Single-spin addressing in an atomic Mott insulator

Ultracold atoms in optical lattices provide a versatile tool with which to investigate fundamental properties of quantum many-body systems. In particular, the high degree of control of experimental parameters has allowed the study of many interesting phenomena, such as quantum phase transitions and quantum spin dynamics. Here we demonstrate how such control can be implemented at the most fundamental level of a single spin at a specific site of an optical lattice. Using a tightly focused laser beam together with a microwave field, we were able to flip the spin of individual atoms in a Mott insulator with sub-diffraction-limited resolution, well below the lattice spacing. The Mott insulator provided us with a large two-dimensional array of perfectly arranged atoms, in which we created arbitrary spin patterns by sequentially addressing selected lattice sites after freezing out the atom distribution. We directly monitored the tunnelling quantum dynamics of single atoms in the lattice prepared along a single line, and observed that our addressing scheme leaves the atoms in the motional ground state. The results should enable studies of entropy transport and the quantum dynamics of spin impurities, the implementation of novel cooling schemes, and the engineering of quantum many-body phases and various quantum information processing applications.     

Observation of squeezed light from one atom excited with two photons

Single quantum emitters such as atoms are well known as non-classical light sources with reduced noise in the intensity, capable of producing photons one by one at given times. However, the light field emitted by a single atom can exhibit much richer dynamics. A prominent example is the predicted ability of a single atom to produce quadrature-squeezed light, which has fluctuations of amplitude or phase that are below the shot-noise level. However, such squeezing is much more difficult to observe than the emission of single photons. Squeezed beams have been generated using macroscopic and mesoscopic media down to a few tens of atoms, but despite experimental efforts, single-atom squeezing has so far escaped observation. Here we generate squeezed light with a single atom in a high-finesse optical resonator. The strong coupling of the atom to the cavity field induces a genuine quantum mechanical nonlinearity, which is several orders of magnitude larger than in typical macroscopic media. This produces observable quadrature squeezing, with an excitation beam containing on average only two photons per system lifetime. In sharp contrast to the emission of single photons, the squeezed light stems from the quantum coherence of photon pairs emitted from the system. The ability of a single atom to induce strong coherent interactions between propagating photons opens up new perspectives for photonic quantum logic with single emitters.     

激子极化激元光子学研究进展

研究光与物质相互作用是腔量子电动力学的一个重要方向.早在20世纪50年代,黄昆先生就提出了固体环境中的光子与晶格连续作用的时间演化图像,并指出光子-声子时间上连续不断的相互转化会在物质中形成声子极化激元波,从理论上计算了声子极化激元波的色散关系.Hopfield把这种图像推广到半导体环境中的光子-激子作用上.随后人们在微腔中实现了单原子、单量子点激子的真空拉比振荡.随着半导体微腔生长和微纳加工工艺的提高,激子极化激元的凝聚、超流、涡旋等宏观量子态被实验证明.通过控制微腔结构和光场调控的手段,人们进一步实现了对宏观量子态的相干调控.有机半导体、钙钛矿、二维半导体等新材料体系展现了极大的激子束缚能,有望实现室温量子器件的制备.微腔激子极化激元的研究进入了黄金时代.本文首先从激子极化激元的基本图像入手,详细介绍激子极化激元的概念、色散关系以及常见的激子极化激元体系.其次,总结了研究微腔激子极化激元的材料体系和实验方法,详细介绍了平板微腔和微纳材料自构型微腔的工作原理和具体实例,以及共焦显微荧光光谱和角分辨荧光光谱.第三,对激子极化激元的量子调控进行了总结.详细介绍了激子极化激元的重要宏观量子态以及通过微纳加工和光场调控的方式对宏观量子态的操控.具体分析了两个量子态操控的实例,包括氧化锌超晶格中多重量子态的制备以及凝聚体的参量散射过程.第四,对新型材料中激子极化激元的研究进行了总结,包括二维半导体、有机半导体和钙钛矿.最后,对本文进行总结,并且从理论、实验的角度分别预测了该领域的发展趋势.     

Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy

Molecular vibrations have oscillation periods that reflect the molecular structure, and are hence being used as a spectroscopic fingerprint for detection and identification. At present, all nonlinear spectroscopy schemes use two or more laser beams to measure such vibrations. The availability of ultrashort (femtosecond) optical pulses with durations shorter than typical molecular vibration periods has enabled the coherent excitation of molecular vibrations using a single pulse. Here we perform single-pulse vibrational spectroscopy on several molecules in the liquid phase, where both the excitation and the readout processes are performed by the same pulse. The main difficulty with single-pulse spectroscopy is that all vibrational levels with energies within the pulse bandwidth are excited. We achieve high spectral resolution, nearly two orders of magnitude better than the pulse bandwidth, by using quantum coherent control techniques. By appropriately modulating the spectral phase of the pulse we are able to exploit the quantum interference between multiple paths to selectively populate a given vibrational level, and to probe this population using the same pulse. This scheme, using a single broadband laser source, is particularly attractive for nonlinear microscopy applications, as we demonstrate by constructing a coherent anti-Stokes Raman (CARS) microscope operating with a single laser beam.     

树枝状CdS纳米结构的合成及光学性质

分别以丙烯基硫脲和五水氯化镉为硫源及镉源,利用水热法合成了树枝状CdS复杂纳米结构,利用X射线衍射谱、场发射扫描电子显微镜、透射电子显微镜、高分辨电子显微镜和电子衍射等对产物的形貌和结构进行表征.利用室温荧光光谱和紫外-可见光吸收谱对产物的光学性质进行研究.结果表明,所得产物是六方晶系的CdS,并且树枝状CdS是单晶.研究了不同硫源和镉源对产物形貌的影响,同时对树枝状CdS复杂纳米结构的形成机制进行了探讨.     

Real-time detection of electron tunnelling in a quantum dot

Nanostructures in which strong (Coulomb) interactions exist between electrons are predicted to exhibit temporal electronic correlations. Although there is ample experimental evidence that such correlations exist, electron dynamics in engineered nanostructures have been observed directly only on long timescales. The faster dynamics associated with electrical currents or charge fluctuations are usually inferred from direct (or quasi-direct) current measurements. Recently, interest in electron dynamics has risen, in part owing to the realization that additional information about electronic interactions can be found in the shot noise or higher statistical moments of a direct current. Furthermore, interest in quantum computation has stimulated investigation of quantum bit (qubit) readout techniques, which for many condensed-matter systems ultimately reduces to single-shot measurements of individual electronic charges. Here we report real-time observation of individual electron tunnelling events in a quantum dot using an integrated radio-frequency single-electron transistor. We use electron counting to measure directly the quantum dot's tunnelling rate and the occupational probabilities of its charge state. Our results provide evidence in favour of long (10 micros or more) inelastic scattering times in nearly isolated dots.     

Internal motions of a quasiparticle governing its ultrafast nonlinear response

A charged particle modifies the structure of the surrounding medium: examples include a proton in ice, an ion in a DNA molecule, an electron at an interface, or an electron in an organic or inorganic crystal. In turn, the medium acts back on the particle. In a polar or ionic solid, a free electron distorts the crystal lattice, displacing the atoms from their equilibrium positions. The electron, when considered together with its surrounding lattice distortion, is a single quasiparticle, known as the Fr?hlich polaron. The basic properties of polarons and their drift motion in a weak electric field are well known. However, their nonlinear high-field properties--relevant for transport on nanometre length and ultrashort timescales--are not understood. Here we show that a high electric field in the terahertz range drives the polaron in a GaAs crystal into a highly nonlinear regime where, in addition to the drift motion, the electron is impulsively moved away from the centre of the surrounding lattice distortion. In this way, coherent lattice vibrations (phonons) and concomitant drift velocity oscillations are induced that persist for several hundred femtoseconds. They modulate the optical response at infrared frequencies between absorption and stimulated emission. Such quantum coherent processes directly affect high-frequency transport in nanostructures and may be exploited in novel terahertz-driven optical modulators and switches.     

