Visualizing dislocation nucleation by indenting colloidal crystals

The formation of dislocations is central to our understanding of yield, work hardening, fracture, and fatigue of crystalline materials. While dislocations have been studied extensively in conventional materials, recent results have shown that colloidal crystals offer a potential model system for visualizing their structure and dynamics directly in real space. Although thermal fluctuations are thought to play a critical role in the nucleation of these defects, it is difficult to observe them directly. Nano-indentation, during which a small tip deforms a crystalline film, is a common tool for introducing dislocations into a small volume that is initially defect-free. Here, we show that an analogue of nano-indentation performed on a colloidal crystal provides direct images of defect formation in real time and on the single particle level, allowing us to probe the effects of thermal fluctuations. We implement a new method to determine the strain tensor of a distorted crystal lattice and we measure the critical dislocation loop size and the rate of dislocation nucleation directly. Using continuum models, we elucidate the relation between thermal fluctuations and the applied strain that governs defect nucleation. Moreover, we estimate that although bond energies between particles are about fifty times larger in atomic systems, the difference in attempt frequencies makes the effects of thermal fluctuations remarkably similar, so that our results are also relevant for atomic crystals.     

Direct observation of the discrete character of intrinsic localized modes in an antiferromagnet

In a strongly nonlinear discrete system, the spatial size of an excitation can become comparable to, and influenced by, the lattice spacing. Such intrinsic localized modes (ILMs)--also called 'discrete breathers' or 'lattice solitons'--are responsible for energy localization in the dynamics of discrete nonlinear lattices. Their energy profiles resemble those of localized modes of defects in a harmonic lattice but, like solitons, they can move (although, unlike solitons, some energy is exchanged during collisions between them). The manipulation of these localized energy 'hotspots' has been achieved in systems as diverse as annular arrays of coupled Josephson junctions, optical waveguide arrays, two-dimensional nonlinear photonic crystals and micromechanical cantilever arrays. There is also some evidence for the existence of localized excitations in atomic lattices, although individual ILMs have yet to be identified. Here we report the observation of countable localized excitations in an antiferromagnetic spin lattice by means of a nonlinear spectroscopic technique. This detection capability permits the properties of individual ILMs to be probed; the disappearance of each ILM registers as a step in the time-dependent signal, with the surprising result that the energy staircase of ILM excitations is uniquely defined.     

光子晶体点缺陷在入射光激励下的响应特性研究

研究了光子晶体点缺陷在入射光激励下的响应特性,通过理论分析可以获得点缺陷的透射谱.分析发现,非线性点缺陷的缺陷模在入射光的激励下发生动态移动,且满足两个特征:首先,入射光功率强度越大,缺陷模移动幅度越大.其次,整个缺陷模的透射率随着功率强度的增大而降低.采用泵浦-探测技术的数值模拟方法可获得非线性点缺陷的动态特征.泵浦光和探测光可以选择不同频率以使缺陷模的特征比较清晰.所得现象与理论分析结果一致.该结论为该类光子晶体的应用提供理论依据.     

On-chip natural assembly of silicon photonic bandgap crystals.

Photonic bandgap crystals can reflect light for any direction of propagation in specific wavelength ranges. This property, which can be used to confine, manipulate and guide photons, should allow the creation of all-optical integrated circuits. To achieve this goal, conventional semiconductor nanofabrication techniques have been adapted to make photonic crystals. A potentially simpler and cheaper approach for creating three-dimensional periodic structures is the natural assembly of colloidal microspheres. However, this approach yields irregular, polycrystalline photonic crystals that are difficult to incorporate into a device. More importantly, it leads to many structural defects that can destroy the photonic bandgap. Here we show that by assembling a thin layer of colloidal spheres on a silicon substrate, we can obtain planar, single-crystalline silicon photonic crystals that have defect densities sufficiently low that the bandgap survives. As expected from theory, we observe unity reflectance in two crystalline directions of our photonic crystals around a wavelength of 1.3 micrometres. We also show that additional fabrication steps, intentional doping and patterning, can be performed, so demonstrating the potential for specific device applications.     

Ionic colloidal crystals of oppositely charged particles

Colloidal suspensions are widely used to study processes such as melting, freezing and glass transitions. This is because they display the same phase behaviour as atoms or molecules, with the nano- to micrometre size of the colloidal particles making it possible to observe them directly in real space. Another attractive feature is that different types of colloidal interactions, such as long-range repulsive, short-range attractive, hard-sphere-like and dipolar, can be realized and give rise to equilibrium phases. However, spherically symmetric, long-range attractions (that is, ionic interactions) have so far always resulted in irreversible colloidal aggregation. Here we show that the electrostatic interaction between oppositely charged particles can be tuned such that large ionic colloidal crystals form readily, with our theory and simulations confirming the stability of these structures. We find that in contrast to atomic systems, the stoichiometry of our colloidal crystals is not dictated by charge neutrality; this allows us to obtain a remarkable diversity of new binary structures. An external electric field melts the crystals, confirming that the constituent particles are indeed oppositely charged. Colloidal model systems can thus be used to study the phase behaviour of ionic species. We also expect that our approach to controlling opposite-charge interactions will facilitate the production of binary crystals of micrometre-sized particles, which could find use as advanced materials for photonic applications.     

