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The amorphous iron-germanium system (a-FexGe1-x) lacks long-range structural order and hence lacks a meaningful Brillouin zone. The magnetization of a-FexGe1-x is well explained by the Stoner model for Fe concentrations x above the onset of magnetic order around x=0.4, indicating that the local order of the amorphous structure preserves the spin-split density of states of the Fe-3d states sufficiently to polarize the electronic structure despite k being a bad quantum number. Measurements reveal an enhanced anomalous Hall resistivity ρxyAH relative to crystalline FeGe; this ρxyAH is compared to density-functional theory calculations of the anomalous Hall conductivity to resolve its underlying mechanisms. The intrinsic mechanism, typically understood as the Berry curvature integrated over occupied k states but shown here to be equivalent to the density of curvature integrated over occupied energies in aperiodic materials, dominates the anomalous Hall conductivity of a-FexGe1-x (0.38≤x≤0.61). The density of curvature is the sum of spin-orbit correlations of local orbital states and can hence be calculated with no reference to k space. This result and the accompanying Stoner-like model for the intrinsic anomalous Hall conductivity establish a unified understanding of the underlying physics of the anomalous Hall effect in both crystalline and disordered systems.

Hexagonal boron nitride (h-BN) hosts pure single-photon emitters that have shown evidence of optically detected electronic spin dynamics. However, the electrical and chemical structures of these optically addressable spins are unknown, and the nature of their spin-optical interactions remains mysterious. Here, we use time-domain optical and microwave experiments to characterize a single emitter in h-BN exhibiting room temperature optically detected magnetic resonance. Using dynamical simulations, we constrain and quantify transition rates in the model, and we design optical control protocols that optimize the signal-to-noise ratio for spin readout. This constitutes a necessary step toward quantum control of spin states in h-BN.

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., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

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., Competing Interests: Competing interests statement:The authors declare no competing interest.

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.

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 ·0.95CH 2 Cl 2 , 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 m 2 /g). The porous structure of V(TCNE) 2 is accessible to the small gas molecules H 2 , N 2 , O 2 , CO 2 , ethane, and ethylene. While V(TCNE) 2 exhibits thermally activated electron transfer with O 2 , all the other studied gases engage in physisorption. The T * value of V(TCNE) 2 is slightly modulated upon adsorption of H 2 ( T * = 583 K) or CO 2 ( 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., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

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 Cu Zn -V S 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 Cu Zn -V S . 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 Cu Zn -V S and related complexes as quantum point defects in ZnS.

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 (WS 2 ). 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., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

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., Competing Interests: The authors declare no competing interests., (© 2021 The Authors.)

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., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)

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., (© 2021 IOP Publishing Ltd.)

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.

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.

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.

We show that the application of a spin-polarized current to a double p domain wall system with a variable distance between the walls results in an interaction between the two domain walls. The transmission spectrum changes from that of a spin-dependent resonant double barrier to one like a [Formula: see text] wall. In addition, the spin torque on each individual wall creates coupled motion in the domain walls. The walls move independently with a fast speed at large separations, but slow considerably at small separations.

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., Competing Interests: Conflicts of interest There are no conflicts to declare.

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.

The spatial resolution of imaging magnetometers has benefited from scanning probe techniques. The requirement that the sample perturbs the scanning probe through a magnetic field external to its volume limits magnetometry to samples with pre-existing magnetization. We propose a magnetometer in which the perturbation is reversed: the probe's magnetic field generates a response of the sample, which acts back on the probe and changes its energy. For an NV^{-} spin center in diamond this perturbation changes the fine-structure splitting of the spin ground state. Sensitive measurement techniques using coherent detection schemes then permit detection of the magnetic response of paramagnetic and diamagnetic materials. This technique can measure the thickness of magnetically dead layers with better than 0.1 Å accuracy.

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.

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.