近场光学与近场光学显微镜

近场光学是研究距离物体表面一个波长以内的光学现象的新型交叉学科。基于非辐射场的探测与成像原理,近场光学显微镜突破常规光学显微镜所受到的衍射极限,在超高光学分辨率下进行纳米尺度光学成像与纳米尺度光谱研究。本文将讨论近场光学的基本原理,非辐射场的探测与高分辨率的关系;光学限阈及隐失场在近场光学中的重要性;以及近场信息的获取方法。对近场光学显微镜的主要类型及相应的仪器发展,分辨率,衬度原理做一综述。同时简要介绍近场光学显微镜在超高分辨率光学成像,近场局域光谱,高密度数据存储,在生命科学,单分子光谱,量子器件发光机制等领域中的应用。     

有机-无机复合钙钛矿单晶材料的研究进展

由于具有可调谐的光学带隙、较高的载流子迁移率、高外量子效率、较长的载流子寿命和载流子扩散长度等优点,新型有机-无机复合钙钛矿材料在太阳能电池、光电探测器、LED等光电领域展现出潜在的应用优势。自2009年第一块钙钛矿太阳能电池获得了3.8%的光电转换效率以来,钙钛矿材料成为世界范围内研究的热点。根据近年来钙钛矿材料的发展历程,概述了钙钛矿单晶材料从含Pb到无Pb(包含Sn-基、Ge-基无铅钙钛矿材料、类钙钛矿材料以及双钙钛矿材料)的发展历程和主要应用领域。     

影响电镜分辨本领的热因素探讨

简述了光学显微镜与电子显微镜的分辨本领 .给出了在考虑相对论效应的情况下高速电子束的波长与加速电压的关系 ,着重论述了由于电子热运动引起的电子波的色散 ,并研究了该色散对电镜分辨本领的影响 .得出了电子热运动引起的色差比加速电压不稳造成的色差还大的主要结论 .     

Experimental observation of the quantum Hall effect and Berry's phase in graphene

When electrons are confined in two-dimensional materials, quantum-mechanically enhanced transport phenomena such as the quantum Hall effect can be observed. Graphene, consisting of an isolated single atomic layer of graphite, is an ideal realization of such a two-dimensional system. However, its behaviour is expected to differ markedly from the well-studied case of quantum wells in conventional semiconductor interfaces. This difference arises from the unique electronic properties of graphene, which exhibits electron-hole degeneracy and vanishing carrier mass near the point of charge neutrality. Indeed, a distinctive half-integer quantum Hall effect has been predicted theoretically, as has the existence of a non-zero Berry's phase (a geometric quantum phase) of the electron wavefunction--a consequence of the exceptional topology of the graphene band structure. Recent advances in micromechanical extraction and fabrication techniques for graphite structures now permit such exotic two-dimensional electron systems to be probed experimentally. Here we report an experimental investigation of magneto-transport in a high-mobility single layer of graphene. Adjusting the chemical potential with the use of the electric field effect, we observe an unusual half-integer quantum Hall effect for both electron and hole carriers in graphene. The relevance of Berry's phase to these experiments is confirmed by magneto-oscillations. In addition to their purely scientific interest, these unusual quantum transport phenomena may lead to new applications in carbon-based electronic and magneto-electronic devices.     

Field-driven photoemission from nanostructures quenches the quiver motion

Strong-field physics, an extreme limit of light-matter interaction, is expanding into the realm of surfaces and nanostructures from its origin in atomic and molecular science. The attraction of nanostructures lies in two intimately connected features: local intensity enhancement and sub-wavelength confinement of optical fields. Local intensity enhancement facilitates access to the strong-field regime and has already sparked various applications, whereas spatial localization has the potential to generate strong-field dynamics exclusive to nanostructures. However, the observation of features unattainable in gaseous media is challenged by many-body effects and material damage, which arise under intense illumination of dense systems. Here, we non-destructively access this regime in the solid state by employing single plasmonic nanotips and few-cycle mid-infrared pulses, making use of the wavelength-dependence of the interaction, that is, the ponderomotive energy. We investigate strong-field photoelectron emission and acceleration from single nanostructures over a broad spectral range, and find kinetic energies of hundreds of electronvolts. We observe the transition to a new regime in strong-field dynamics, in which the electrons escape the nanolocalized field within a fraction of an optical half-cycle. The transition into this regime, characterized by a spatial adiabaticity parameter, would require relativistic electrons in the absence of nanostructures. These results establish new degrees of freedom for the manipulation and control of electron dynamics on femtosecond and attosecond timescales, combining optical near-fields and nanoscopic sources.     

