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.     

Decoherence of quantum superpositions through coupling to engineered reservoirs

The theory of quantum mechanics applies to closed systems. In such ideal situations, a single atom can, for example, exist simultaneously in a superposition of two different spatial locations. In contrast, real systems always interact with their environment, with the consequence that macroscopic quantum superpositions (as illustrated by the 'Schrodinger's cat' thought-experiment) are not observed. Moreover, macroscopic superpositions decay so quickly that even the dynamics of decoherence cannot be observed. However, mesoscopic systems offer the possibility of observing the decoherence of such quantum superpositions. Here we present measurements of the decoherence of superposed motional states of a single trapped atom. Decoherence is induced by coupling the atom to engineered reservoirs, in which the coupling and state of the environment are controllable. We perform three experiments, finding that the decoherence rate scales with the square of a quantity describing the amplitude of the superposition state.     

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.     

有限格点一维分子晶体系统的极化子

本文从量子化的Holstein模型出发,将系统的基态试探波函数取作相干态,由能量极小原理,利用模拟退火法,计算系统的基态能量、晶格位移.     

Superconductivity in molecular crystals induced by charge injection

Progress in the field of superconductivity is often linked to the discovery of new classes of materials, with the layered copper oxides being a particularly impressive example. The superconductors known today include a wide spectrum of materials, ranging in complexity from simple elemental metals, to alloys and binary compounds of metals, to multi-component compounds of metals and chalcogens or metalloids, doped fullerenes and organic charge-transfer salts. Here we present a new class of superconductors: insulating organic molecular crystals that are made metallic through charge injection. The first examples are pentacene, tetracene and anthracene, the last having the highest transition temperature, at 4 K. We anticipate that many other organic molecular crystals can also be made superconducting by this method, which will lead to surprising findings in the vast composition space of molecular crystals.     

Kondo effect in quantum dots and molecular devices

Kondo effect is a very important many-body phenomenon in condensed mailer physics, which explains why the resistance increases as the temperature is lowered （usually 〈10 K） in dilute magnetic alloy, and why the conductance increases as temperature is decreased in quantum dots. This paper simply introduces equilihrium and nonequilibrium Kondo effects in quantum dots together with the Kondo effect in quantum dots with even number of electrons （when the singlet and triplet states are degenerate）. Furthermore, Kondn effect in single aton/molecular transistorss is introduced, which indicates a new way in study Kondo effect.     

单价离子晶体结合能的一种量子计算方法

将单价离子晶体的离子进行非谐振子处理，利用微扰理论求解微扰项对能级的修正值，与经典结果比较，这种量子方法计算出的单价离子晶体结合能更为精确．     

Modular and predictable assembly of porous organic molecular crystals

Nanoporous molecular frameworks are important in applications such as separation, storage and catalysis. Empirical rules exist for their assembly but it is still challenging to place and segregate functionality in three-dimensional porous solids in a predictable way. Indeed, recent studies of mixed crystalline frameworks suggest a preference for the statistical distribution of functionalities throughout the pores rather than, for example, the functional group localization found in the reactive sites of enzymes. This is a potential limitation for 'one-pot' chemical syntheses of porous frameworks from simple starting materials. An alternative strategy is to prepare porous solids from synthetically preorganized molecular pores. In principle, functional organic pore modules could be covalently prefabricated and then assembled to produce materials with specific properties. However, this vision of mix-and-match assembly is far from being realized, not least because of the challenge in reliably predicting three-dimensional structures for molecular crystals, which lack the strong directional bonding found in networks. Here we show that highly porous crystalline solids can be produced by mixing different organic cage modules that self-assemble by means of chiral recognition. The structures of the resulting materials can be predicted computationally, allowing in silico materials design strategies. The constituent pore modules are synthesized in high yields on gram scales in a one-step reaction. Assembly of the porous co-crystals is as simple as combining the modules in solution and removing the solvent. In some cases, the chiral recognition between modules can be exploited to produce porous organic nanoparticles. We show that the method is valid for four different cage modules and can in principle be generalized in a computationally predictable manner based on a lock-and-key assembly between modules.     

Controlling the dynamics of spontaneous emission from quantum dots by photonic crystals

Control of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals' lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.     

