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.     

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.     

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.     

量子纠缠对两个原子玻色-爱因斯坦凝聚隧穿动力学的影响

研究了两原子玻色-爱因斯坦凝聚系统初态处于纠缠相干态时的布居差和隧穿电流,详细讨论了量子纠缠对两个凝聚间的隧穿动力学的影响．     

Scaling of entanglement close to a quantum phase transition

Classical phase transitions occur when a physical system reaches a state below a critical temperature characterized by macroscopic order. Quantum phase transitions occur at absolute zero; they are induced by the change of an external parameter or coupling constant, and are driven by quantum fluctuations. Examples include transitions in quantum Hall systems, localization in Si-MOSFETs (metal oxide silicon field-effect transistors; ref. 4) and the superconductor-insulator transition in two-dimensional systems. Both classical and quantum critical points are governed by a diverging correlation length, although quantum systems possess additional correlations that do not have a classical counterpart. This phenomenon, known as entanglement, is the resource that enables quantum computation and communication. The role of entanglement at a phase transition is not captured by statistical mechanics-a complete classification of the critical many-body state requires the introduction of concepts from quantum information theory. Here we connect the theory of critical phenomena with quantum information by exploring the entangling resources of a system close to its quantum critical point. We demonstrate, for a class of one-dimensional magnetic systems, that entanglement shows scaling behaviour in the vicinity of the transition point.     

Preparation and measurement of three-qubit entanglement in a superconducting circuit

Traditionally, quantum entanglement has been central to foundational discussions of quantum mechanics. The measurement of correlations between entangled particles can have results at odds with classical behaviour. These discrepancies grow exponentially with the number of entangled particles. With the ample experimental confirmation of quantum mechanical predictions, entanglement has evolved from a philosophical conundrum into a key resource for technologies such as quantum communication and computation. Although entanglement in superconducting circuits has been limited so far to two qubits, the extension of entanglement to three, eight and ten qubits has been achieved among spins, ions and photons, respectively. A key question for solid-state quantum information processing is whether an engineered system could display the multi-qubit entanglement necessary for quantum error correction, which starts with tripartite entanglement. Here, using a circuit quantum electrodynamics architecture, we demonstrate deterministic production of three-qubit Greenberger-Horne-Zeilinger (GHZ) states with fidelity of 88 per cent, measured with quantum state tomography. Several entanglement witnesses detect genuine three-qubit entanglement by violating biseparable bounds by 830?±?80 per cent. We demonstrate the first step of basic quantum error correction, namely the encoding of a logical qubit into a manifold of GHZ-like states using a repetition code. The integration of this encoding with decoding and error-correcting steps in a feedback loop will be the next step for quantum computing with integrated circuits.     

量子纠缠控制的核磁共振实验演示

量子纠缠在量子信息领域中有着极重要的应用,是当前人们研究的热门课题之一[1-2].量子纠缠控制是一种量子相干控制,即系统的量子力学进程在我们的控制之下,并使之产生期望的结果[3-4].我们在一个3量子位的核磁共振量子计算机实现了2个方面量子纠缠控制:纠缠互换与存储.我们使用赝纯态作为系统的初始状态.通过赝纯态,系统的微观性质可用宏观信号表述出来.     

海森伯格XXZ模型的热纠缠

负值度(Negativity)是一种通用的纠缠度量,可方便地计算两体量子系统的纠缠度.利用负值度研究了两量子比特各向异性海森伯格XXZ模型的热纠缠,讨论了在热平衡时温度和外加磁场对热纠缠的影响.当温度小于临界温度时,热纠缠的大小依赖于外加磁场的强弱;当温度大于临界温度时,纠缠消失.     

