Completely Subradiant Multi‐Atom Architectures Through 2D Photonic Crystals

Following recent advances in the manipulation of atoms trapped near 1D waveguides and proposals to use surface acoustic waves on piezoelectric substrates for the same purpose, the potential of two‐dimensional platforms is shown. Directional emission of atoms near photonic crystal slabs with square symmetry is used, in the ideal case, to build perfect subradiant states of 2 distant atoms, possible in 2D only for finite lattices with perfectly reflecting boundaries. These allow the design of massively parallel 1D arrays of atoms above a single crystal, useful for multi‐port output of nonclassical light, by exploiting destructive interference of guided resonance modes. Directionality of the emission is shown to be present whenever a linear iso‐frequency manifold is present in the dispersion relation of the crystal. Multi‐atom radiance properties can be predicted from a simple cross‐talk coefficient of a master equation, in good agreement with exact atom‐crystal dynamics, showing its predictive power. Departing from the ideal theoretical case, possible experimental issues in photonic crystal implementations are also discussed, and an outlook of other relevant modern platforms for 2D propagation of excitations is given.     

Amplification of Solar Energy Conversion in Quantum‐Confined CdSe‐Sensitized TiO2 Photonic Crystals by Trapping Light

Photonic effects amplifying solar energy conversion are reported in titania inverse opals sensitized with quantum‐confined CdSe films. TiO₂ inverse opals (i‐TiO₂‐o) and unstructured nanocrystalline TiO₂ (nc‐TiO₂) films are sensitized with CdSe deposited via successive ionic layer adsorption and reaction (SILAR) by generating Se^2? in situ under inert atmosphere, and the film absorbance is tuned by the number of SILAR cycles. Photonic effects are investigated while varying the i‐TiO₂‐o stop band position relative to CdSe films’ absorbance. i‐TiO₂‐o films with stop band at 700 and 560 nm are sensitized with CdSe having absorption edges at 600 and 650 nm thus tuning absorbance to the red and the blue of the stop band. Significant amplification in photon‐to‐current conversion efficiency is measured when CdSe films prepared via two cycles are adsorbed on i‐TiO₂‐o with a stop band at 700 nm, with a maximum average enhancement factor equal to 6.7 ± 1.6 at 640 nm, 60 nm to the blue of the stop band center, relative to nc‐TiO₂ sensitized with comparable CdSe amounts. The gain is observed over a wide frequency range to the blue of the stop band and is greatest when film absorbance was low. The photocurrent gain is not a result of differences in the rates of charge separation or charge transport, and occurs in the same frequency range where absorbance amplification is measured to the blue of the 700‐i‐TiO₂‐o stop band, and is thus attributed to slow light effects enhancing absorbance in the photonic crystal environment.     

用时域有限差分方法研究非惯性坐标系下光子晶体传输特性

将时域有限差分（FDTD）方法用于非惯性坐标系下光子晶体理论研究,给出了非惯性坐标系下的差分方程和理想匹配层（PML）边界条件。设计了一个包含闭合环行腔和定向耦合器的光子晶体结构。定向耦合器的耦合长度为43a,这样的耦合长度既保证了闭合环行腔的高Q值,又保证了必要的频率分辨力。理论计算表明：光子晶体转动时,闭合环行腔里顺时针与逆时针方向传播的光有频差产生,此频差大小与光子晶体的转动角速度有关。     

Comb of high‐Q Resonances in a Compact Photonic Cavity

The optical equivalent of the quantum mechanical oscillator is demonstrated in a photonic crystal cavity, owing to the balance of the background dispersion and a bichromatic potential. Consequently, several equi‐spaced resonances with large loaded Q factors are obtained within a very tiny volume. A detailed statistical analysis is carried out by exploiting the complex reflection spectra measured with Optical Coherent Tomography. The log‐normal distribution of the intrinsic Q‐factors is centered at 0.7 million. The device is made of Ga_0.5In_0.5P in order to suppress the two photon absorption in the Telecom spectral range considered here. This is crucial to turn the strong localization of light into ultra‐efficient parametric interactions.     