Observation of two-dimensional discrete solitons in optically induced nonlinear photonic lattices

Nonlinear periodic lattices occur in a large variety of systems, such as biological molecules, nonlinear optical waveguides, solid-state systems and Bose-Einstein condensates. The underlying dynamics in these systems is dominated by the interplay between tunnelling between adjacent potential wells and nonlinearity. A balance between these two effects can result in a self-localized state: a lattice or 'discrete' soliton. Direct observation of lattice solitons has so far been limited to one-dimensional systems, namely in arrays of nonlinear optical waveguides. However, many fundamental features are expected to occur in higher dimensions, such as vortex lattice solitons, bright lattice solitons that carry angular momentum, and three-dimensional collisions between lattice solitons. Here, we report the experimental observation of two-dimensional (2D) lattice solitons. We use optical induction, the interference of two or more plane waves in a photosensitive material, to create a 2D photonic lattice in which the solitons form. Our results pave the way for the realization of a variety of nonlinear localization phenomena in photonic lattices and crystals. Finally, our observation directly relates to the proposed lattice solitons in Bose-Einstein condensates, which can be observed in optically induced periodic potentials.     

A colloidal model system with an interaction tunable from hard sphere to soft and dipolar

Monodisperse colloidal suspensions of micrometre-sized spheres are playing an increasingly important role as model systems to study, in real space, a variety of phenomena in condensed matter physics--such as glass transitions and crystal nucleation. But to date, no quantitative real-space studies have been performed on crystal melting, or have investigated systems with long-range repulsive potentials. Here we demonstrate a charge- and sterically stabilized colloidal suspension--poly(methyl methacrylate) spheres in a mixture of cycloheptyl (or cyclohexyl) bromide and decalin--where both the repulsive range and the anisotropy of the interparticle interaction potential can be controlled. This combination of two independent tuning parameters gives rise to a rich phase behaviour, with several unusual colloidal (liquid) crystalline phases, which we explore in real space by confocal microscopy. The softness of the interaction is tuned in this colloidal suspension by varying the solvent salt concentration; the anisotropic (dipolar) contribution to the interaction potential can be independently controlled with an external electric field ranging from a small perturbation to the point where it completely determines the phase behaviour. We also demonstrate that the electric field can be used as a pseudo-thermodynamic temperature switch to enable real-space studies of melting transitions. We expect studies of this colloidal model system to contribute to our understanding of, for example, electro- and magneto-rheological fluids.     

Colloidal ordering from phase separation in a liquid-crystalline continuous phase

Some binary mixtures exist as a single phase at high temperatures and as two phases at lower temperatures; rapid cooling therefore induces phase separation that proceeds through the initial formation of small particles and subsequent growth and coarsening. In solid and liquid media, this process leads to growing particles with a range of sizes, which eventually separate to form a macroscopically distinct phase. Such behaviour is of particular interest in systems composed of an isotropic fluid and a liquid crystal, where the random distribution of liquid-crystal droplets in an isotropic polymer matrix may give rise to interesting electro-optical properties. Here we report that a binary mixture consisting of an isotropic fluid and a liquid crystal forming the continuous phase does not fully separate into two phases, but self-organizes into highly ordered arrays of monodisperse colloidal droplet chains. We find that the size and spatial organization of the droplets are controlled by the orientational elasticity of the liquid-crystal phase and the defects caused by droplets exceeding a critical size. We expect that our approach to forming monodisperse, spatially ordered droplets in liquid crystals will allow the controlled design of ordered composites that may have useful rheological and optical properties.     

Structural diversity in binary nanoparticle superlattices

Assembly of small building blocks such as atoms, molecules and nanoparticles into macroscopic structures--that is, 'bottom up' assembly--is a theme that runs through chemistry, biology and material science. Bacteria, macromolecules and nanoparticles can self-assemble, generating ordered structures with a precision that challenges current lithographic techniques. The assembly of nanoparticles of two different materials into a binary nanoparticle superlattice (BNSL) can provide a general and inexpensive path to a large variety of materials (metamaterials) with precisely controlled chemical composition and tight placement of the components. Maximization of the nanoparticle packing density has been proposed as the driving force for BNSL formation, and only a few BNSL structures have been predicted to be thermodynamically stable. Recently, colloidal crystals with micrometre-scale lattice spacings have been grown from oppositely charged polymethyl methacrylate spheres. Here we demonstrate formation of more than 15 different BNSL structures, using combinations of semiconducting, metallic and magnetic nanoparticle building blocks. At least ten of these colloidal crystalline structures have not been reported previously. We demonstrate that electrical charges on sterically stabilized nanoparticles determine BNSL stoichiometry; additional contributions from entropic, van der Waals, steric and dipolar forces stabilize the variety of BNSL structures.     

