Exchange-biased quantum tunnelling in a supramolecular dimer of single-molecule magnets

Various present and future specialized applications of magnets require monodisperse, small magnetic particles, and the discovery of molecules that can function as nanoscale magnets was an important development in this regard. These molecules act as single-domain magnetic particles that, below their blocking temperature, exhibit magnetization hysteresis, a classical property of macroscopic magnets. Such 'single-molecule magnets' (SMMs) straddle the interface between classical and quantum mechanical behaviour because they also display quantum tunnelling of magnetization and quantum phase interference. Quantum tunnelling of magnetization can be advantageous for some potential applications of SMMs, for example, in providing the quantum superposition of states required for quantum computing. However, it is a disadvantage in other applications, such as information storage, where it would lead to information loss. Thus it is important to both understand and control the quantum properties of SMMs. Here we report a supramolecular SMM dimer in which antiferromagnetic coupling between the two components results in quantum behaviour different from that of the individual SMMs. Our experimental observations and theoretical analysis suggest a means of tuning the quantum tunnelling of magnetization in SMMs. This system may also prove useful for studying quantum tunnelling of relevance to mesoscopic antiferromagnets.     

Detecting excitation and magnetization of individual dopants in a semiconductor

An individual magnetic atom doped into a semiconductor is a promising building block for bottom-up spintronic devices and quantum logic gates. Moreover, it provides a perfect model system for the atomic-scale investigation of fundamental effects such as magnetism in dilute magnetic semiconductors. However, dopants in semiconductors so far have not been studied by magnetically sensitive techniques with atomic resolution that correlate the atomic structure with the dopant's magnetism. Here we show electrical excitation and read-out of a spin associated with a single magnetic dopant in a semiconductor host. We use spin-resolved scanning tunnelling spectroscopy to measure the spin excitations and the magnetization curve of individual iron surface-dopants embedded within a two-dimensional electron gas confined to an indium antimonide (110) surface. The dopants act like isolated quantum spins the states of which are governed by a substantial magnetic anisotropy that forces the spin to lie in the surface plane. This result is corroborated by our first principles calculations. The demonstrated methodology opens new routes for the investigation of sample systems that are more widely studied in the field of spintronics-that is, Mn in GaAs (ref. 5), magnetic ions in semiconductor quantum dots, nitrogen-vacancy centres in diamond and phosphorus spins in silicon.     

Chiral magnetic order at surfaces driven by inversion asymmetry

Chirality is a fascinating phenomenon that can manifest itself in subtle ways, for example in biochemistry (in the observed single-handedness of biomolecules) and in particle physics (in the charge-parity violation of electroweak interactions). In condensed matter, magnetic materials can also display single-handed, or homochiral, spin structures. This may be caused by the Dzyaloshinskii-Moriya interaction, which arises from spin-orbit scattering of electrons in an inversion-asymmetric crystal field. This effect is typically irrelevant in bulk metals as their crystals are inversion symmetric. However, low-dimensional systems lack structural inversion symmetry, so that homochiral spin structures may occur. Here we report the observation of magnetic order of a specific chirality in a single atomic layer of manganese on a tungsten (110) substrate. Spin-polarized scanning tunnelling microscopy reveals that adjacent spins are not perfectly antiferromagnetic but slightly canted, resulting in a spin spiral structure with a period of about 12 nm. We show by quantitative theory that this chiral order is caused by the Dzyaloshinskii-Moriya interaction and leads to a left-rotating spin cycloid. Our findings confirm the significance of this interaction for magnets in reduced dimensions. Chirality in nanoscale magnets may play a crucial role in spintronic devices, where the spin rather than the charge of an electron is used for data transmission and manipulation. For instance, a spin-polarized current flowing through chiral magnetic structures will exert a spin-torque on the magnetic structure, causing a variety of excitations or manipulations of the magnetization and giving rise to microwave emission, magnetization switching, or magnetic motors.     

Atom-by-atom substitution of Mn in GaAs and visualization of their hole-mediated interactions

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.     