Visualizing heavy fermions emerging in a quantum critical Kondo lattice

In solids containing elements with f orbitals, the interaction between f-electron spins and those of itinerant electrons leads to the development of low-energy fermionic excitations with a heavy effective mass. These excitations are fundamental to the appearance of unconventional superconductivity and non-Fermi-liquid behaviour observed in actinide- and lanthanide-based compounds. Here we use spectroscopic mapping with the scanning tunnelling microscope to detect the emergence of heavy excitations with lowering of temperature in a prototypical family of cerium-based heavy-fermion compounds. We demonstrate the sensitivity of the tunnelling process to the composite nature of these heavy quasiparticles, which arises from quantum entanglement of itinerant conduction and f electrons. Scattering and interference of the composite quasiparticles is used to resolve their energy-momentum structure and to extract their mass enhancement, which develops with decreasing temperature. The lifetime of the emergent heavy quasiparticles reveals signatures of enhanced scattering and their spectral lineshape shows evidence of energy-temperature scaling. These findings demonstrate that proximity to a quantum critical point results in critical damping of the emergent heavy excitation of our Kondo lattice system.     

Quantum tunnelling of the magnetization in a monolayer of oriented single-molecule magnets

A fundamental step towards atomic- or molecular-scale spintronic devices has recently been made by demonstrating that the spin of an individual atom deposited on a surface, or of a small paramagnetic molecule embedded in a nanojunction, can be externally controlled. An appealing next step is the extension of such a capability to the field of information storage, by taking advantage of the magnetic bistability and rich quantum behaviour of single-molecule magnets (SMMs). Recently, a proof of concept that the magnetic memory effect is retained when SMMs are chemically anchored to a metallic surface was provided. However, control of the nanoscale organization of these complex systems is required for SMMs to be integrated into molecular spintronic devices. Here we show that a preferential orientation of Fe(4) complexes on a gold surface can be achieved by chemical tailoring. As a result, the most striking quantum feature of SMMs-their stepped hysteresis loop, which results from resonant quantum tunnelling of the magnetization-can be clearly detected using synchrotron-based spectroscopic techniques. With the aid of multiple theoretical approaches, we relate the angular dependence of the quantum tunnelling resonances to the adsorption geometry, and demonstrate that molecules predominantly lie with their easy axes close to the surface normal. Our findings prove that the quantum spin dynamics can be observed in SMMs chemically grafted to surfaces, and offer a tool to reveal the organization of matter at the nanoscale.     

Decoherence in crystals of quantum molecular magnets

Quantum decoherence is a central concept in physics. Applications such as quantum information processing depend on understanding it; there are even fundamental theories proposed that go beyond quantum mechanics, in which the breakdown of quantum theory would appear as an 'intrinsic' decoherence, mimicking the more familiar environmental decoherence processes. Such applications cannot be optimized, and such theories cannot be tested, until we have a firm handle on ordinary environmental decoherence processes. Here we show that the theory for insulating electronic spin systems can make accurate and testable predictions for environmental decoherence in molecular-based quantum magnets. Experiments on molecular magnets have successfully demonstrated quantum-coherent phenomena but the decoherence processes that ultimately limit such behaviour were not well constrained. For molecular magnets, theory predicts three principal contributions to environmental decoherence: from phonons, from nuclear spins and from intermolecular dipolar interactions. We use high magnetic fields on single crystals of Fe(8) molecular magnets (in which the Fe ions are surrounded by organic ligands) to suppress dipolar and nuclear-spin decoherence. In these high-field experiments, we find that the decoherence time varies strongly as a function of temperature and magnetic field. The theoretical predictions are fully verified experimentally, and there are no other visible decoherence sources. In these high fields, we obtain a maximum decoherence quality-factor of 1.49?×?10(6); our investigation suggests that the environmental decoherence time can be extended up to about 500 microseconds, with a decoherence quality factor of ～6?×?10(7), by optimizing the temperature, magnetic field and nuclear isotopic concentrations.     

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.     

