in the Kondo model occurs over a characteristic length scale ξ K , that defines the size of the Kondo screening cloud or ‘mist’. The presence of such a length scale in experimental and numerical results is rather subtle. A consistent way to show the presence of the screening cloud is to demonstrate scaling in the spatial correlations in terms of the single variable, r/ξK instead of the correlations depending on r and ξ K separately. Here we study the paradigmatic one channel Kondo model using a spin chain representation, with an impurity spin at one end of the chain coupled with a strength JK′ . Using Fermi liquid theory combined with numerical results, we obtain new high precision estimates of the non-universal terms in the entanglement entropy which leads to a verification of the expected non-integer ground-state degeneracy, g. This then allows us to study the impurity contribution to the entanglement in detail. If the impurity coupling JK′ is varied, a precise determination of ξ K can then be obtained. The length scale, ξ K , is then shown to characterize the scaling of both the uniform and alternating part of a measure of the magnetization of part of an odd length chain.

Quantum criticality features in the Co,Fe doped MnSi

An universal line revealing an independence of spin fluctuation contributions to the heat capacity on impurity content and its nature is discovered in the helical phase of Mn(Co,Fe)Si. This situation declares an invariance of the heat capacity of spin subsystem under doping, which probably arises as a result of relative stiffness of the helical spin structure in respect to the impurity spins. On the other hand the situation drastically changes at the helical fluctuation region when no long range spin order exists. At low temperatures the spin fluctuation contributions to the heat capacity for a whole set of compositions of Mn(Co,Fe)Si are described by a single power expression with an exponent less then unity, which implies divergence of the ratio Cp/T at T→0. The current data are revealing that a singular quantum critical point does not exist in the system under study. In its place, one can see some sort of a quantum critical cloud covering a significant range of dopant concentrations.

Molecular Control of Triplet-Pair Spin Polarization and Its Optoelectronic Magnetic Resonance Probes.

ConspectusPreparing and manipulating pure magnetic states in molecular systems are the key initial requirements for harnessing the power of synthetic chemistry to drive practical quantum sensing and computing technologies. One route for achieving the requisite higher spin states in organic systems exploits the phenomenon of singlet fission, which produces pairs of triplet excited states from initially photoexcited singlets in molecular assemblies with multiple chromophores. The resulting spin states are characterized by total spin (quintet, triplet, or singlet) and its projection onto a specified molecular or magnetic field axis. These excited states are typically highly polarized but exhibit an impure spin population pattern. Herein, we report the prediction and experimental verification of molecular design rules that drive the population of a single pure magnetic state and describe the progress toward its experimental realization.A vital feature of this work is the close partnership among theory, chemical synthesis, and spectroscopy. We begin by presenting our theoretical framework for understanding spin manifold interconversion in singlet fission systems. This theory makes specific testable predictions about the intermolecular structure and orientation relative to an external magnetic field that should lead to pure magnetic state preparation and provides a powerful tool for interpreting magnetic spectra. We then test these predictions through detailed magnetic spectroscopy experiments on a series of new molecular architectures that meet one or more of the identified structural criteria. Many of these architectures rely on the synthesis of molecules with features unique to this effort: rigid bridges between chromophores in dimers, heteroacenes with tailored singlet/triplet-pair energy level matching, or side-group engineering to produce specific crystal structures. The spin evolution of these systems is revealed through our application and development of several magnetic resonance methods, each of which has different sensitivities and relevance in environments relevant to quantum applications.Our theoretical predictions prove to be remarkably consistent with our experimental results, though experimentally meeting all the structural prescriptions demanded by theory for true pure-state preparation remains a challenge. Our magnetic spectra agree with our model of triplet-pair behavior, including funneling of the population to the ms = 0 magnetic sublevel of the quintet under specified conditions in dimers and crystals, showing that this phenomenon is subject to control through molecular design. Moreover, our demonstration of novel and/or highly sensitive detection mechanisms of spin states in singlet fission systems, including photoluminescence (PL), photoinduced absorption (PA), and magnetoconductance (MC), points the way toward both a deeper understanding of how these systems evolve and technologically feasible routes toward experiments at the single-molecule quantum limit that are desirable for computational applications.

Observing the universal screening of a Kondo impurity

The Kondo effect, deriving from a local magnetic impurity mediating electron-electron interactions, constitutes a flourishing basis for understanding a large variety of intricate many-body problems. Its experimental implementation in tunable circuits has made possible important advances through well-controlled investigations. However, these have mostly concerned transport properties, whereas thermodynamic observations - notably the fundamental measurement of the spin of the Kondo impurity - remain elusive in test-bed circuits. Here, with a novel combination of a ‘charge’ Kondo circuit with a charge sensor, we directly observe the state of the impurity and its progressive screening. We establish the universal renormalization flow from a single free spin to a screened singlet, the associated reduction in the magnetization, and the relationship between scaling Kondo temperature and microscopic parameters. In our device, a Kondo pseudospin is realized by two degenerate charge states of a metallic island, which we measure with a non-invasive, capacitively coupled charge sensor. Such pseudospin probe of an engineered Kondo system opens the way to the thermodynamic investigation of many exotic quantum states, including the clear observation of Majorana zero modes through their fractional entropy.