Electrical detection of the spin resonance of a single electron in a silicon field-effect transistor

The ability to manipulate and monitor a single-electron spin using electron spin resonance is a long-sought goal. Such control would be invaluable for nanoscopic spin electronics, quantum information processing using individual electron spin qubits and magnetic resonance imaging of single molecules. There have been several examples of magnetic resonance detection of a single-electron spin in solids. Spin resonance of a nitrogen-vacancy defect centre in diamond has been detected optically, and spin precession of a localized electron spin on a surface was detected using scanning tunnelling microscopy. Spins in semiconductors are particularly attractive for study because of their very long decoherence times. Here we demonstrate electrical sensing of the magnetic resonance spin-flips of a single electron paramagnetic spin centre, formed by a defect in the gate oxide of a standard silicon transistor. The spin orientation is converted to electric charge, which we measure as a change in the source/drain channel current. Our set-up may facilitate the direct study of the physics of spin decoherence, and has the practical advantage of being composed of test transistors in a conventional, commercial, silicon integrated circuit. It is well known from the rich literature of magnetic resonance studies that there sometimes exist structural paramagnetic defects near the Si/SiO2 interface. For a small transistor, there might be only one isolated trap state that is within a tunnelling distance of the channel, and that has a charging energy close to the Fermi level.     

Tunable quantum tunnelling of magnetic domain walls

Perhaps the most anticipated, yet experimentally elusive, macroscopic quantum phenomenon is spin tunnelling in a ferromagnet, which may be formulated in terms of domain wall tunnelling. One approach to identifying such a process is to focus on mesoscopic systems where the number of domain walls is finite and the motion of a single wall has measurable consequences. Research of this type includes magnetotransport measurements on thin ferromagnetic wires, and magnetization experiments on single particles, nanomagnet ensembles and rare-earth multilayers. A second method is to investigate macroscopic disordered ferromagnets, whose dynamics are dominated by domain wall motion, and search the associated relaxation-time distribution functions for the signature of quantum effects. But whereas the classical, thermal processes that operate in these experiments are easily regulated via temperature, the quantum processes have so far not been tunable, making difficult a definitive interpretation of the results in terms of tunnelling. Here we describe a disordered magnetic system for which it is possible to adjust the quantum tunnelling probabilities. For this material, we can model both the classical, thermally activated response at high temperatures and the athermal, tunnelling behaviour at low temperatures within a unified framework, where the domain wall is described as a particle with a fixed mass. We show that it is possible to tune the quantum tunnelling processes by adjusting the 'mass' of this particle with an external magnetic field.     

Transformation of spin information into large electrical signals using carbon nanotubes

Spin electronics (spintronics) exploits the magnetic nature of electrons, and this principle is commercially applied in, for example, the spin valves of disk-drive read heads. There is currently widespread interest in developing new types of spintronic devices based on industrially relevant semiconductors, in which a spin-polarized current flows through a lateral channel between a spin-polarized source and drain. However, the transformation of spin information into large electrical signals is limited by spin relaxation, so that the magnetoresistive signals are below 1% (ref. 2). Here we report large magnetoresistance effects (61% at 5 K), which correspond to large output signals (65 mV), in devices where the non-magnetic channel is a multiwall carbon nanotube that spans a 1.5 microm gap between epitaxial electrodes of the highly spin polarized manganite La(0.7)Sr(0.3)MnO3. This spintronic system combines a number of favourable properties that enable this performance; the long spin lifetime in nanotubes due to the small spin-orbit coupling of carbon; the high Fermi velocity in nanotubes that limits the carrier dwell time; the high spin polarization in the manganite electrodes, which remains high right up to the manganite-nanotube interface; and the resistance of the interfacial barrier for spin injection. We support these conclusions regarding the interface using density functional theory calculations. The success of our experiments with such chemically and geometrically different materials should inspire new avenues in materials selection for future spintronics applications.     

Supercurrent reversal in quantum dots

When two superconductors are electrically connected by a weak link--such as a tunnel barrier--a zero-resistance supercurrent can flow. This supercurrent is carried by Cooper pairs of electrons with a combined charge of twice the elementary charge, e. The 2e charge quantum is clearly visible in the height of voltage steps in Josephson junctions under microwave irradiation, and in the magnetic flux periodicity of h/2e (where h is Planck's constant) in superconducting quantum interference devices. Here we study supercurrents through a quantum dot created in a semiconductor nanowire by local electrostatic gating. Owing to strong Coulomb interaction, electrons only tunnel one-by-one through the discrete energy levels of the quantum dot. This nevertheless can yield a supercurrent when subsequent tunnel events are coherent. These quantum coherent tunnelling processes can result in either a positive or a negative supercurrent, that is, in a normal or a pi-junction, respectively. We demonstrate that the supercurrent reverses sign by adding a single electron spin to the quantum dot. When excited states of the quantum dot are involved in transport, the supercurrent sign also depends on the character of the orbital wavefunctions.     

