Magnetic superstructure in the two-dimensional quantum antiferromagnet SrCu2(BO3)2

We report the observation of magnetic superstructure in a magnetization plateau state of SrCu2(BO3)2, a frustrated quasi-two-dimensional quantum spin system. The Cu and B nuclear magnetic resonance (NMR) spectra at 35 millikelvin indicate an apparently discontinuous phase transition from uniform magnetization to a modulated superstructure near 27 tesla, above which a magnetization plateau at 1/8 of the full saturation has been observed. Comparison of the Cu NMR spectrum and the theoretical analysis of a Heisenberg spin model demonstrates the crystallization of itinerant triplets in the plateau phase within a large rhomboid unit cell (16 spins per layer) showing oscillations of the spin polarization. Thus, we are now in possession of an interesting model system to study a localization transition of strongly interacting quantum particles.     

Magnetization precession by hot spin injection

As electrons are injected at various energies into ferromagnetic material with their spin polarization vector perpendicular to the axis of the magnetization, we observe precessional motion of the spin polarization on the femtosecond time scale. Because of angular momentum conservation, the magnetization vector must precess as well. We show that spin injection will generate the precessional magnetization reversal in nanosized ferromagnetic bits. At reasonable injected current densities this occurs on the picosecond time scale.     

Direct observation of internal spin structure of magnetic vortex cores

Thin film nanoscale elements with a curling magnetic structure (vortex) are a promising candidate for future nonvolatile data storage devices. Their properties are strongly influenced by the spin structure in the vortex core. We have used spin-polarized scanning tunneling microscopy on nanoscale iron islands to probe for the first time the internal spin structure of magnetic vortex cores. Using tips coated with a layer of antiferromagnetic chromium, we obtained images of the curling in-plane magnetization around and of the out-of-plane magnetization inside the core region. The experimental data are compared with micromagnetic simulations. The results confirm theoretical predictions that the size and the shape of the vortex core as well as its magnetic field dependence are governed by only two material parameters, the exchange stiffness and the saturation magnetization that determines the stray field energy.     

Ferromagnetic imprinting of nuclear spins in semiconductors

We examine how a ferromagnetic layer affects the coherent electron spin dynamics in a neighboring gallium arsenide semiconductor. Ultrafast optical pump-probe measurements reveal that the spin dynamics are unexpectedly dominated by hyperpolarized nuclear spins that align along the ferromagnet's magnetization. We find evidence that photoexcited carriers acquire spin-polarization from the ferromagnet, and dynamically polarize these nuclear spins. The resulting hyperfine fields are as high as 9000 gauss in small external fields (less than 1000 gauss), enabling ferromagnetic control of local electron spin coherence.     

Imaging spin transport in lateral ferromagnet/semiconductor structures

We directly imaged electrical spin injection and accumulation in the gallium arsenide channel of lateral spin-transport devices, which have ferromagnetic source and drain tunnel-barrier contacts. The emission of spins from the source was observed, and a region of spin accumulation was imaged near the ferromagnetic drain contact. Both injected and accumulated spins have the same orientation (antiparallel to the contact magnetization), and we show that the accumulated spin polarization flows away from the drain (against the net electron current), indicating that electron spins are polarized by reflection from the ferromagnetic drain contact. The electrical conductance can be modulated by controlling the spin orientation of optically injected electrons flowing through the drain.     

Large magnetic anisotropy of a single atomic spin embedded in a surface molecular network

Magnetic anisotropy allows magnets to maintain their direction of magnetization over time. Using a scanning tunneling microscope to observe spin excitations, we determined the orientation and strength of the anisotropies of individual iron and manganese atoms on a thin layer of copper nitride. The relative intensities of the inelastic tunneling processes are consistent with dipolar interactions, as seen for inelastic neutron scattering. First-principles calculations indicate that the magnetic atoms become incorporated into a polar covalent surface molecular network in the copper nitride. These structures, which provide atom-by-atom accessibility via local probes, have the potential for engineering anisotropies large enough to produce stable magnetization at low temperatures for a single atomic spin.     

Imaging precessional motion of the magnetization vector

We report on imaging of three-dimensional precessional orbits of the magnetization vector in a magnetic field by means of a time-resolved vectorial Kerr experiment that measures all three components of the magnetization vector with picosecond resolution. Images of the precessional mode taken with submicrometer spatial resolution reveal that the dynamical excitation in this time regime roughly mirrors the symmetry of the underlying equilibrium spin configuration and that its propagation has a non-wavelike character. These results should form the basis for realistic models of the magnetization dynamics in a largely unexplored but technologically increasingly relevant time scale.     

Spin-polarized light-emitting diode based on an organic bipolar spin valve

The spin-polarized organic light-emitting diode (spin-OLED) has been a long-sought device within the field of organic spintronics. We designed, fabricated, and studied a spin-OLED with ferromagnetic electrodes that acts as a bipolar organic spin valve (OSV), based on a deuterated derivative of poly(phenylene-vinylene) with small hyperfine interaction. In the double-injection limit, the device shows ~1% spin valve magneto-electroluminescence (MEL) response, which follows the ferromagnetic electrode coercive fields and originates from the bipolar spin-polarized space charge-limited current. In stark contrast to the response properties of homopolar OSV devices, the MEL response in the double-injection device is practically independent of bias voltage, and its temperature dependence follows that of the ferromagnetic electrode magnetization. Our findings provide a pathway for organic displays controlled by external magnetic fields.     

