Quantum computing in molecular magnets

Shor and Grover demonstrated that a quantum computer can outperform any classical computer in factoring numbers and in searching a database by exploiting the parallelism of quantum mechanics. Whereas Shor's algorithm requires both superposition and entanglement of a many-particle system, the superposition of single-particle quantum states is sufficient for Grover's algorithm. Recently, the latter has been successfully implemented using Rydberg atoms. Here we propose an implementation of Grover's algorithm that uses molecular magnets, which are solid-state systems with a large spin; their spin eigenstates make them natural candidates for single-particle systems. We show theoretically that molecular magnets can be used to build dense and efficient memory devices based on the Grover algorithm. In particular, one single crystal can serve as a storage unit of a dynamic random access memory device. Fast electron spin resonance pulses can be used to decode and read out stored numbers of up to 105, with access times as short as 10-10 seconds. We show that our proposal should be feasible using the molecular magnets Fe8 and Mn12.     

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.     

Macroscopic Quantum Phenomena and Topological Phase Interference Effects in Single-Domain Magnets

The tunneling of macroscopic object is one of the most fascinating phenomena in condensed matter physics. During the last decade, the problem of quantum tunneling of magnetization in nanometer-scale magnets has attracted a great deal of theoretical and experimental interest. A review of recent theoretical research of the macroscopic quantum phenomena in nanometer-scale single-domain magnets is presented in this paper. It includes macroscopic quantum tunneling (MQT) and coherence (MQC) in single-domain magnetic particles, the topological phase interference or spin-parity effects, and tunneling of magnetization in an arbitrarily directed magnetic field. The general formulas are shown to evaluate the tunneling rate and the tunneling level splitting for single-domain AFM particles. A nontrivial generalization of Kramers degeneracy for double-well system is provided to coherently spin tunneling for spin systems with m-fold rotational symmetry. The effects induced by the external magnetic field have been studied, where the field is along the easy, medium, hard axis, or arbitrary direction.     

Modulating the magnetic relaxation of lanthanide-based single-molecule magnets

In the area of molecular magnetism,single molecule magnets (SMMs) containing lanthanide elements are of immense scientific and technological interest because of their large energy barriers and high measured hysteresis temperature.Although there has been significant progress in the synthesis and characterization of lanthanide-based SMMs,there are still challenges,for instance,how single-ion anisotropy of lanthanide elements can be exploited,and how zero-field tunneling of magnetization can be suppressed.This article is devoted to the progress in various methodologies for modulating magnetic relaxation,especially in terms of crystal field and magnetic interactions.The crystal field plays a dominant role in creating single-molecule magnets with largely anisotropic f-elements,while the strong coupling between magnetic centers is able to suppress quantum tunneling of magnetization efficiently.     

GaN量子点弹性模量的分子动力学模拟

 应用一种分子动力学的方法,模拟预测了氮化镓（GaN）量子点在应变状态下的弹性模量和体积模量.通过在闪锌矿和纤维锌矿两类模型上施加不同形式的应变,得出了体应变和系统能量之间的关系.进一步利用分子动力学方法模拟出系统的能量,并计算出GaN材料在应变状态的弹性模量.在零应变状态下,预测结果同以往的理论值和实验值相吻合.     

（Nd，Dy）－（Fe，Co，Nb）－B稀土永磁体中的无沉淀区

研究了ＮｄＤｙＦｅＣｏＮｂＢ磁体平均晶粒尺寸与内禀矫顽力ｉＨｃ间的关系，发现随Ｎｂ含量增加，晶粒尺寸Ｄ减小，ｉＨｃ升高，但二者间不符合线性关系，尤其在低Ｎｂ含量范围，对显微组织的研究表明，加入Ｎｂ后，磁体显微组织除晶内出现沉淀和晶粒尺寸变化外，另一个显著特征是晶界附近无沉淀区的形成，讨论了其与矫顽力间的关系．     

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.     

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.     

具有分子双稳性的一维自由基磁相变材料的研究

具有分子双稳性的化合物是实现分子集合体作为新的光开关和信息存储元件的理想分子体系。本文合成苄基吡啶衍生物,研究其分子构象与堆积的关系,并研究了构建—维分子基磁体以及常温常压下的电学、磁学等性质。     

二茂铁及其衍生物的研究状况

二茂铁的发现对金属有机化学的迅速发展起着举足轻重的作用。笔者着重探讨了近十多年来，二茂铁及衍生物的研究状况，主要从分子铁磁体、分子电子器件、非线性光学材料、接臂型大环配合物等方面进行探讨。     

低碳经济下钕铁硼永磁体防护新技术

发展低碳经济是当今世界经济发展的潮流,是人类可持续发展的必然选择。针对NdFeB永磁体各种防护保护技术的特点,概述了钕铁硼永磁体表面防护处理常见方法———电镀,存在的环保和污染问题。论述了气相沉积技术原理、特点以及在钕铁硼永磁体表面防护处理上的应用。提出了气相沉积金属镀层需要解决的主要问题,而高效、清洁、环保的气相沉积技术是今后钕铁硼永磁体防护热点方向之一。     

单分子磁体与分子自旋电子材料

从单分子磁体合成、结构和性质及其在分子自旋晶体管、分子自旋电子管中的应用等方面,结合最新研究成果对这一有着应用前景的领域作了简要概述.单分子磁体是由内部的磁核和外围的有机分子壳层组成,可以通过修饰有机配体的基团和交换内部磁性离子等方法改善其物理和化学性能:带有烷基间隔基的[Co(Tpy-(CH2)5-SH)2]单核磁分子是一个弱偶合体系,而无烷基间隔基的[Co(TerPy)2]是强偶合,且Kondo温度异常地高(约25 K);将含两个磁中心的二核钒分子([(N,N',N"-trimethyl-1,4,7-triazacyclononane)2 V2(CN)4(μ-C4N4)])嫁接到电极表面出现有趣物理效应.上述就是在分子水平上研究电子自旋和电荷的分子自旋电子装置.     