We demonstrate that electron spin relaxation in GaAs in the proximity of a Fe/MgO layer is dominated by interaction with an exchange-driven hyperfine field at temperatures below 60 K. Temperature-dependent spin-resolved optical pump-probe spectroscopy reveals a strong correlation of the electron spin relaxation with carrier freeze-out, in quantitative agreement with a theoretical interpretation that at low temperatures the free-carrier spin lifetime is dominated by inhomogeneity in the local hyperfine field due to carrier localization. As the regime of large nuclear inhomogeneity is accessible in these heterostructures for magnetic fields <3  kG, inferences from this result resolve a long-standing and contentious dispute concerning the origin of spin relaxation in GaAs at low temperature when a magnetic field is present. Further, this improved fundamental understanding clarifies the importance of future experiments probing the time-dependent exchange interaction at a ferromagnet-semiconductor interface and its consequences for spin dissipation and transport during spin pumping.

We present the measurement of ferromagnetic resonance (FMR-)driven spin pumping and three-terminal electrical spin injection within the same silicon-based device. Both effects manifest in a dc spin accumulation voltage V&#95;{s} that is suppressed as an applied field is rotated to the out-of-plane direction, i.e., the oblique Hanle geometry. Comparison of V&#95;{s} between these two spin injection mechanisms reveals an anomalously strong suppression of FMR-driven spin pumping with increasing out-of-plane field H&#95;{app}^{z}. We propose that the presence of the large ac component to the spin current generated by the spin pumping approach, expected to exceed the dc value by 2 orders of magnitude, is the origin of this discrepancy through its influence on the spin dynamics at the oxide-silicon interface. This convolution, wherein the dynamics of both the injector and the interface play a significant role in the spin accumulation, represents a new regime for spin injection that is not well described by existing models of either FMR-driven spin pumping or electrical spin injection.

Until recently the important role that spin-physics ('spintronics') plays in organic light-emitting devices and photovoltaic cells was not sufficiently recognized. This attitude has begun to change. We review our recent work that shows that spatially rapidly varying local magnetic fields that may be present in the organic layer dramatically affect electronic transport properties and electroluminescence efficiency. Competition between spin-dynamics due to these spatially varying fields and an applied, spatially homogeneous magnetic field leads to large magnetoresistance, even at room temperature where the thermodynamic influences of the resulting nuclear and electronic Zeeman splittings are negligible. Spatially rapidly varying local magnetic fields are naturally present in many organic materials in the form of nuclear hyperfine fields, but we will also review a second method of controlling the electrical conductivity/electroluminescence, using the spatially varying magnetic fringe fields of a magnetically unsaturated ferromagnet. Fringe-field magnetoresistance has a magnitude of several per cent and is hysteretic and anisotropic. This new method of control is sensitive to even remanent magnetic states, leading to different conductivity/electroluminescence values in the absence of an applied field. We briefly review a model based on fringe-field-induced polaron-pair spin-dynamics that successfully describes several key features of the experimental fringe-field magnetoresistance and magnetoelectroluminescence., (© 2015 The Author(s) Published by the Royal Society. All rights reserved.)

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.

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.

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.

Circulating orbital currents produced by the spin-orbit interaction for a single electron spin in a quantum dot are explicitly evaluated at zero magnetic field, along with their effect on the total magnetic moment (spin and orbital) of the electron spin. The currents are dominated by coherent superpositions of the conduction and valence envelope functions of the electronic state, are smoothly varying within the quantum dot, and are peaked roughly halfway between the dot center and edge. Thus the spatial structure of the spin contribution to the magnetic moment (which is peaked at the dot center) differs greatly from the spatial structure of the orbital contribution. Even when the spin and orbital magnetic moments cancel (for g=0) the spin can interact strongly with local magnetic fields, e.g., from other spins, which has implications for spin lifetimes and spin manipulation.

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.