Magnetic bistability of molecules in homogeneous solution at room temperature

Magnetic bistability, as manifested in the magnetization of ferromagnetic materials or spin crossover in transition metal complexes, has essentially been restricted to either bulk materials or to very low temperatures. We now present a molecular spin switch that is bistable at room temperature in homogeneous solution. Irradiation of a carefully designed nickel complex with blue-green light (500 nanometers) induces coordination of a tethered pyridine ligand and concomitant electronic rearrangement from a diamagnetic to a paramagnetic state in up to 75% of the ensemble. The process is fully reversible on irradiation with violet-blue light (435 nanometers). No fatigue or degradation is observed after several thousand cycles at room temperature under air. Preliminary data show promise for applications in magnetic resonance imaging.     

Current-induced magnetization switching with a spin-polarized scanning tunneling microscope

Switching the magnetization of a magnetic bit by injection of a spin-polarized current offers the possibility for the development of innovative high-density data storage technologies. We show how individual superparamagnetic iron nanoislands with typical sizes of 100 atoms can be addressed and locally switched using a magnetic scanning probe tip, thus demonstrating current-induced magnetization reversal across a vacuum barrier combined with the ultimate resolution of spin-polarized scanning tunneling microscopy. Our technique allows us to separate and quantify three fundamental contributions involved in magnetization switching (i.e., current-induced spin torque, heating the island by the tunneling current, and Oersted field effects), thereby providing an improved understanding of the switching mechanism.     

Spontaneous Magnetic Ordering in the Fullerene Charge-Transfer Salt (TDAE)C60

The zero-field muon spin relaxation technique has been used in the direct observation of spontaneous magnetic order below a Curie temperature (T(c)) of approximately 16.1 kelvin in the fullerene charge-transfer salt (tetrakisdimethylaminoethylene)C(60) [(TDAE)C(60)]. Coherent ordering of the electronic magnetic moments leads to a local field of 68(1) gauss at the muon site at 3.2 kelvin (parentheses indicate the error in the last digit). Substantial spatially inhomogeneous effects are manifested in the distribution of the local fields, whose width amounts to 48(2) gauss at the same temperature. The temperature evolution of the internal magnetic field below the freezing temperature mirrors that of the saturation magnetization, closely following the behavior expected for collective spin wave (magnon) excitations. The transition to a ferromagnetic state with a T(c) higher than that of any other organic material is now authenticated.     

Some developments in nuclear magnetic resonance of solids

Nuclear magnetic resonance (NMR) spectroscopy continues to evolve as a primary technique in the study of solids. This review briefly describes some developments in modern NMR that demonstrate its exciting potential as an analytical tool in fields as diverse as physics, chemistry, biology, geology, and materials science. Topics covered include motional narrowing by sample reorientation, multiple-quantum and overtone spectroscopy, probing porous solids with guest atoms and molecules, two-dimensional NMR studies of chemical exchange and spin diffusion, experiments at extreme temperatures, NMR imaging of solid materials, and low-frequency and zero-field magnetic resonance. These developments permit increasingly complex structural and dynamical behavior to be probed at a molecular level and thus add to our understanding of macroscopic properties of materials.     

A magnetically focused molecular beam of ortho-water

Like dihydrogen, water exists as two spin isomers, ortho and para, with the nuclear magnetic moments of the hydrogen atoms either parallel or antiparallel. The ratio of the two spin isomers and their physical properties play an important role in a wide variety of research fields, ranging from astrophysics to nuclear magnetic resonance (NMR). Unlike ortho and para H(2), however, the two water isomers remain challenging to separate, and as a consequence, very little is currently known about their different physical properties. Here, we report the formation of a magnetically focused molecular beam of ortho-water. The beam we formed also had a particular spin projection. Thus, in the presence of holding magnetic fields, the water molecules are hyperpolarized, laying the foundation for ultrasensitive NMR experiments in the future.     

Spin transfer torques in MnSi at ultralow current densities

Spin manipulation using electric currents is one of the most promising directions in the field of spintronics. We used neutron scattering to observe the influence of an electric current on the magnetic structure in a bulk material. In the skyrmion lattice of manganese silicon, where the spins form a lattice of magnetic vortices similar to the vortex lattice in type II superconductors, we observe the rotation of the diffraction pattern in response to currents that are over five orders of magnitude smaller than those typically applied in experimental studies on current-driven magnetization dynamics in nanostructures. We attribute our observations to an extremely efficient coupling of inhomogeneous spin currents to topologically stable knots in spin structures.     