Orbital Kondo effect in carbon nanotubes

Progress in the fabrication of nanometre-scale electronic devices is opening new opportunities to uncover deeper aspects of the Kondo effect--a characteristic phenomenon in the physics of strongly correlated electrons. Artificial single-impurity Kondo systems have been realized in various nanostructures, including semiconductor quantum dots, carbon nanotubes and individual molecules. The Kondo effect is usually regarded as a spin-related phenomenon, namely the coherent exchange of the spin between a localized state and a Fermi sea of delocalized electrons. In principle, however, the role of the spin could be replaced by other degrees of freedom, such as an orbital quantum number. Here we show that the unique electronic structure of carbon nanotubes enables the observation of a purely orbital Kondo effect. We use a magnetic field to tune spin-polarized states into orbital degeneracy and conclude that the orbital quantum number is conserved during tunnelling. When orbital and spin degeneracies are present simultaneously, we observe a strongly enhanced Kondo effect, with a multiple splitting of the Kondo resonance at finite field and predicted to obey a so-called SU4 symmetry.     

Quantum oscillations in a molecular magnet

The term 'molecular magnet' generally refers to a molecular entity containing several magnetic ions whose coupled spins generate a collective spin, S (ref. 1). Such complex multi-spin systems provide attractive targets for the study of quantum effects at the mesoscopic scale. In these molecules, the large energy barriers between collective spin states can be crossed by thermal activation or quantum tunnelling, depending on the temperature or an applied magnetic field. There is the hope that these mesoscopic spin states can be harnessed for the realization of quantum bits--'qubits', the basic building blocks of a quantum computer--based on molecular magnets. But strong decoherence must be overcome if the envisaged applications are to become practical. Here we report the observation and analysis of Rabi oscillations (quantum oscillations resulting from the coherent absorption and emission of photons driven by an electromagnetic wave) of a molecular magnet in a hybrid system, in which discrete and well-separated magnetic clusters are embedded in a self-organized non-magnetic environment. Each cluster contains 15 antiferromagnetically coupled S = 1/2 spins, leading to an S = 1/2 collective ground state. When this system is placed into a resonant cavity, the microwave field induces oscillatory transitions between the ground and excited collective spin states, indicative of long-lived quantum coherence. The present observation of quantum oscillations suggests that low-dimension self-organized qubit networks having coherence times of the order of 100 micros (at liquid helium temperatures) are a realistic prospect.     

Quantum simulation of antiferromagnetic spin chains in an optical lattice

Understanding exotic forms of magnetism in quantum mechanical systems is a central goal of modern condensed matter physics, with implications for systems ranging from high-temperature superconductors to spintronic devices. Simulating magnetic materials in the vicinity of a quantum phase transition is computationally intractable on classical computers, owing to the extreme complexity arising from quantum entanglement between the constituent magnetic spins. Here we use a degenerate Bose gas of rubidium atoms confined in an optical lattice to simulate a chain of interacting quantum Ising spins as they undergo a phase transition. Strong spin interactions are achieved through a site-occupation to pseudo-spin mapping. As we vary a magnetic field, quantum fluctuations drive a phase transition from a paramagnetic phase into an antiferromagnetic phase. In the paramagnetic phase, the interaction between the spins is overwhelmed by the applied field, which aligns the spins. In the antiferromagnetic phase, the interaction dominates and produces staggered magnetic ordering. Magnetic domain formation is observed through both in situ site-resolved imaging and noise correlation measurements. By demonstrating a route to quantum magnetism in an optical lattice, this work should facilitate further investigations of magnetic models using ultracold atoms, thereby improving our understanding of real magnetic materials.     

