Strong Photon-Magnon Coupling Using a Lithographically Defined Organic Ferrimagnet.

A cavity-magnonic system composed of a superconducting microwave resonator coupled to a magnon mode hosted by the organic-based ferrimagnet vanadium tetracyanoethylene (V[TCNE]x) is demonstrated. This work is motivated by the challenge of scalably integrating a low-damping magnetic system with planar superconducting circuits. V[TCNE]x has ultra-low intrinsic damping, can be grown at low processing temperatures on arbitrary substrates, and can be patterned via electron beam lithography. The devices operate in the strong coupling regime, with a cooperativity exceeding 1000 for coupling between the Kittel mode and the resonator mode at T≈0.4 K, suitable for scalable quantum circuit integration. Higher-order magnon modes are also observed with much narrower linewidths than the Kittel mode. This work paves the way for high-cooperativity hybrid quantum devices in which magnonic circuits can be designed and fabricated as easily as electrical wires.

Magnon-mediated qubit coupling determined via dissipation measurements.

Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets-systems with naturally commensurate energies-have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV-NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems.

Dissipationless Circulating Currents and Fringe Magnetic Fields Near a Single Spin Embedded in a Two-Dimensional Electron Gas.

Theoretical calculations predict the anisotropic dissipationless circulating current induced by a spin defect in a two-dimensional electron gas. The shape and spatial extent of these dissipationless circulating currents depend dramatically on the relative strengths of spin-orbit fields with differing spatial symmetry, offering the potential to use an electric gate to manipulate nanoscale magnetic fields and couple magnetic defects. The spatial structure of the magnetic field produced by this current is calculated and provides a direct way to measure the spin-orbit fields of the host, as well as the defect spin orientation, e.g., through scanning nanoscale magnetometry.

Permanent Porosity in the Room-Temperature Magnet and Magnonic Material V(TCNE)2.

Materials that simultaneously exhibit permanent porosity and high-temperature magnetic order could lead to advances in fundamental physics and numerous emerging technologies. Herein, we show that the archetypal molecule-based magnet and magnonic material V(TCNE)2 (TCNE = tetracyanoethylene) can be desolvated to generate a room-temperature microporous magnet. The solution-phase reaction of V(CO)6 with TCNE yields V(TCNE)2·0.95CH2Cl2, for which a characteristic temperature of T* = 646 K is estimated from a Bloch fit to variable-temperature magnetization data. Removal of the solvent under reduced pressure affords the activated compound V(TCNE)2, which exhibits a T* value of 590 K and permanent microporosity (Langmuir surface area of 850 m2/g). The porous structure of V(TCNE)2 is accessible to the small gas molecules H2, N2, O2, CO2, ethane, and ethylene. While V(TCNE)2 exhibits thermally activated electron transfer with O2, all the other studied gases engage in physisorption. The T* value of V(TCNE)2 is slightly modulated upon adsorption of H2 (T* = 583 K) or CO2 (T* = 596 K), while it decreases more significantly upon ethylene insertion (T* = 459 K). These results provide an initial demonstration of microporosity in a room-temperature magnet and highlight the possibility of further incorporation of small-molecule guests, potentially even molecular qubits, toward future applications.

Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals.

Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for biosensing and optoelectronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the CuZn-VS complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First-principles calculations confirm the thermodynamic stability and electronic structure of CuZn-VS. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and an anomalous plateau in the intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of CuZn-VS and related complexes as quantum point defects in ZnS.

High-Frequency Sheet Conductance of Nanolayered WS2 Crystals for Two-Dimensional Nanodevices.

Time-resolved terahertz (THz) spectroscopy is a powerful technique for the determination of charge transport properties in photoexcited semiconductors. However, the relatively long wavelengths of THz radiation and the diffraction limit imposed by optical imaging systems reduce the applicability of THz spectroscopy to large samples with dimensions in the millimeter to centimeter range. Exploiting THz near-field spectroscopy, we present the first time-resolved THz measurements on a single exfoliated 2D nanolayered crystal of a transition metal dichalcogenide (WS2). The high spatial resolution of THz near-field spectroscopy enables mapping of the sheet conductance for an increasing number of atomic layers. The single-crystalline structure of the nanolayered crystal allows for the direct observation of low-energy phonon modes, which are present in all thicknesses, coupling with free carriers. Density functional theory calculations show that the phonon mode corresponds to the breathing mode between atomic layers in the weakly bonded van der Waals layers, which can be strongly influenced by substrate-induced strain. The non-invasive and high-resolution mapping technique of carrier dynamics in nanolayered crystals by time-resolved THz time domain spectroscopy enables possibilities for the investigation of the relation between phonons and charge transport in nanoscale semiconductors for applications in two-dimensional nanodevices.