Sub-ångstrom resolution using aberration corrected electron optics

Following the invention of electron optics during the 1930s, lens aberrations have limited the achievable spatial resolution to about 50 times the wavelength of the imaging electrons. This situation is similar to that faced by Leeuwenhoek in the seventeenth century, whose work to improve the quality of glass lenses led directly to his discovery of the ubiquitous "animalcules" in canal water, the first hints of the cellular basis of life. The electron optical aberration problem was well understood from the start, but more than 60 years elapsed before a practical correction scheme for electron microscopy was demonstrated, and even then the remaining chromatic aberrations still limited the resolution. We report here the implementation of a computer-controlled aberration correction system in a scanning transmission electron microscope, which is less sensitive to chromatic aberration. Using this approach, we achieve an electron probe smaller than 1 A. This performance, about 20 times the electron wavelength at 120 keV energy, allows dynamic imaging of single atoms, clusters of a few atoms, and single atomic layer 'rafts' of atoms coexisting with Au islands on a carbon substrate. This technique should also allow atomic column imaging of semiconductors, for detection of single dopant atoms, using an electron beam with energy below the damage threshold for silicon.     

Element-selective imaging of atomic columns in a crystal using STEM and EELS

Microstructure characterization has become indispensable to the study of complex materials, such as strongly correlated oxides, and can obtain useful information about the origin of their physical properties. Although atomically resolved measurements have long been possible, an important goal in microstructure characterization is to achieve element-selective imaging at atomic resolution. A combination of scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS) is a promising technique for atomic-column analysis. However, two-dimensional analysis has not yet been performed owing to several difficulties, such as delocalization in inelastic scattering or instrumentation instabilities. Here we demonstrate atomic-column imaging of a crystal specimen using localized inelastic scattering and a stabilized scanning transmission electron microscope. The atomic columns of La, Mn and O in the layered manganite La1.2Sr1.8Mn2O7 are visualized as two-dimensional images.     

掺杂效应对氧化锡纳米晶微结构、形貌及其光学性能的影响

以二价SnCl2无机盐为原料，基于配合物前躯体方法制备了氧化锡及铜离子掺杂氧化锡纳米晶．根据DSC和TG分析结果在550℃对前驱体进行煅烧．运用FTIR、UV-VIS、XRD和TEM／HRTEM等测试手段对两纳米晶材料进行了分析表征．掺杂后掺杂相氧化物分散驻留在SnO2晶粒表面，阻止了SnO2晶粒表面的扩散，从而抑制其晶粒生长．此外，铜离子掺杂使得表面缺陷附近的自由电子能有效的定域化，从而使SnO2纳米晶体系的直接和间接带隙能均向高能方向移动．试验证明以无机盐代替金属醇盐为原料是切实可行的，且配合物前躯体法简单易操作，将有利于产业化．     

Reducing Zn diffusion in single axial junction InP nanowire solar cells for improved performance

In this work axial n-i-p junction InP nanowires were grown by selective-area metal organic vapor phase epitaxy (SA-MOVPE) technique with the growth sequence starting from n-segment. The optical properties and carrier lifetimes of the n-, i- and p-type segments were studied and compared using time-resolved photoluminescence (PL) and cathodoluminescence (CL) measurements. We demonstrate for the first time that CL is capable of resolving the electrical profile of the nanowires, namely the varied lengths of the n-, i- and p-segments, providing a simple and effective approach for nanowire growth calibration and optimization. The CL result was further confirmed by electron beam induced current (EBIC) and photocurrent mapping measurements performed from the fabricated single nanowire solar cell devices. It is revealed that despite a non-optimized device structure (very long n-region and short i-region), the n-i-p nanowire solar cells show improved power conversion efficiency (PCE) than the previously reported p-i-n (growth starts with p-segment) single nanowire solar cells due to reduced p-type dopant (Zn) diffusion during the growth of n-i-p solar cell structure.     

Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb

The control of the broadband frequency comb emitted from a mode-locked femtosecond laser has permitted a wide range of scientific and technological advances--ranging from the counting of optical cycles for next-generation atomic clocks to measurements of phase-sensitive high-field processes. A unique advantage of the stabilized frequency comb is that it provides, in a single laser beam, about a million optical modes with very narrow linewidths and absolute frequency positions known to better than one part in 10(15) (ref. 5). One important application of this vast array of highly coherent optical fields is precision spectroscopy, in which a large number of modes can be used to map internal atomic energy structure and dynamics. However, an efficient means of simultaneously identifying, addressing and measuring the amplitude or relative phase of individual modes has not existed. Here we use a high-resolution disperser to separate the individual modes of a stabilized frequency comb into a two-dimensional array in the image plane of the spectrometer. We illustrate the power of this technique for high-resolution spectral fingerprinting of molecular iodine vapour, acquiring in a few milliseconds absorption images covering over 6 THz of bandwidth with high frequency resolution. Our technique for direct and parallel accessing of stabilized frequency comb modes could find application in high-bandwidth spread-spectrum communications with increased security, high-resolution coherent quantum control, and arbitrary optical waveform synthesis with control at the optical radian level.     

Coherent branched flow in a two-dimensional electron gas

Semiconductor nanostructures based on two-dimensional electron gases (2DEGs) could form the basis of future devices for sensing, information processing and quantum computation. Although electron transport in 2DEG nanostructures has been well studied, and many remarkable phenomena have already been discovered (for example, weak localization, quantum chaos, universal conductance fluctuations), fundamental aspects of the electron flow through these structures have so far not been clarified. However, it has recently become possible to image current directly through 2DEG devices using scanning probe microscope techniques. Here, we use such a technique to observe electron flow through a narrow constriction in a 2DEG-a quantum point contact. The images show that the electron flow from the point contact forms narrow, branching strands instead of smoothly spreading fans. Our theoretical study of this flow indicates that this branching of current flux is due to focusing of the electron paths by ripples in the background potential. The strands are decorated by interference fringes separated by half the Fermi wavelength, indicating the persistence of quantum mechanical phase coherence in the electron flow. These findings may have important implications for a better understanding of electron transport in 2DEGs and for the design of future nanostructure devices.     

Adaptive subwavelength control of nano-optical fields

Adaptive shaping of the phase and amplitude of femtosecond laser pulses has been developed into an efficient tool for the directed manipulation of interference phenomena, thus providing coherent control over various quantum-mechanical systems. Temporal resolution in the femtosecond or even attosecond range has been demonstrated, but spatial resolution is limited by diffraction to approximately half the wavelength of the light field (that is, several hundred nanometres). Theory has indicated that the spatial limitation to coherent control can be overcome with the illumination of nanostructures: the spatial near-field distribution was shown to depend on the linear chirp of an irradiating laser pulse. An extension of this idea to adaptive control, combining multiparameter pulse shaping with a learning algorithm, demonstrated the generation of user-specified optical near-field distributions in an optimal and flexible fashion. Shaping of the polarization of the laser pulse provides a particularly efficient and versatile nano-optical manipulation method. Here we demonstrate the feasibility of this concept experimentally, by tailoring the optical near field in the vicinity of silver nanostructures through adaptive polarization shaping of femtosecond laser pulses and then probing the lateral field distribution by two-photon photoemission electron microscopy. In this combination of adaptive control and nano-optics, we achieve subwavelength dynamic localization of electromagnetic intensity on the nanometre scale and thus overcome the spatial restrictions of conventional optics. This experimental realization of theoretical suggestions opens a number of perspectives in coherent control, nano-optics, nonlinear spectroscopy, and other research fields in which optical investigations are carried out with spatial or temporal resolution.     

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.