Dimensional reduction at a quantum critical point

Competition between electronic ground states near a quantum critical point (QCP)--the location of a zero-temperature phase transition driven solely by quantum-mechanical fluctuations--is expected to lead to unconventional behaviour in low-dimensional systems. New electronic phases of matter have been predicted to occur in the vicinity of a QCP by two-dimensional theories, and explanations based on these ideas have been proposed for significant unsolved problems in condensed-matter physics, such as non-Fermi-liquid behaviour and high-temperature superconductivity. But the real materials to which these ideas have been applied are usually rendered three-dimensional by a finite electronic coupling between their component layers; a two-dimensional QCP has not been experimentally observed in any bulk three-dimensional system, and mechanisms for dimensional reduction have remained the subject of theoretical conjecture. Here we show evidence that the Bose-Einstein condensate of spin triplets in the three-dimensional Mott insulator BaCuSi2O6 (refs 12-16) provides an experimentally verifiable example of dimensional reduction at a QCP. The interplay of correlations on a geometrically frustrated lattice causes the individual two-dimensional layers of spin-(1/2) Cu2+ pairs (spin dimers) to become decoupled at the QCP, giving rise to a two-dimensional QCP characterized by linear power law scaling distinctly different from that of its three-dimensional counterpart. Thus the very notion of dimensionality can be said to acquire an 'emergent' nature: although the individual particles move on a three-dimensional lattice, their collective behaviour occurs in lower-dimensional space.     

Experimental measurement of the photonic properties of icosahedral quasicrystals

Quasicrystalline structures may have optical bandgap properties-frequency ranges in which the propagation of light is forbidden-that make them well-suited to the scientific and technological applications for which photonic crystals are normally considered. Such quasicrystals can be constructed from two or more types of dielectric material arranged in a quasiperiodic pattern whose rotational symmetry is forbidden for periodic crystals (such as five-fold symmetry in the plane and icosahedral symmetry in three dimensions). Because quasicrystals have higher point group symmetry than ordinary crystals, their gap centre frequencies are closer and the gaps widths are more uniform-optimal conditions for forming a complete bandgap that is more closely spherically symmetric. Although previous studies have focused on one-dimensional and two-dimensional quasicrystals, where exact (one-dimensional) or approximate (two-dimensional) band structures can be calculated numerically, analogous calculations for the three-dimensional case are computationally challenging and have not yet been performed. Here we circumvent the computational problem by doing an experiment. Using stereolithography, we construct a photonic quasicrystal with centimetre-scale cells and perform microwave transmission measurements. We show that three-dimensional icosahedral quasicrystals exhibit sizeable stop gaps and, despite their quasiperiodicity, yield uncomplicated spectra that allow us to experimentally determine the faces of their effective Brillouin zones. Our studies confirm that they are excellent candidates for photonic bandgap materials.     

Liquid crystal phase transitions in suspensions of polydisperse plate-like particles

Colloidal suspensions that form periodic self-assembling structures on sub-micrometre scales are of potential technological interest; for example, three-dimensional arrangements of spheres in colloidal crystals might serve as photonic materials, intended to manipulate light. Colloidal particles with non-spherical shapes (such as rods and plates) are of particular interest because of their ability to form liquid crystals. Nematic liquid crystals possess orientational order; smectic and columnar liquid crystals additionally exhibit positional order (in one or two dimensions respectively). However, such positional ordering may be inhibited in polydisperse colloidal suspensions. Here we describe a suspension of plate-like colloids that shows isotropic, nematic and columnar phases on increasing the particle concentration. We find that the columnar two-dimensional crystal persists for a polydispersity of up to 25%, with a cross-over to smectic-like ordering at very high particle concentrations. Our results imply that liquid crystalline order in synthetic mesoscopic materials may be easier to achieve than previously thought.     