Lanthanides are vital components in lighting, imaging technologies and future quantum memory applications owing to their narrow optical transitions and long spin coherence times. Recently, diamond has become a pre-eminent platform for the realisation of many experiments in quantum information science. Here we demonstrate a promising approach to incorporate Eu ions into diamond, providing a means to harness the exceptional characteristics of both lanthanides and diamond in a single material. Polyelectrolytes are used to electrostatically assemble Eu(III) chelate molecules on diamond and subsequently chemical vapour deposition is employed for the diamond growth. Fluorescence measurements show that the Eu atoms retain the characteristic optical signature of Eu(III) upon incorporation into the diamond lattice. Computational modelling supports the experimental findings, corroborating that Eu(III) in diamond is a stable configuration. The formed defects demonstrate the outstanding chemical control over the incorporation of impurities into diamond enabled by the electrostatic assembly together with chemical vapour deposition growth.

A theory is introduced for spin relaxation and spin diffusion of hopping carriers in a disordered system. For disorder described by a distribution of waiting times between hops (e.g., from multiple traps, site-energy disorder, and/or positional disorder) the dominant spin relaxation mechanisms in organic semiconductors (hyperfine, hopping-induced spin-orbit, and intrasite spin relaxation) each produce different characteristic spin relaxation and spin diffusion dependences on temperature. The resulting unique experimental signatures predicted by the theory for each mechanism in organic semiconductors provide a prescription for determining the dominant spin relaxation mechanism.

A model for magnetoresistance in positionally disordered organic materials is presented and solved using percolation theory. The model describes the effects of spin dynamics on hopping transport by considering changes in the effective density of hopping sites, a key quantity determining the properties of percolative transport. Faster spin-flip transitions open up "spin-blocked" pathways to become viable conduction channels and hence produce magnetoresistance. Features of this percolative magnetoresistance can be found analytically in several regimes, and agree with previous measurements, including the sensitive dependence of the magnetic-field dependence of the magnetoresistance on the ratio of the carrier hopping time to the hyperfine-induced carrier spin precession time. Studies of magnetoresistance in known systems with controllable positional disorder would provide an additional stringent test of this theory.

The sensitive dependence of a semiconductor's electronic, optical and magnetic properties on dopants has provided an extensive range of tunable phenomena to explore and apply to devices. Recently it has become possible to move past the tunable properties of an ensemble of dopants to identify the effects of a solitary dopant on commercial device performance as well as locally on the fundamental properties of a semiconductor. New applications that require the discrete character of a single dopant, such as single-spin devices in the area of quantum information or single-dopant transistors, demand a further focus on the properties of a specific dopant. This article describes the huge advances in the past decade towards observing, controllably creating and manipulating single dopants, as well as their application in novel devices which allow opening the new field of solotronics (solitary dopant optoelectronics).

We find a dramatic enhancement of electron propagation along a narrow range of real-space angles from an isotropic source in a two-dimensional quantum well made from a zinc-blende semiconductor. This "electron-beam" formation is caused by the interplay between spin-orbit interaction originating from a perpendicular electric field to the quantum well and the intrinsic spin-orbit field of the zinc-blende crystal lattice in a quantum well, in situations where the two fields are different in strength but of the same order of magnitude. Beam formation is associated with caustics and can be described semiclassically using a stationary phase analysis.

Measurements of the local density of states of individual acceptors in III-V semiconductors show that the symmetry of the acceptor states strongly depends on the depth of the atom below a (110) surface. Tight-binding calculations performed for a uniformly strained bulk material demonstrate that strain induced by the surface relaxation is responsible for the observed depth-dependent symmetry breaking of acceptor wave functions. As this effect is strongest for weakly bound acceptors, it explains within a unified approach the commonly observed triangular shapes of shallow acceptors and the crosslike shapes of deeply bound acceptor states in III-V materials.