Large magnon-induced anomalous Nernst conductivity in single-crystal MnBi.

Thermoelectric modules are a promising approach to energy harvesting and efficient cooling. In addition to the longitudinal Seebeck effect, transverse devices utilizing the anomalous Nernst effect (ANE) have recently attracted interest. For high conversion efficiency, it is required that the material have a large ANE thermoelectric power and low electrical resistance, which lead to the conductivity of the ANE. ANE is usually explained in terms of intrinsic contributions from Berry curvature. Our observations suggest that extrinsic contributions also matter. Studying single-crystal manganese-bismuth (MnBi), we find a high ANE thermopower (∼10 µV/K) under 0.6 T at 80 K, and a transverse thermoelectric conductivity of over 40 A/Km. With insight from theoretical calculations, we attribute this large ANE predominantly to a new advective magnon contribution arising from magnon-electron spin-angular momentum transfer. We propose that introducing a large spin-orbit coupling into ferromagnetic materials may enhance the ANE through the extrinsic contribution of magnons.

Thermal chiral anomaly in the magnetic-field-induced ideal Weyl phase of Bi1-xSbx.

The chiral anomaly is the predicted breakdown of chiral symmetry in a Weyl semimetal with monopoles of opposite chirality when an electric field is applied parallel to a magnetic field. It occurs because of charge pumping between monopoles of opposite chirality. Experimental observation of this fundamental effect is plagued by concerns about the current pathways. Here we demonstrate the thermal chiral anomaly, energy pumping between monopoles, in topological insulator bismuth-antimony alloys driven into an ideal Weyl semimetal state by a Zeeman field, with the chemical potential pinned at the Weyl points and in the absence of any trivial Fermi surface pockets. The experimental signature is a large enhancement of the thermal conductivity in an applied magnetic field parallel to the thermal gradient. This work demonstrates both pumping of energy and charge between the two Weyl points of opposite chirality and that they are related by the Wiedemann-Franz law.

Tunable tunnel barriers in a semiconductor via ionization of individual atoms.

We report scanning tunneling microscopy (STM) studies of individual adatoms deposited on an InSb(110) surface. The adatoms can be reproducibly dropped off from the STM tip by voltage pulses, and impact tunneling into the surface by up to ∼100×. The spatial extent and magnitude of the tunneling effect are widely tunable by imaging conditions such as bias voltage, set current and photoillumination. We attribute the effect to occupation of a (+/0) charge transition level, and switching of the associated adatom-induced band bending. The effect in STM topographic images is well reproduced by transport modeling of filling and emptying rates as a function of the tip position. STM atomic contrast and tunneling spectra are in good agreement with density functional theory calculations for In adatoms. The adatom ionization effect can extend to distances greater than 50 nm away, which we attribute to the low concentration and low binding energy of the residual donors in the undoped InSb crystal. These studies demonstrate how individual atoms can be used to sensitively control current flow in nanoscale devices.

Image of Dynamic Local Exchange Interactions in the dc Magnetoresistance of Spin-Polarized Current through a Dopant.

We predict strong, dynamical effects in the dc magnetoresistance of current flowing from a spin-polarized electrical contact through a magnetic dopant in a nonmagnetic host. Using the stochastic Liouville formalism we calculate clearly defined resonances in the dc magnetoresistance when the applied magnetic field matches the exchange interaction with a nearby spin. At these resonances spin precession in the applied magnetic field is canceled by spin evolution in the exchange field, preserving a dynamic bottleneck for spin transport through the dopant. Similar features emerge when the dopant spin is coupled to nearby nuclei through the hyperfine interaction. These features provide a precise means of measuring exchange or hyperfine couplings between localized spins near a surface using spin-polarized scanning tunneling microscopy, without any ac electric or magnetic fields, even when the exchange or hyperfine energy is orders of magnitude smaller than the thermal energy.

Strain Effects on the Energy-Level Alignment at Metal/Organic Semiconductor Interfaces.