Polarons and confinement of electronic motion to two dimensions in a layered manganite

A remarkable feature of layered transition--metal oxides-most famously, the high-temperature superconductors--is that they can display hugely anisotropic electrical and optical properties (for example, seeming to be insulating perpendicular to the layers and metallic within them), even when prepared as bulk three-dimensional single crystals. This is the phenomenon of 'confinement', a concept at odds with the conventional theory of solids, and recognized as due to magnetic and electron-lattice interactions within the layers that must be overcome at a substantial energy cost if electrons are to be transferred between layers. The associated energy gap, or 'pseudogap', is particularly obvious in experiments where charge is moved perpendicular to the planes, most notably scanning tunnelling microscopy and polarized infrared spectroscopy. Here, using the same experimental tools, we show that there is a second family of transition-metal oxides--the layered manganites La(2-2x)Sr(1+2x)Mn2O7--with even more extreme confinement and pseudogap effects. The data demonstrate quantitatively that because the charge carriers are attached to polarons (lattice- and spin-textures within the planes), it is as difficult to remove them from the planes through vacuum-tunnelling into a conventional metallic tip, as it is for them to move between Mn-rich layers within the material itself.     

Quantum suppression of superconductivity in ultrathin nanowires

It is of fundamental importance to establish whether there is a limit to how thin a superconducting wire can be, while retaining its superconducting character--and if there is a limit, to determine what sets it. This issue may also be of practical importance in defining the limit to miniaturization of superconducting electronic circuits. At high temperatures, the resistance of linear superconductors is caused by excitations called thermally activated phase slips. Quantum tunnelling of phase slips is another possible source of resistance that is still being debated. It has been theoretically predicted that such quantum phase slips can destroy superconductivity in very narrow wires. Here we report resistance measurements on ultrathin (< or = 10 nm) nanowires produced by coating carbon nanotubes with a superconducting Mo-Ge alloy. We find that nanowires can be superconducting or insulating depending on the ratio of their normal-state resistance (R(N)) to the quantum resistance for Cooper pairs (Rq). If R(N) < Rq, quantum tunnelling of phase slips is prohibited by strong damping, and so the wires stay superconducting. In contrast, we observe an insulating state for R(N) > Rq, which we explain in terms of proliferation of quantum phase slips and a corresponding localization of Cooper pairs.     

Kondo resonance in a single-molecule transistor

When an individual molecule, nanocrystal, nanotube or lithographically defined quantum dot is attached to metallic electrodes via tunnel barriers, electron transport is dominated by single-electron charging and energy-level quantization. As the coupling to the electrodes increases, higher-order tunnelling and correlated electron motion give rise to new phenomena, including the Kondo resonance. To date, all of the studies of Kondo phenomena in quantum dots have been performed on systems where precise control over the spin degrees of freedom is difficult. Molecules incorporating transition-metal atoms provide powerful new systems in this regard, because the spin and orbital degrees of freedom can be controlled through well-defined chemistry. Here we report the observation of the Kondo effect in single-molecule transistors, where an individual divanadium molecule serves as a spin impurity. We find that the Kondo resonance can be tuned reversibly using the gate voltage to alter the charge and spin state of the molecule. The resonance persists at temperatures up to 30 K and when the energy separation between the molecular state and the Fermi level of the metal exceeds 100 meV.     

Quantum phase transition in a resonant level coupled to interacting leads

A Luttinger liquid is an interacting one-dimensional electronic system, quite distinct from the 'conventional' Fermi liquids formed by interacting electrons in two and three dimensions. Some of the most striking properties of Luttinger liquids are revealed in the process of electron tunnelling. For example, as a function of the applied bias voltage or temperature, the tunnelling current exhibits a non-trivial power-law suppression. (There is no such suppression in a conventional Fermi liquid.) Here, using a carbon nanotube connected to resistive leads, we create a system that emulates tunnelling in a Luttinger liquid, by controlling the interaction of the tunnelling electron with its environment. We further replace a single tunnelling barrier with a double-barrier, resonant-level structure and investigate resonant tunnelling between Luttinger liquids. At low temperatures, we observe perfect transparency of the resonant level embedded in the interacting environment, and the width of the resonance tends to zero. We argue that this behaviour results from many-body physics of interacting electrons, and signals the presence of a quantum phase transition. Given that many parameters, including the interaction strength, can be precisely controlled in our samples, this is an attractive model system for studying quantum critical phenomena in general, with wide-reaching implications for understanding quantum phase transitions in more complex systems, such as cold atoms and strongly correlated bulk materials.     