Quantum phase transition in a single-molecule quantum dot

Quantum criticality is the intriguing possibility offered by the laws of quantum mechanics when the wave function of a many-particle physical system is forced to evolve continuously between two distinct, competing ground states. This phenomenon, often related to a zero-temperature magnetic phase transition, is believed to govern many of the fascinating properties of strongly correlated systems such as heavy-fermion compounds or high-temperature superconductors. In contrast to bulk materials with very complex electronic structures, artificial nanoscale devices could offer a new and simpler means of understanding quantum phase transitions. Here we demonstrate this possibility in a single-molecule quantum dot, where a gate voltage induces a crossing of two different types of electron spin state (singlet and triplet) at zero magnetic field. The quantum dot is operated in the Kondo regime, where the electron spin on the quantum dot is partially screened by metallic electrodes. This strong electronic coupling between the quantum dot and the metallic contacts provides the strong electron correlations necessary to observe quantum critical behaviour. The quantum magnetic phase transition between two different Kondo regimes is achieved by tuning gate voltages and is fundamentally different from previously observed Kondo transitions in semiconductor and nanotube quantum dots. Our work may offer new directions in terms of control and tunability for molecular spintronics.     

Optically programmable electron spin memory using semiconductor quantum dots

The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.     

Entangled quantum state of magnetic dipoles

Free magnetic moments usually manifest themselves in Curie laws, where weak external magnetic fields produce magnetizations that vary as the reciprocal of the temperature (1/T). For a variety of materials that do not display static magnetism, including doped semiconductors and certain rare-earth intermetallics, the 1/T law is replaced by a power law T(-alpha) with alpha < 1. Here we show that a much simpler material system-namely, the insulating magnetic salt LiHo(x)Y(1-x)F(4)-can also display such a power law. Moreover, by comparing the results of numerical simulations of this system with susceptibility and specific-heat data, we show that both energy-level splitting and quantum entanglement are crucial to describing its behaviour. The second of these quantum mechanical effects-entanglement, where the wavefunction of a system with several degrees of freedom cannot be written as a product of wavefunctions for each degree of freedom-becomes visible for remarkably small tunnelling terms, and is activated well before tunnelling has visible effects on the spectrum. This finding is significant because it shows that entanglement, rather than energy-level redistribution, can underlie the magnetic behaviour of a simple insulating quantum spin system.     

Single-shot read-out of an individual electron spin in a quantum dot

Spin is a fundamental property of all elementary particles. Classically it can be viewed as a tiny magnetic moment, but a measurement of an electron spin along the direction of an external magnetic field can have only two outcomes: parallel or anti-parallel to the field. This discreteness reflects the quantum mechanical nature of spin. Ensembles of many spins have found diverse applications ranging from magnetic resonance imaging to magneto-electronic devices, while individual spins are considered as carriers for quantum information. Read-out of single spin states has been achieved using optical techniques, and is within reach of magnetic resonance force microscopy. However, electrical read-out of single spins has so far remained elusive. Here we demonstrate electrical single-shot measurement of the state of an individual electron spin in a semiconductor quantum dot. We use spin-to-charge conversion of a single electron confined in the dot, and detect the single-electron charge using a quantum point contact; the spin measurement visibility is approximately 65%. Furthermore, we observe very long single-spin energy relaxation times (up to approximately 0.85 ms at a magnetic field of 8 T), which are encouraging for the use of electron spins as carriers of quantum information.     

Emerging local Kondo screening and spatial coherence in the heavy-fermion metal YbRh2Si2

The entanglement of quantum states is both a central concept in fundamental physics and a potential tool for realizing advanced materials and applications. The quantum superpositions underlying entanglement are at the heart of the intricate interplay of localized spin states and itinerant electronic states that gives rise to the Kondo effect in certain dilute magnetic alloys. In systems where the density of localized spin states is sufficiently high, they can no longer be treated as non-interacting; if they form a dense periodic array, a Kondo lattice may be established. Such a Kondo lattice gives rise to the emergence of charge carriers with enhanced effective masses, but the precise nature of the coherent Kondo state responsible for the generation of these heavy fermions remains highly debated. Here we use atomic-resolution tunnelling spectroscopy to investigate the low-energy excitations of a generic Kondo lattice system, YbRh(2)Si(2). We find that the hybridization of the conduction electrons with the localized 4f electrons results in a decrease in the tunnelling conductance at the Fermi energy. In addition, we observe unambiguously the crystal-field excitations of the Yb(3+) ions. A strongly temperature-dependent peak in the tunnelling conductance is attributed to the Fano resonance resulting from tunnelling into the coherent heavy-fermion states that emerge at low temperature. Taken together, these features reveal how quantum coherence develops in heavy 4f-electron Kondo lattices. Our results demonstrate the efficiency of real-space electronic structure imaging for the investigation of strong electronic correlations, specifically with respect to coherence phenomena, phase coexistence and quantum criticality.     