Self‐Assembled Fluorescent and Antibacterial GHK‐Cu Nanoparticles for Wound Healing Applications

GHK‐Cu is demonstrated with the abilities to improve wound healing, accelerate anti‐inflammatory activity, and repair DNA damage. However, the instability of the GHK‐Cu in biological fluids is always a big challenge for its long‐term and efficient function at the target site. Therefore, the self‐assembled GHK‐Cu nanoparticles (GHK‐Cu NPs) are investigated in this work to solve the instability issue. The crystalline nanostructure within the GHK‐Cu nanoparticles offers them visible and near‐infrared fluorescent properties. With the excellent self‐assembly performance, the antibacterial properties of GHK‐Cu NPs are demonstrated using E. coli and S. aureus. The L929 dermal fibroblast cells are utilized to prove the good biocompatibility and enhanced wound healing applications of GHK‐Cu NPs. This study could pave the way for the design and elaboration of a new class of fluorescent peptides with various biological functions in biomedical applications.     

DNA‐Mediated Stabilization of Self‐Assembling Bead Monolayers for Microfluidic Applications

Forming ordered 2D or 3D arrays of colloidal particles on the micro‐ or nanometer scale in a bottom‐up process is a challenging task. In previous works by various groups, hybridization between DNA strands localized on the particle surface is used to create crystalline arrays. However, this method requires an annealing process with a duration of one day or more and usually yields agglomerates of only a few dozen particles. In this work, a method for the rapid formation of highly‐ordered 2D agglomerates of superparamagnetic microparticles (beads) is presented. Dipolar coupling between the beads under the influence of a rotating magnetic field leads to the formation of a dense monolayer. The monolayer is then stabilized through DNA hybridization between DNA strands immobilized on the bead surface and a linker strand in solution. The whole self‐assembly process requires less than an hour and is therefore significantly faster than comparable methods.     

温度、密度对磁化等离子体光子晶体缺陷模的影响

采用等温近似,用磁化等离子体的分段线形电流密度卷积(Piecewise Linear Current Density Recursive Convolution,PLCDRC)时域有限差分(Finite-differentce Time-domain,FDTD)算法研究了具有单一缺陷层的一维磁化等离子体光子晶体的缺陷模特性;以高斯脉冲为激励源,用算法公式计算所得的电磁波透射系数,讨论了温度和等离子体层密度对其缺陷模的影响。结果表明:改变温度和等离子体层密度可以获得不同的缺陷模。     

Colloidal Crystals of NaYF4 Upconversion Nanocrystals Studied by Small‐Angle X‐Ray Scattering (SAXS)

Spherical NaYF₄ upconversion nanocrystals with mean radii of about 5 and 11 nm are observed to form colloidal crystals, i.e., 3D assemblies of the particles with long‐range order. The colloidal crystals of the larger particles form directly in solution when dispersions of the particles in toluene are stored at room temperature for several weeks. Crystallization of the smaller particles takes place when their dispersions in hexane are slowly dried at elevated temperatures. The formation and the structure of the colloidal crystals are studied by small‐angle X‐ray scattering (SAXS). SAXS measurements show that the smaller as well as the larger particles assemble into a face‐centered cubic lattice with unit cell dimensions of a = 18.7 nm and a = 35.5 nm, respectively. The SAXS data also show that the particles in the colloidal crystals still bear a layer of oleic acid on their surfaces. The thickness of this layer is 1.5–1.8 nm, as determined by comparing the unit cell dimensions of the colloidal crystals with the mean particle sizes. The latter could be very precisely determined from the distinct oscillations observed in the SAXS data of dilute colloidal dispersions of the nanocrystals.     

Self‐organized colloidal crystals for photonics and laser applications

We present an overview of recent developments in the fabrication and uses of colloidal crystals (CCs) for photonics and laser applications. Microparticles with a diameter in the range from 10 nm to 10 μm often have an intrinsic capability to spontaneously organize themselves from a colloidal suspension into 3D lattice structures. Such highly ordered 3D architectures of microparticles are called colloidal crystals (CCs). The CC structures have received tremendous attention as one of the facile and high‐throughput fabrication techniques of photonic crystals (PCs). We introduce here interesting precedents not only of diverse techniques of high‐quality CC structures, but also of their versatile applications in optical sensors responding to various external stimuli. This review also highlights a new potential use of the CCs as low‐threshold laser devices. We believe that a wide variety of CC architectures will play leading roles in the next generation of optoelectronic devices.     