Mapping photonic entanglement into and out of a quantum memory

Developments in quantum information science rely critically on entanglement-a fundamental aspect of quantum mechanics that causes parts of a composite system to show correlations stronger than can be explained classically. In particular, scalable quantum networks require the capability to create, store and distribute entanglement among distant matter nodes by means of photonic channels. Atomic ensembles can play the role of such nodes. So far, in the photon-counting regime, heralded entanglement between atomic ensembles has been successfully demonstrated through probabilistic protocols. But an inherent drawback of this approach is the compromise between the amount of entanglement and its preparation probability, leading to intrinsically low count rates for high entanglement. Here we report a protocol where entanglement between two atomic ensembles is created by coherent mapping of an entangled state of light. By splitting a single photon and performing subsequent state transfer, we separate the generation of entanglement and its storage. After a programmable delay, the stored entanglement is mapped back into photonic modes with overall efficiency of 17%. Together with improvements in single-photon sources, our protocol will allow 'on-demand' entanglement of atomic ensembles, a powerful resource for quantum information science.     

Resolving the time when an electron exits a tunnelling barrier

The tunnelling of a particle through a barrier is one of the most fundamental and ubiquitous quantum processes. When induced by an intense laser field, electron tunnelling from atoms and molecules initiates a broad range of phenomena such as the generation of attosecond pulses, laser-induced electron diffraction and holography. These processes evolve on the attosecond timescale (1?attosecond?≡?1?as = 10(-18)?seconds) and are well suited to the investigation of a general issue much debated since the early days of quantum mechanics--the link between the tunnelling of an electron through a barrier and its dynamics outside the barrier. Previous experiments have measured tunnelling rates with attosecond time resolution and tunnelling delay times. Here we study laser-induced tunnelling by using a weak probe field to steer the tunnelled electron in the lateral direction and then monitor the effect on the attosecond light bursts emitted when the liberated electron re-encounters the parent ion. We show that this approach allows us to measure the time at which the electron exits from the tunnelling barrier. We demonstrate the high sensitivity of the measurement by detecting subtle delays in ionization times from two orbitals of a carbon dioxide molecule. Measurement of the tunnelling process is essential for all attosecond experiments where strong-field ionization initiates ultrafast dynamics. Our approach provides a general tool for time-resolving multi-electron rearrangements in atoms and molecules--one of the key challenges in ultrafast science.     

Entanglement in a solid-state spin ensemble

Entanglement is the quintessential quantum phenomenon. It is a necessary ingredient in most emerging quantum technologies, including quantum repeaters, quantum information processing and the strongest forms of quantum cryptography. Spin ensembles, such as those used in liquid-state nuclear magnetic resonance, have been important for the development of quantum control methods. However, these demonstrations contain no entanglement and ultimately constitute classical simulations of quantum algorithms. Here we report the on-demand generation of entanglement between an ensemble of electron and nuclear spins in isotopically engineered, phosphorus-doped silicon. We combined high-field (3.4?T), low-temperature (2.9?K) electron spin resonance with hyperpolarization of the (31)P nuclear spin to obtain an initial state of sufficient purity to create a non-classical, inseparable state. The state was verified using density matrix tomography based on geometric phase gates, and had a fidelity of 98% relative to the ideal state at this field and temperature. The entanglement operation was performed simultaneously, with high fidelity, on 10(10) spin pairs; this fulfils one of the essential requirements for a silicon-based quantum information processor.