We analyze the interaction of a nanomagnet (ferromagnetic) with a single photonic mode of a cavity in a fully quantum-mechanical treatment and find that exceptionally large quantum-coherent magnet-photon coupling can be achieved. Coupling terms in excess of several THz are predicted to be achievable in a spherical cavity of approximately 1 mm radius with a nanomagnet of approximately 100 nm radius and ferromagnetic resonance frequency of approximately 200 GHz. Eigenstates of the magnet-photon system correspond to entangled states of spin orientation and photon number, in which over 10{5} values of each quantum number are represented; conversely, initial (coherent) states of definite spin and photon number evolve dynamically to produce large oscillations in the microwave power (and nanomagnet spin orientation), and are characterized by exceptionally long dephasing times.

An ac electric field applied to a single donor-bound electron in a semiconductor modulates the orbital character of its wave function, which affects the electron's spin dynamics via the spin-orbit interaction. Numerical calculations of the spin dynamics of a single hydrogenic donor (Si) embedded in GaAs, using a real-space multiband k.p formalism, show the high symmetry of the hydrogenic donor state results in strongly nonlinear dependences of the electronic g tensor on applied fields. A nontrivial consequence is that the most rapid Rabi oscillations occur for electric fields modulated at a subharmonic of the Larmor frequency.

We describe the results of a theoretical analysis of the localization of functionalized metal or semiconductor nanoparticles at the interface of two immiscible electrolytic solutions and discuss various options that this interface may offer for a new kind of self-assembled, electro-optic devices.

Control of the fundamental absorption edge of a quantum dot with an applied electric field has been limited by the breakdown fields of the solid-state material surrounding the dot. However, much larger fields can be applied at the interface of two immiscible electrolytic solutions (ITIES) in an electrochemical cell. These electric fields also localize the quantum dots at the ITIES. Our analysis shows that semiconductor nanocrystals localized at the ITIES should have electric-field-tunable optical properties across much of the visible spectrum. The transparency of the liquids in such cells indicates that this configuration would be well suited for electrically tunable optical filters with wide-angle acceptance.

The magnetic circular dichroism of III-V diluted magnetic semiconductors, calculated within a theoretical framework suitable for highly disordered materials, is shown to be dominated by optical transitions between the bulk bands and an impurity band formed from magnetic dopant states. The real-space Green's functions incorporate spatial correlations in the disordered conduction band and valence-band electronic structure, and include extended and localized states on an equal basis. Our findings reconcile unusual trends in the experimental magnetic circular dichroism in III-V diluted magnetic semiconductors with the antiferromagnetic p-d exchange interaction between a magnetic dopant spin and its host.

Controlling and monitoring individual spins is desirable for building spin-based devices, as well as implementing quantum information processing schemes. As with trapped ions in cold gases, magnetic ions trapped on a semiconductor lattice have uniform properties and relatively long spin lifetimes. Furthermore, diluted magnetic moments in semiconductors can be strongly coupled to the surrounding host, permitting optical or electrical spin manipulation. Here we describe the zero-field optical manipulation of a few hundred manganese ions in a single gallium arsenide quantum well. Optically created mobile electron spins dynamically generate an energy splitting of the ion spins and enable magnetic moment orientation solely by changing either photon helicity or energy. These polarized manganese spins precess in a transverse field, enabling measurements of the spin lifetimes. As the magnetic ion concentration is reduced and the manganese spin lifetime increases, coherent optical control and readout of single manganese spins in gallium arsenide should be possible.

We develop a quantitatively predictive theory for impurity-band ferromagnetism in the low-doping regime of Ga1-xMnxAs. We compare it with measurements of a series of samples whose compositions span the transition from paramagnetic insulating to ferromagnetic conducting behavior. The theoretical Curie temperatures depend sensitively on the local fluctuations in the Mn-hole binding energy, which originate from Mn disorder and As antisite defects. The experimentally determined hopping energy is an excellent predictor of the Curie temperature, in agreement with the theory.