Liquid‐Crystal‐Mediated Self‐Assembly of Porous α‐Fe2O3 Nanorods on PEDOT:PSS‐Functionalized Graphene as a Flexible Ternary Architecture for Capacitive Energy Storage

A novel aqueous‐based self‐assembly approach to a composite of iron oxide nanorods on conductive‐polymer (CP)‐functionalized, ultralarge graphene oxide (GO) liquid crystals (LCs) is demonstrated here for the fabrication of a flexible hybrid material for charge capacitive application. Uniform decoration of α‐Fe₂O₃ nanorods on a poly(3,4‐ethylene‐dioxythiophene): poly(styrenesulfonate) (PEDOT:PSS)‐functionalized, ultralarge GO scaffold results in a 3D interconnected layer‐by‐layer (LBL) architecture. This advanced interpenetrating network of ternary components is lightweight, foldable, and possesses highly conductive pathways for facile ion transportation and charge storage, making it promising for high‐performance energy‐storage applications. Having such structural merits and good synergistic effects, the flexible architecture exhibits a high specific discharge capacitance of 875 F g^?1 and excellent volumetric specific capacitance of 868 F cm^?3 at 5 mV s^?1, as well as a promising energy density of 118 W h kg^?1 (at 0.5 A g^?1) and promising cyclability, with capacity retention of 100% after 5000 charge–discharge (CD) cycles. This synthesis method provides a simple, yet efficient approach for the solution‐processed LBL insertion of the hematite nanorods (HNR) into CP‐functionalized novel composite structure. It provides great promise for the fabrication of a variety of metal‐oxide (MO)‐nanomaterial‐based binder and current collector‐free flexible composite electrodes for high‐performance energy‐storage applications.     

Phase‐matching properties of BaGa4S7 and BaGa4Se7: Wide‐bandgap nonlinear crystals for the mid‐infrared

Biaxial BaGa₄S₇ and BaGa₄Se₇ crystals transparent in the mid‐IR have been grown by the Bridgman–Stockbarger technique in sufficiently large sizes and with good optical quality to measure the refractive indices and analyze phase‐matching properties. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

圆柱形散射子二维光子晶体的态密度与局域态密度

二维光子晶体只有赝带隙,因此能否利用二维光子晶体有效控制原子自发辐射是令人感兴趣也是有实际意义的问题。其中最重要的因素是态密度和局域态密度的性质。采用平面波展开结合晶体群论的方法计算了二维正方格子光子晶体的态密度和局域态密度。其中散射子为空气圆柱,放置在均匀的电介质背景上。结果显示两个特点:第一,总态密度和局域态密度在原来二维光子晶体赝带隙处虽然已经不为零,但是取值明显低于赝带隙范围之外的值,即存在一个准光子带隙。第二,局域态密度在空气散射子界面处发生突变,空气散射子区域的局域态密度相对较大,这可由电位移矢量的连续性来理解。由于这两个特点在其他二维光子晶体中也被发现过,它们可能是普遍存在的。     

Self‐Organization of Anisotropic and Binary Colloids in Thermo‐Switchable 1D Microconfinement

Anisotropic and binary colloids self‐assemble into a variety of novel supracolloidal structures within the thermo‐switchable confinement of molecular microtubes, achieving structuring at multiple length scales and dimensionalities. The multistage self‐assembly strategy involving hard colloidal particles and a soft supramolecular template is generic for colloids with different geometries and materials as well as their binary mixtures. The colloidal architectures can be controlled by colloid shape, size, and concentration. Colloidal cubes align in chains with face‐to‐face arrangement, whereas rod‐like colloids predominantly self‐organize in end‐to‐end configurations with their long axis parallel with the long axis of the microtubes. The 1D microconfinement imposed on binary mixtures of anisotropic and isotropic colloids further increases the diversity of colloid‐in‐tube structures. In cube–sphere mixtures, cubes may act as additional confiners, locking in colloidal sphere chains, while a “colloidal Morse code” is generated where rods and spheres alternate in the case of rod–sphere mixtures. The versatile confined colloidal superstructures including their thermoresponsive assembly and disassembly are relevant for the development of stimulus–responsive materials where controlled release and encapsulation are desired.     

Angular‐ and polarization‐independent structural colors based on 1D photonic crystals

Wide‐angle, polarization‐independent structural reflective colors from both directions based on a one‐dimensional photonic crystal are demonstrated. Our device produces a distinct and saturated color with high angular tolerant performance up to ±70° for any polarization state of an incident light wave, which is highly desirable for a broad range of research areas. Moreover, the purity of the color and luminous intensity of the proposed device are improved as compared to conventional colorant‐based color filters and colloidal glasses. The present approach may have the potential to replace existing color filters and pigments and pave the way for various applications, including color displays and image sensor technologies.