Flexible and wearable devices are among the upcoming trends in the opto-electronics market. Nevertheless, bendable devices should ensure the same efficiency and stability as their rigid analogs. It is well-known that the energy barriers between the metal Fermi energy and the molecular levels of organic semiconductors devoted to charge transport are key parameters in the performance of organic-based electronic devices. Therefore, it is paramount to understand how the energy barriers at metal/organic semiconductor interfaces change with bending. In this work, we experimentally measure the interface energy barriers between a metallic contact and small semiconducting molecules. The measurements are performed in operative conditions, while the samples are bent by a controlled applied mechanical strain. We determine that energy barriers are not sensitive to bending of the sample, but we observe that the hopping transport of the charges in flat molecules can be tuned by mechanical strain. The theoretical model developed for this work confirms our experimental observations.

Impact of the Synthesis Method on the Solid-State Charge Transport of Radical Polymers.

There are conflicting reports in the literature about the presence of room temperature conductivity in poly(2,2,6,6-tetramethylpiperidinyloxy methacrylate) (PTMA), a redox active polymer with radical groups pendent to an insulating backbone. To understand the variability in the findings across the literature and synthetic methods, we prepared PTMA using three living methods - anionic, ATRP and RAFT polymerization. We find that all three synthetic methods produce PTMA with radical yields of 70 - 80%, controlled molecular weight, and low dispersity. Additionally, we used on-chip EPR to probe the robustness of radical content in solid films under ambient air and light, and found negligible change in the radical content over time. Electrically, we found that PTMA is highly insulating - conductivity in the range 10-11 S/cm - regardless of the synthetic method of preparation. These findings provide greater clarity for potential applications of PTMA in energy storage.

Blurring the Boundaries Between Topological and Nontopological Phenomena in Dots.

We investigate the electronic and transport properties of topological and nontopological InAs_{0.85}Bi_{0.15} quantum dots (QDs) described by a ∼30 meV gapped Bernevig-Hughes-Zhang (BHZ) model with cylindrical confinement, i.e., "BHZ dots." Via modified Bessel functions, we analytically show that nontopological dots quite unexpectedly have discrete helical edge states, i.e., Kramers pairs with spin-angular-momentum locking similar to topological dots. These unusual nontopological edge states are geometrically protected due to confinement for a wide range of parameters and remarkably contrast with the bulk-edge correspondence in topological insulators, as no bulk topological invariant guarantees their existence. Moreover, for a conduction window with four edge states, we find that the two-terminal conductance G versus the QD radius R and the gate V_{g} controlling its levels shows a double peak at 2e^{2}/h for both topological and trivial BHZ QDs. This is in stark contrast to conductance measurements in 2D quantum spin Hall and trivial insulators. All of these results were also found in HgTe QDs. Bi-based BHZ dots should also prove important as hosts to room temperature edge spin qubits.

Strong Modulation of Spin Currents in Bilayer Graphene by Static and Fluctuating Proximity Exchange Fields.

Two-dimensional materials provide a unique platform to explore the full potential of magnetic proximity-driven phenomena, which can be further used for applications in next-generation spintronic devices. Of particular interest is to understand and control spin currents in graphene by the magnetic exchange field of a nearby ferromagnetic material in graphene-ferromagnetic-insulator (FMI) heterostructures. Here, we present the experimental study showing the strong modulation of spin currents in graphene layers by controlling the direction of the exchange field due to FMI magnetization. Owing to clean interfaces, a strong magnetic exchange coupling leads to the experimental observation of complete spin modulation at low externally applied magnetic fields in short graphene channels. Additionally, we discover that the graphene spin current can be fully dephased by randomly fluctuating exchange fields. This is manifested as an unusually strong temperature dependence of the nonlocal spin signals in graphene, which is due to spin relaxation by thermally induced transverse fluctuations of the FMI magnetization.

Temperature Dependence of Wavelength Selectable Zero-Phonon Emission from Single Defects in Hexagonal Boron Nitride.

We investigate the distribution and temperature-dependent optical properties of sharp, zero-phonon emission from defect-based single photon sources in multilayer hexagonal boron nitride (h-BN) flakes. We observe sharp emission lines from optically active defects distributed across an energy range that exceeds 500 meV. Spectrally resolved photon-correlation measurements verify single photon emission, even when multiple emission lines are simultaneously excited within the same h-BN flake. We also present a detailed study of the temperature-dependent line width, spectral energy shift, and intensity for two different zero-phonon lines centered at 575 and 682 nm, which reveals a nearly identical temperature dependence despite a large difference in transition energy. Our temperature-dependent results are well described by a lattice vibration model that considers piezoelectric coupling to in-plane phonons. Finally, polarization spectroscopy measurements suggest that whereas the 575 nm emission line is directly excited by 532 nm excitation, the 682 nm line is excited indirectly.