金属玻璃的液态结构及其动力学胶体模拟

研究金属玻璃对于改善性能,开发新的合金体系有重要意义。由于实验手段的局限,目前为止还未能直接观测到液态结构的演化过程。胶体体系可以得到直观可视的粒子图像,已被应用于模拟研究原子体系的物理变化过程。通过不同的胶体体积浓度来模拟金属玻璃熔体,分析了不同胶体液态体系中的团簇结构,并对胶体粒子的扩散规律进行了探讨。结果表明液态体系的浓度越高,粒子的扩散速率越慢,局域特征结构发生变化,并在高浓度液态结构中观察到了结构的局域有序性动力学阻滞形成的笼子效应,为胶体体系液态微结构随浓度的演化提供了直接的实验证据。     

Bottom-up fabrication approaches to novel plasmonic materials

Recent research effort towards developing novel metal nanoparticles (NPs) and their ordered arrays have been motivated by the emergence of plasmonics. In particular, tuning the size, morphology, composition and the separation of metal NPs has allowed us to engineer the collective properties of plasmonic crystals for specific applications. Here we present our recent development of bottom-up growth methods and demonstrate convenience for the preparation of such plasmonic materials. By implementation of physical, chemical, or electrochemical deposition of a metal in combination with micromolding on two-dimensional colloidal crystals, metallic NPs with a variety of morphologies can be created in an ordered lattice. The prepared novel plasmonic crystals could find applications in optics, optoelectronics, materials science, sensing and biophysics.     

二维耦合干摩擦振子黏滑运动分析

针对工程中广泛存在的二维干摩擦问题,通过引入斜弹簧建立一种可考虑x,y两个方向耦合的振子模型。定义摩擦力方位角来描述动、静摩擦力矢量分量,并考虑振子振动过程中可能出现黏滞,提出了一种分析二维耦合干摩擦振子黏滑运动的方法,给出了二维耦合干摩擦振子黏滑运动的复杂边界条件。基于指数型动态摩擦模型对二维耦合干摩擦振子的黏滑运动进行了数值仿真,给出了x方向和y方向相同激振频率相同相位角、相同激振频率不同相位角、不同激振频率不同相位角3种工况下的仿真结果及系统解随激振频率和相位角的变化规律。仿真结果表明,二维耦合摩擦振子运动中可能出现黏滑状态转换;当x方向和y方向的激励频率和相位角均不相等时,与前两种工况相比,质量块的运动轨迹、系统相图均为更加复杂的平面曲线,同时一个周期内系统可出现多次黏滑转换;两个方向激振频率相同时,改变激振频率和激励相位角,系统的解均没有出现次谐波,振子为周期运动。所提出的方法可为进一步研究二维耦合干摩擦振子的动力学特性及运动稳定性提供参考。     

Two-substrate vertical deposition for stable colloidal crystal chips

By combining vertical deposition with micromolding in capillaries method, we have demonstrated the two-substrate vertical deposition, an alternative and versatile procedure for fabricating high-quality stable colloidal crystal chips. Apparent bright colors, special UV-vis spectra, scanning electron microscopy (SEM) and atomic force microscopy (AFM) images all prove that high-quality colloidal crystal structures are formed in between the two substrates.During the two-substrate vertical deposition for colloidal crystal chips, capillary force and evaporation of the medium are critical to the formation of the colloidal crystals; while the confinement in between two close substrates makes the resulting colloidal crystal chips more stable. Due to the excellent stability, these colloidal crystal chips can be used to construct some composite optical devices via a simpler and more flexible process. Meanwhile, they can also be further used as the templates for ordered multiporous materials.     

Chiral colloidal clusters

Chirality is an important element of biology, chemistry and physics. Once symmetry is broken and a handedness is established, biochemical pathways are set. In DNA, the double helix arises from the existence of two competing length scales, one set by the distance between monomers in the sugar backbone, and the other set by the stacking of the base pairs. Here we use a colloidal system to explore a simple forcing route to chiral structures. To do so we have designed magnetic colloids that, depending on both their shape and induced magnetization, self-assemble with controlled helicity. We model the two length scales with asymmetric colloidal dumbbells linked by a magnetic belt at their waist. In the presence of a magnetic field the belts assemble into a chain and the steric constraints imposed by the asymmetric spheres force the chain to coil. We show that if the size ratio between the spheres is large enough, a single helicity is adopted, right or left. The realization of chiral colloidal clusters opens up a new link between colloidal science and chemistry. These colloidal clusters may also find use as mesopolymers, as optical and light-activated structures, and as models for enantiomeric separation.     

Thermally fluctuating superconductors in two dimensions

In many two-dimensional superconducting systems, such as Josephson-junction arrays, granular superconducting films, and the high-temperature superconductors, it appears that the electrons bind into Cooper pairs below a pairing temperature (T(P)) that is well above the Kosterlitz-Thouless temperature (T(KT)) the temperature below which there is long-range superconducting order). The electron dynamics at temperatures between T(KT) and T(P) involve a complex interplay of thermal and quantum fluctuations, for which no quantitative theory exists. Here we report numerical results for this region, by exploiting its proximity to a T = 0 superconductor-insulator quantum phase transition. This quantum critical point need not be experimentally accessible for our results to apply. We characterize the static, thermodynamic properties by a single dimensionless parameter, gamma(T). Quantitative and universal results are obtained for the frequency dependence of the conductivity, which are dependent only upon gamma(T) and fundamental constants of nature.