     

A Photonic Nanojet as Tunable and Polarization‐Sensitive Optical Tweezers

The ability to manipulate small objects with focused laser beams has opened a venue for investigating dynamical phenomena relevant to both fundamental and applied sciences. However, manipulating nano‐sized objects requires subwavelength field localization, provided by auxiliary nano‐ and microstructures. Particularly, dielectric microparticles can be used to confine light to an intense beam with a subwavelength waist, called a photonic nanojet (PNJ), which can provide sufficient field gradients for trapping nano‐objects. Herein, the scheme for wavelength‐tunable and nanoscale‐precise optical trapping is elaborated, and the possibility of lateral nanoparticle movement using the PNJ's side lobes is shown for the first time. In addition, the possibility of subwavelength positioning using polarization switching is shown. The estimated stability with respect to Brownian motion is higher compared to conventional optical trapping schemes.     

Self‐association in {2‐[3,4‐alkylenedioxy‐5‐(3‐pyridyl)]‐thienyl}alkanols: an NMR,IR, and single‐crystal X‐ray study

syn‐2,2,4,4‐Tetramethyl‐3‐{2‐[3,4‐alkylenedioxy‐5‐(3‐pyridyl)]thienyl}pentan‐3‐ols self‐associate both in the solid state and in solution. Single‐crystal X‐ray diffraction study of the 3,4‐ethylenedioxythiophene (EDOT) derivative shows that it exists as a centrosymmetric head‐to‐tail, syn dimer in the solid state. The IR spectra of the solids display only a broad OH absorption around 3300 cm^?1, corresponding to a hydrogen‐bonded species. ¹H Nuclear Overhauser Effect Spectroscopy (NOESY) NMR experiments in benzene reveal interactions between the tert‐butyl groups and the H2 and H6 protons of the pyridyl group. Two approaches have been used to determine association constants of the EDOT derivative by NMR titration, based on the concentration dependence of (i) the syn/anti ratio and (ii) the OH proton shift of the syn rotamer. Reasonably concordant results are obtained from 298 to 323 K (3.6 and 3.9 M^?1, respectively, at 298 K). Similar values are obtained from the syn OH proton shift variation for the 3,4‐methylenedioxythiophene (MDOT) derivative. Concentration‐dependent variation of the anti OH proton shift in the latter suggests that the anti isomer associates in the form of an open, singly hydrogen‐bonded dimer, with a much smaller association constant than the syn rotamer. Self‐association constants for 3‐pyridyl‐EDOT‐alkanols with smaller substituents vary by a factor of 4 from (i‐Pr)₂ up to (CD₃)₂, while the hetero‐association constants for the same compounds with pyridine vary slightly less. Copyright © 2007 John Wiley & Sons, Ltd.     

Zinc Oxide–Porphyrin Hybrid Rhombuses: Catalytically Active Microstructures via Self‐Assembly

A novel self‐assembled organic–inorganic hybrid structure consisting of zinc oxide and two oppositely charged porphyrins, showing significantly enhanced photocatalytic activity, is presented. Electrostatic self‐assembly of the cationic tetra‐(N‐methyl‐4‐pyridyl)porphyrin (TMPyP) with preformed assemblies of ZnO nanorods and the anionic tetra‐(4‐sulfonatophenyl)porphyrin (TPPS) in ethanol results in porphyrin microrhombuses decorated with ZnO nanorods. The structure formation is followed spectroscopically. The shape of the microrhombuses and the number of attached ZnO nanoparticles can be tuned through the porphyrin ratio TMPyP/TPPS. An enhanced and selective catalytic activity is found, giving insight into the degradation mechanism. Due to the tool‐box principle and its versatility, the concept may have great impact in fields such as solar‐energy conversion and optoelectronics.     

Self‐doping PPV oligomers – electrochemistry and structure of the self‐doped systems

A novel class of self‐doping conjugated oligomers, E,E‐2‐(sulfoalkoxy)‐5‐alkoxy‐1,4‐bis[2‐(2,4,6‐trimethoxyphenyl) ethenyl]benzenes, is presented. The synthesis and spectroscopic characterisation of five such oligomers are described, and an electrochemical analysis using cyclic voltammetry is performed to determine the anodic peak potentials. A structural study is performed on six self‐doping oligomers in which the structures and energies of the possible mono‐molecular forms of the electrically conducting doped material are described and evaluated using Hirshfeld charges and the Quantum Theory of Atoms In Molecules. Copyright © 2009 John Wiley & Sons, Ltd.