Kondo effect in an integer-spin quantum dot

The Kondo effect--a many-body phenomenon in condensed-matter physics involving the interaction between a localized spin and free electrons--was discovered in metals containing small amounts of magnetic impurities, although it is now recognized to be of fundamental importance in a wide class of correlated electron systems. In fabricated structures, the control of single, localized spins is of technological relevance for nanoscale electronics. Experiments have already demonstrated artificial realizations of isolated magnetic impurities at metallic surfaces, nanoscale magnets, controlled transitions between two-electron singlet and triplet states, and a tunable Kondo effect in semiconductor quantum dots. Here we report an unexpected Kondo effect in a few-electron quantum dot containing singlet and triplet spin states, whose energy difference can be tuned with a magnetic field. We observe the effect for an even number of electrons, when the singlet and triplet states are degenerate. The characteristic energy scale is much larger than in the ordinary spin-1/2 case.     

Electronic measurement and control of spin transport in silicon

The spin lifetime and diffusion length of electrons are transport parameters that define the scale of coherence in spintronic devices and circuits. As these parameters are many orders of magnitude larger in semiconductors than in metals, semiconductors could be the most suitable for spintronics. So far, spin transport has only been measured in direct-bandgap semiconductors or in combination with magnetic semiconductors, excluding a wide range of non-magnetic semiconductors with indirect bandgaps. Most notable in this group is silicon, Si, which (in addition to its market entrenchment in electronics) has long been predicted a superior semiconductor for spintronics with enhanced lifetime and transport length due to low spin-orbit scattering and lattice inversion symmetry. Despite this promise, a demonstration of coherent spin transport in Si has remained elusive, because most experiments focused on magnetoresistive devices; these methods fail because of a fundamental impedance mismatch between ferromagnetic metal and semiconductor, and measurements are obscured by other magnetoelectronic effects. Here we demonstrate conduction-band spin transport across 10 mum undoped Si in a device that operates by spin-dependent ballistic hot-electron filtering through ferromagnetic thin films for both spin injection and spin detection. As it is not based on magnetoresistance, the hot-electron spin injection and spin detection avoids impedance mismatch issues and prevents interference from parasitic effects. The clean collector current shows independent magnetic and electrical control of spin precession, and thus confirms spin coherent drift in the conduction band of silicon.     

Microwave oscillations of a nanomagnet driven by a spin-polarized current

The recent discovery that a spin-polarized electrical current can apply a large torque to a ferromagnet, through direct transfer of spin angular momentum, offers the possibility of manipulating magnetic-device elements without applying cumbersome magnetic fields. However, a central question remains unresolved: what type of magnetic motions can be generated by this torque? Theory predicts that spin transfer may be able to drive a nanomagnet into types of oscillatory magnetic modes not attainable with magnetic fields alone, but existing measurement techniques have provided only indirect evidence for dynamical states. The nature of the possible motions has not been determined. Here we demonstrate a technique that allows direct electrical measurements of microwave-frequency dynamics in individual nanomagnets, propelled by a d.c. spin-polarized current. We show that spin transfer can produce several different types of magnetic excitation. Although there is no mechanical motion, a simple magnetic-multilayer structure acts like a nanoscale motor; it converts energy from a d.c. electrical current into high-frequency magnetic rotations that might be applied in new devices including microwave sources and resonators.     

Giant magnetoresistance in organic spin-valves

A spin valve is a layered structure of magnetic and non-magnetic (spacer) materials whose electrical resistance depends on the spin state of electrons passing through the device and so can be controlled by an external magnetic field. The discoveries of giant magnetoresistance and tunnelling magnetoresistance in metallic spin valves have revolutionized applications such as magnetic recording and memory, and launched the new field of spin electronics--'spintronics'. Intense research efforts are now devoted to extending these spin-dependent effects to semiconductor materials. But while there have been noteworthy advances in spin injection and detection using inorganic semiconductors, spin-valve devices with semiconducting spacers have not yet been demonstrated. pi-conjugated organic semiconductors may offer a promising alternative approach to semiconductor spintronics, by virtue of their relatively strong electron-phonon coupling and large spin coherence. Here we report the injection, transport and detection of spin-polarized carriers using an organic semiconductor as the spacer layer in a spin-valve structure, yielding low-temperature giant magnetoresistance effects as large as 40 per cent.