Counting edge modes via dynamics of boundary spin impurities

Counting edge modes via dynamics of boundary spin impurities

Emergent Heavy Local Fermi Liquid in the Ferromagnetic Kondo Model with Integer Impurity Spin

Emergent Heavy Local Fermi Liquid in the Ferromagnetic Kondo Model with Integer Impurity Spin

Ruderman-Kittel-Kasuya-Yosida-Type Interlayer Dzyaloshinskii-Moriya Interaction in Synthetic Magnets.

Conduction electron spins interacting with magnetic impurity spins can mediate an interlayer exchange interaction, namely, the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction. This discovery opened the way to significant technological developments in the field of magnetic storage and spintronics. So far, the RKKY-type interlayer interaction has been found to construct symmetric coupling of magnetism; however, the asymmetric counterpart remains unexplored. Here we report unprecedented RKKY-type interlayer Dzyaloshinskii-Moriya interaction (DMI) in synthetic magnets, exhibiting a damped oscillatory feature. This asymmetric interlayer interaction is found to be dramatically dependent on the intermediate coupling layer. By introducing the Fert-Lévy model to the trilayer system, we reveal that the in-plane inversion symmetry breaking plays a pivotal role for generating interlayer DMI and the RKKY oscillation is an intrinsic behavior in metallic multilayers. Our finding fills up the empty block for RKKY-type asymmetric interlayer exchange coupling in comparison to the well-known (symmetric) RKKY-type interlayer exchange coupling.

Polarons in binary Bose–Einstein condensates

Bose polarons are quasiparticles formed through the interaction between impurities and Bose–Einstein condensates. In this paper, we derive an effective Fröhlich Hamiltonian using the generalized Bogoliubov transformation. The effective Fröhlich Hamiltonian encompasses two types of effective interactions: impurity-density (ID) coupling and impurity-spin (IS) coupling. Furthermore, we employ the Lee–Low–Pines variational approach to investigate the relevant properties of Bose polarons induced by the ID and IS coupling. These properties include the ground state energy, effective mass, and average number of virtual phonons. Our findings reveal that the contribution resulting from IS couplings to the ground energy decreases to zero near the miscible–immiscible boundary. Additionally, the increase of the IS coupling induces a greater number of virtual phonons, impeding the movement of impurities and leading to a significant increase in the effective mass of Bose polarons.

Robust spin polarization of Yu-Shiba-Rusinov states in superconductor/ferromagnetic insulator heterostructures

Yu-Shiba-Rusinov (YSR) states arise as subgap excitations of a magnetic impurity in a superconducting host. Taking into account the quantum nature of the impurity spin in a single-site approximation, we study the spectral properties of the YSR excitations of a system of magnetic impurity in a spin-split superconductor, i.e., a superconductor in proximity to a ferromagnetic insulator at zero external magnetic fields. The YSR excitations of this system exhibit a robust spin polarization that is protected from fluctuations and environmental noise by the exchange field of the ferromagnetic insulator, which can be as large as a few Tesla. We compare the results of this quantum approach to the classical approach, which conventionally predicts fully polarized YSR excitations even in the absence of exchange and external magnetic field. Turning on a small magnetic field, we show the latter splits the YSR excitations in the regime where the impurity is strongly coupled to the superconductor, whilst the classical approach predicts no such splitting. The studied system can potentially be realized in a tunnel junction connected to a quantum dot in proximity to a spin-split superconductor.

Field-induced local Fermi-liquid states in the underscreened Kondo model for Eu compounds

We have studied an underscreened Kondo model for the impurity spin S=7/2S=7/2 capturing the 4f4f characteristics of a nearly divalent Eu ion. By using the numerical renormalization group method, it is shown that an unusual heavy-fermion state is induced from the underscreened spin state when a weak crystal field is introduced. It is also found that the application of the magnetic field enhances the effective mass of the heavy fermions, reflecting the field-induced level crossing of the spin states. We will discuss the mechanism of these mass enhancements in terms of a realization of the two-stage Kondo effect.

Model for 1/f flux noise in superconducting aluminum devices: Impact of external magnetic fields

Superconducting quantum interference devices and related circuits made of aluminum are known to display 1/ω flux noise, where ω is frequency. A recent experiment showed that the application of an external magnetic field in the 10–100 G range changed the noise to a single Lorentzian peaked at ω = 0. Here, it is shown that a model based on independent impurity spin flips with coexisting cross and direct mechanisms of spin relaxation may explain these experiments. The model shows that application of an external magnetic field can be used to reduce the impact of flux noise in qubits.