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.     

量子围栏中金属表面态电子概率密度分布

量子围栏是以原子为材料在金属表面构成的闭合图案,由于电子具有波动性,因此,在量子围栏内可明显观察到二维电子概率驻波.文中以圆形和方形量子围栏为例,应用有限元数学方法,借助MATLAB数学软件,用计算机求解出被束缚在围栏中金属表面态电子相应于不同本征值的波函数及概率密度分布,与实验结果一致.该方法可方便求得处在任意形状势阱中的微观粒子波函数及概率密度分布情况,为定量研究电子被微观散射物散射产生的干涉现象提供新的手段.     

NdFeB系永磁体的矫顽力

根据TEM观察,建立了三元烧结NdFeB系永磁体的显微结构模型。运用微磁学理论对矫顽力模型作了计算,并讨论了Nd_2Fe_(14)B晶粒和NdFeB系永磁体的矫顽力。提出了烧结NdFeB系永磁体Nd_2Fe_(14)B晶粒的外延壳磁硬化理论和提高其矫顽力的途径。     

Nd-Fe-B磁体热等静压烧结的实验研究

研究了热等静压烧结对Nd-Fe-B磁体的致密度、显微组织及磁性能的影响.结果表明:与常压烧结磁体相比,热等静压烧结磁体的内部存在较多的孔洞,致密度、晶粒取向度及磁性都有所降低.用加热Ar气热膨胀而产生热等静压进行烧结的办法不适于制造高性能的烧结磁体.     

Quantum superposition of distinct macroscopic states

In 1935, Schrodinger attempted to demonstrate the limitations of quantum mechanics using a thought experiment in which a cat is put in a quantum superposition of alive and dead states. The idea remained an academic curiosity until the 1980s when it was proposed that, under suitable conditions, a macroscopic object with many microscopic degrees of freedom could behave quantum mechanically, provided that it was sufficiently decoupled from its environment. Although much progress has been made in demonstrating the macroscopic quantum behaviour of various systems such as superconductors, nanoscale magnets, laser-cooled trapped ions, photons in a microwave cavity and C60 molecules, there has been no experimental demonstration of a quantum superposition of truly macroscopically distinct states. Here we present experimental evidence that a superconducting quantum interference device (SQUID) can be put into a superposition of two magnetic-flux states: one corresponding to a few microamperes of current flowing clockwise, the other corresponding to the same amount of current flowing anticlockwise.     

氧对Sm(Co,Fe,Cu,Zr)z永磁体性能和显微组织的影响

研究了氧对Sm(Co, Fe, Cu, Zr)z永磁体性能的影响,并借助SEM、EDS和TEM等方法分析了永磁体的显微组织变化,讨论了影响磁体性能的原因.结果表明:在氧含量不高时(质量分数＜0.32%)对磁性能的影响不明显,永磁体具有良好的磁性能;在0.32%～0.4%时,随氧含量的增加磁性能开始下降;氧含量大于0.4%后,磁性能急剧恶化;当大于0.7%后,磁性能基本消失.随着氧含量的增加,磁体的晶粒尺寸减小,以Sm2O3为主的白色析出物增多.非磁性相的增多和有效Sm含量的减少是影响磁性能的主要原因.     

Quantum distribution of protons in solid molecular hydrogen at megabar pressures

Solid hydrogen, a simple system consisting only of protons and electrons, exhibits a variety of structural phase transitions at high pressures. Experimental studies based on static compression up to about 230 GPa revealed three relevant phases of solid molecular hydrogen: phase I (high-temperature, low-pressure phase), phase II (low-temperature phase) and phase III (high-pressure phase). Spectroscopic data suggest that symmetry breaking, possibly related to orientational ordering, accompanies the transition into phases II and III. The boundaries dividing the three phases exhibit a strong isotope effect, indicating that the quantum-mechanical properties of hydrogen nuclei are important. Here we report the quantum distributions of protons in the three phases of solid hydrogen, obtained by a first-principles path-integral molecular dynamics method. We show that quantum fluctuations of protons effectively hinder molecular rotation--that is, a quantum localization occurs. The obtained crystal structures have entirely different symmetries from those predicted by the conventional simulations which treat protons classically.     

单三重混合态的量子干涉效应

为了更深入地研究分子碰撞转动传能中干涉通道间量子干涉效应的本质,采用量子力学的一级波恩近似、各向异性相互作用势和直线轨迹近似,建立了单三重混合态Na2分子与Na(3s)的碰撞传能的干涉相位角的理论模型,得到了计算干涉相位角的方法.研究得到:影响干涉相位角的实验条件,干涉角和碰撞速度和碰撞参数的关系.此模型的建立有利于指导利用分子束进行此类实验,从而更清晰地理解量子干涉内部信息.