We present low-temperature scanning tunneling spectroscopy measurements on Mn acceptors in InAs in comparison with tight-binding calculations. We find a strong (001)-mirror asymmetry of the bound hole wave function close to the (110) surface. In addition, multiple acceptor-related peaks are observed and are attributed to a spin-orbit splitting of the acceptor level. Because of the p-d exchange interaction the local density of states near the acceptors is enhanced in the valence band and suppressed in the conduction band. We also observe signs of anisotropic scattering of the conduction band states by neutral acceptors.

Transition-metal dopants such as Mn determine the ferromagnetism in dilute magnetic semiconductors such as Ga(1-x)Mn(x)As. Recently, the acceptor states of Mn dopants in GaAs were found to be highly anisotropic owing to the symmetry of the host crystal. Here, we show how the shape of such a state can be modified by local strain. The Mn acceptors near InAs quantum dots are mapped at room temperature by scanning tunnelling microscopy. Dramatic distortions and a reduction in the symmetry of the wavefunction of the hole bound to the Mn acceptor are observed originating from strain induced by quantum dots. Calculations of the acceptor-state wavefunction in the presence of strain, within a tight-binding model and within an effective-mass model, agree with the experimentally observed shape. The magnetic easy axes of strained lightly doped Ga(1-x)Mn(x)As can be explained on the basis of the observed local density of states for the single Mn spin.

A self-consistent treatment of the spin-Hall effect requires consideration of the spin-orbit coupling and electron-impurity scattering on equal footing. This is done here for the experimentally relevant case of a [110] GaAs quantum well [Sih, Nature Phys. 1, 31 (2005)]. Working within the framework of the exact linear response formalism we calculate the spin-Hall conductivity including the Dresselhaus linear and cubic terms in the band structure, as well as the electron-impurity scattering and electron-electron interaction to all orders. We show that the spin-Hall conductivity naturally separates into two contributions, skew-scattering and side-jump, and we propose an experiment to distinguish between them.

We propose a method for all-electrical manipulation of single ion spins substituted into a semiconductor. Mn ions with a bound hole in GaAs form a natural example. Direct electrical manipulation of the ion spin is possible, because electric fields manipulate the orbital wave function of the hole, and through the spin-orbit coupling the spin is reoriented as well. Coupling ion spins can be achieved using gates to control the size of the hole wave function. Coherent manipulation of ionic spins may find applications in high-density storage and in scalable coherent or quantum information processing.

The discovery of ferromagnetism in Mn-doped GaAs has ignited interest in the development of semiconductor technologies based on electron spin and has led to several proof-of-concept spintronic devices. A major hurdle for realistic applications of Ga(1-x)Mn(x)As, or other dilute magnetic semiconductors, remains that their ferromagnetic transition temperature is below room temperature. Enhancing ferromagnetism in semiconductors requires us to understand the mechanisms for interaction between magnetic dopants, such as Mn, and identify the circumstances in which ferromagnetic interactions are maximized. Here we describe an atom-by-atom substitution technique using a scanning tunnelling microscope (STM) and apply it to perform a controlled study at the atomic scale of the interactions between isolated Mn acceptors, which are mediated by holes in GaAs. High-resolution STM measurements are used to visualize the GaAs electronic states that participate in the Mn-Mn interaction and to quantify the interaction strengths as a function of relative position and orientation. Our experimental findings, which can be explained using tight-binding model calculations, reveal a strong dependence of ferromagnetic interaction on crystallographic orientation. This anisotropic interaction can potentially be exploited by growing oriented Ga(1-x)Mn(x)As structures to enhance the ferromagnetic transition temperature beyond that achieved in randomly doped samples.

We show that electron and hole Landé g factors in self-assembled III-V quantum dots have a rich structure intermediate between that of paramagnetic atomic impurities and bulk semiconductors. Strain, dot geometry, and confinement energy modify the effective g factors, yet are insufficient to explain our results. We find that the dot's discrete energy spectrum quenches the orbital angular momentum, pushing the electron g factor towards 2, even when all the materials have negative bulk g factors. The approximate shape of a dot can be determined from measurements of the g factor asymmetry.