All-optical magnetic resonance in semiconductors

A scheme is proposed wherein nuclear magnetic resonance (NMR) can be induced and monitored using only optical fields. In analogy to radio-frequency fields used in traditional NMR, circularly polarized light creates electron spins in semiconductors whose hyperfine coupling could tip nuclear moments. Time-resolved Faraday rotation experiments were performed in which the frequency of electron Larmor precession was used as a magnetometer of local magnetic fields experienced by electrons in n-type gallium arsenide. Electron spin excitation by a periodic optical pulse train appears not only to prepare a hyperpolarized nuclear moment but also to destroy it resonantly at magnetic fields proportional to the pulse frequency. This resonant behavior is in many ways supportive of a simple model of optically induced NMR, but a curious discrepancy between one of the observed frequencies and classic NMR values suggests that this phenomenon is more complex.     

Ultraslow electron spin dynamics in GaAs quantum wells probed by optically pumped NMR

Optically pumped nuclear magnetic resonance (OPNMR) measurements were performed in two different electron-doped multiple quantum well samples near the fractional quantum Hall effect ground state nu = 13. Below 0.5 kelvin, the spectra provide evidence that spin-reversed charged excitations of the nu = 13 ground state are localized over the NMR time scale of about 40 microseconds. Furthermore, by varying NMR pulse parameters, the electron spin temperature (as measured by the Knight shift) could be driven above the lattice temperature, which shows that the value of the electron spin-lattice relaxation time tau1s is between 100 microseconds and 500 milliseconds at nu = 13.     

Observation of half-height magnetization steps in Sr2RuO4

Spin-triplet superfluids can support exotic objects, such as half-quantum vortices characterized by the nontrivial winding of the spin structure. We present cantilever magnetometry measurements performed on mesoscopic samples of Sr(2)RuO(4), a spin-triplet superconductor. With micrometer-sized annular-shaped samples, we observed transitions between integer fluxoid states as well as a regime characterized by "half-integer transitions"--steps in the magnetization with half the height of the ones we observed between integer fluxoid states. These half-height steps are consistent with the existence of half-quantum vortices in superconducting Sr(2)RuO(4).     

Multiple-quantum nuclear magnetic resonance spectroscopy

A nuclear magnetic resonance (NMR) event is popularly viewed as the flip of a single spin in a magnetc field, stimulated by the absorption or emission of only one quantum of radio-frequency energy. Nevertheless, resonances between nuclear spin states that differ by more than one unit in the Zeeman quantum number also can be induced in systems of coupled spins by suitably designed sequences of radio-frequency pulses. Pairs of states excited in this way oscillate coherently at the frequencies of the corresponding multiple-quantum transitions and produce a response that may be monitored indirectly in a two-dimensional time-domain experiment. The pattern of multiple-quantum excitation and response, influenced largely by the concerted interactions of groups of coupled nuclei, simplifies the NMR spectrum in some instances and provides significant new information in others. Applications of multiple-quantum NMR extend to problems in many different areas, ranging from studies of the structure and function of proteins and nucleic acids in solution to investigations of the arrangements of atoms in amorphous semiconductors. The specific spectroscopic techniques are varied as well and include methods designed, for example, to simplify spectral analysis for liquids and liquid crystals, eliminate inhomogeneous broadening, study interatomic connectivity in liquid-state molecules, identify clusters of atoms in solids, enhance the spatial resolution in solid-state imaging experiments, and probe correlated molecular motions.     

A molecular-based magnet with a fully interlocked three-dimensional structure

A compound has been synthesized with the formula (rad)(2)Mn(2)[Cu(opba)](3)(DMSO)(2).2H(2)O, where rad(+) is 2-(4-N-methylpyridinium)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide, opba is orthophenylenebis(oxamato), and DMSO is dimethyl sulfoxide. It consists of two nearly perpendicular graphite-like networks with edge-sharing Mn(II)(6)Cu(II)(6) hexagons. The two networks are fully interlocked with the same topological relationship as that between adjacent rings of a necklace. The compound has three kinds of spin carriers: Mn(II) and Cu(II) ions, antiferromagnetically coupled through oxamato bridges, and rad(+) radical cations, bridging the Cu(II) ions through the nitronyl nitroxide groups and forming Cu-rad chains. The temperature dependence of the magnetization reveals that below 22.5 K, the compound behaves as a magnet.     

Determination of membrane protein structure by rotational resonance NMR: bacteriorhodopsin

Rotationally resonant magnetization exchange, a new nuclear magnetic resonance (NMR) technique for measuring internuclear distances between like spins in solids, was used to determine the distance between the C-8 and C-18 carbons of retinal in two model compounds and in the membrane protein bacteriorhodopsin. Magnetization transfer between inequivalent spins with an isotropic shift separation, delta, is driven by magic angle spinning at a speed omega r that matches the rotational resonance condition delta = n omega r, where n is a small integer. The distances measured in this way for both the 6-s-cis- and 6-s-trans-retinoic acid model compounds agreed well with crystallographically known distances. In bacteriorhodopsin the exchange trajectory between C-8 and C-18 was in good agreement with the internuclear distance for a 6-s-trans configuration [4.2 angstroms (A)] and inconsistent with that for a 6-s-cis configuration (3.1 A). The results illustrate that rotational resonance can be used for structural studies in membrane proteins and in other situations where diffraction and solution NMR techniques yield limited information.