Rapid and reversible shape changes of molecular crystals on photoirradiation

The development of actuators based on materials that reversibly change shape and/or size in response to external stimuli has attracted interest for some time. A particularly intriguing possibility is offered by light-responsive materials, which allow remote operation without the need for direct contact to the actuator. The photo-response of these materials is based on the photoisomerization of constituent molecules (typically trans-cis isomerization of azobenzene chromophores), which gives rise to molecular motions and thereby deforms the bulk material. This effect has been used to create light-deformable polymer films and gels, but the response of these systems is relatively slow. Here we report that molecular crystals based on diarylethene chromophores and with sizes ranging from 10 to 100 micrometres exhibit rapid and reversible macroscopic changes in shape and size induced by ultraviolet and visible light. We find that on exposure to ultraviolet light, a single crystal of 1,2-bis(2-ethyl-5-phenyl-3-thienyl)perfluorocyclopentene changes from a square shape to a lozenge shape, whereas a rectangular single crystal of 1,2-bis(5-methyl-2-phenyl-4-thiazolyl)perfluorocyclopentene contracts by about 5-7 per cent. The deformed crystals are thermally stable, and switch back to their original state on irradiation with visible light. We find that our crystals respond in about 25 microseconds (that is, about five orders of magnitude faster than the response time of the azobenzene-based polymer systems) and that they can move microscopic objects, making them promising materials for possible light-driven actuator applications.     

大分子双缝衍射中的退相干现象

利用量子理论分析C60分子的双缝衍射实验数据,得到了C60分子的双缝衍射强度表达式,并利用退相干效应对衍射强度进行修正.所得结果与实验数据相符.     

内嵌富勒烯量子位的消相干研究

利用马尔可夫近似方法计算了X@C60（X=^14N,^15N,^31P）量子位中电子自旋在核子的精细作用和外磁场作用下的密度算符演化行为,得出量子位驰豫时间在10～100ns范围,与其它文献相符．     

原子运动对两原子纠缠消相干的影响

在两原子JC模型中引入了原子运动和场模结构参数,研究了原子运动对两原子系统共生纠缠度的影响,得出系统的消相干性质随原子质心运动参数变化的规律.结果表明,原子质心运动在系统内部会引起较为显著的纠缠消相干.然而,通过选择适当的系统参数,可以最大限度地抑制这种消相干效应.     

退相干和量子力学的诠释

近二十年来,针对量子力学围绕其概念基础产生的哲学争议,产生了不同于“哥本哈根诠释”和“正统”解释的可供选择的解诠方案。在解决测量问题上,退相干单独不能解决测量问题,但是退相干把环境相互作用包括进来不仅提出了新的观念问题,而且暗示了基本问题的解决方案。     

AIF分子外场效应的量子化学研究

选取密度泛函B3LYP方法和6—311＋＋g（d,P）基组对AlF分子在不同外电场（-0．015～0．015 a.u．）及没有外场下分子基态的稳定电子结构进行计算,研究了外电场对AlF分子基态总能量、键长、偶极矩、能隙、电荷分布及红外光谱等的影响．结果表明,随着Al→F方向外电场的增加,分子键长和偶极矩递减,原子电荷也递减,总能量升高,能隙增大,频率随Al→F方向外电场的增加而增加,其红外强度则递减;在外电场作用下,AlF基态分子势能曲线升高,离解能增大。     

Decoherence of matter waves by thermal emission of radiation

Emergent quantum technologies have led to increasing interest in decoherence--the processes that limit the appearance of quantum effects and turn them into classical phenomena. One important cause of decoherence is the interaction of a quantum system with its environment, which 'entangles' the two and distributes the quantum coherence over so many degrees of freedom as to render it unobservable. Decoherence theory has been complemented by experiments using matter waves coupled to external photons or molecules, and by investigations using coherent photon states, trapped ions and electron interferometers. Large molecules are particularly suitable for the investigation of the quantum-classical transition because they can store much energy in numerous internal degrees of freedom; the internal energy can be converted into thermal radiation and thus induce decoherence. Here we report matter wave interferometer experiments in which C70 molecules lose their quantum behaviour by thermal emission of radiation. We find good quantitative agreement between our experimental observations and microscopic decoherence theory. Decoherence by emission of thermal radiation is a general mechanism that should be relevant to all macroscopic bodies.     

相位阻尼对量子传输保真度的影响

研究了在相位阻尼作用下一个二能级原子与两个不同光场相互作用的系统中的量子态的保真度.讨论了相位阻尼和失谐对量子传输的最大保真度的影响,并且获得了通过该信道进行量子传输的最大保真度.此外,还分析了通过该信道进行量子传输的平均保真度.