Nonlocal Drag of Magnons in a Ferromagnetic Bilayer.

Quantized spin waves, or magnons, in a magnetic insulator are assumed to interact weakly with the surroundings, and to flow with little dissipation or drag, producing exceptionally long diffusion lengths and relaxation times. In analogy to Coulomb drag in bilayer two-dimensional electron gases, in which the contribution of the Coulomb interaction to the electric resistivity is studied by measuring the interlayer resistivity (transresistivity), we predict a nonlocal drag of magnons in a ferromagnetic bilayer structure based on semiclassical Boltzmann equations. Nonlocal magnon drag depends on magnetic dipolar interactions between the layers and manifests in the magnon current transresistivity and the magnon thermal transresistivity, whereby a magnon current in one layer induces a chemical potential gradient and/or a temperature gradient in the other layer. The largest drag effect occurs when the magnon current flows parallel to the magnetization; however, for oblique magnon currents a large transverse current of magnons emerges. We examine the effect for practical parameters, and find that the predicted induced temperature gradient is readily observable.

Tunable giant spin hall conductivities in a strong spin-orbit semimetal: Bi(1-x) Sb(x).

Intrinsic spin Hall conductivities are calculated for strong spin-orbit Bi(1-x)Sb(x) semimetals, from the Kubo formula and using Berry curvatures evaluated throughout the Brillouin zone from a tight-binding Hamiltonian. Nearly crossing bands with strong spin-orbit interaction generate giant spin Hall conductivities in these materials, ranging from 474 (ℏ/e)(Ω cm)^{-1} for bismuth to 96 (ℏ/e)(Ω cm)^{-1} for antimony; the value for bismuth is more than twice that of platinum. The large spin Hall conductivities persist for alloy compositions corresponding to a three-dimensional topological insulator state, such as Bi(0.83)Sb(0.17). The spin Hall conductivity could be changed by a factor of 5 for doped Bi, or for Bi(0.83)Sb(0.17), by changing the chemical potential by 0.5 eV, suggesting the potential for doping or voltage tuned spin Hall current.

Electrical control of Faraday rotation at a liquid-liquid interface.

A theory is developed for the Faraday rotation of light from a monolayer of charged magnetic nanoparticles at an electrified liquid-liquid interface. The polarization fields of neighboring nanoparticles enhance the Faraday rotation. At such interfaces, and for realistic sizes and charges of nanoparticles, their adsorption-desorption can be controlled with a voltage variation<1 V, providing electrovariable Faraday rotation. A calculation based on the Maxwell-Garnett theory predicts that the corresponding redistribution of 40 nm nanoparticles of yttrium iron garnet can switch a cavity with a quality factor larger than 10(4) for light of wavelength 500 nm at normal incidence.

Electric-field coupling to spin waves in a centrosymmetric ferrite.

We experimentally demonstrate that the spin-orbit interaction can be utilized for direct electric-field tuning of the propagation of spin waves in a single-crystal yttrium iron garnet magnonic waveguide. Magnetoelectric coupling not due to the spin-orbit interaction and, hence, an order of magnitude weaker leads to electric-field modification of the spin-wave velocity for waveguide geometries where the spin-orbit interaction will not contribute. A theory of the phase shift, validated by the experiment data, shows that, in the exchange spin wave regime, this electric tuning can have high efficiency. Our findings point to an important avenue for manipulating spin waves and developing electrically tunable magnonic devices.

Organic magnetoelectroluminescence for room temperature transduction between magnetic and optical information.

Magnetic and spin-based technologies for data storage and processing provide unique challenges for information transduction to light because of magnetic metals' optical loss, and the inefficiency and resistivity of semiconductor spin-based emitters at room temperature. Transduction between magnetic and optical information in typical organic semiconductors poses additional challenges, as the spin-orbit interaction is weak and spin injection from magnetic electrodes has been limited to low temperature and low polarization efficiency. Here we demonstrate room temperature information transduction between a magnet and an organic light-emitting diode that does not require electrical current, based on control via the magnet's remanent field of the exciton recombination process in the organic semiconductor. This demonstration is explained quantitatively within a theory of spin-dependent exciton recombination in the organic semiconductor, driven primarily by gradients in the remanent fringe fields of a few nanometre-thick magnetic film.