Optically excited secondary emission spectra of photonic crystals based on synthetic opals

The photonic dispersion, the group-velocity dispersion, the effective mass, refractive index, and the spectral distribution of the density of photonic states near the edge of the photonic stop band are numerically calculated in the one-dimensional model for photonic crystals based on synthetic opals. The fluorescence spectra of rhodamine 6G and 2,5-bis(2-benzoxazolyl)hydroquinone molecules infiltrated into a synthetic opal are measured. For both substances, it is observed that the spontaneous emission intensity in the range of the photonic stop band is appreciably suppressed. A blue shift of the fluorescence spectrum of rhodamine 6G molecules is revealed. Secondary emission of synthetic opals infiltrated with colloidal silver is observed in the Stokes range under excitation of opals by radiation at λ = 400 nm. The spectrum of the secondary emission is located in the range 450–590 nm, which contains the stop band and intervals near its edges.     

Optical characterization of synthetic opals

The results of a structural-optical characterization of synthetic opals are presented. Information on the growth-induced features of the opal structure was derived from an analysis of the position and width of the one-dimensional photonic band gap. The structure of the samples was found to vary substantially along the growth axis coinciding with the [111] direction of the fcc lattice. It was shown that the regions corresponding to early stages in the opal structure growth are typically strongly disordered, which manifests itself, in particular, in the crystallites being misoriented relative to the sample growth axis. It was concluded that the regions of synthetic opals most suitable for application as photonic crystals are those corresponding to later growth stages.     

Bragg diffraction of light in synthetic opals

Three-dimensional light diffraction from the crystal structure, formed by closely packed a-SiO₂ spheres of submicron size, of samples of synthetic opals was visualized. The diffraction pattern of a monochromatic light beam was established to consist of a series of strong maxima whose number and angular position depend on the wavelength and mutual orientation of the incident beam and the crystallographic planes of the sample. The diffraction patterns were studied under oblique incidence on the (111) growth surface of the sample and with light propagated in the (111) plane in various directions perpendicular to the sample growth axis. The spectral and angular relations of diffracted intensity were studied in considerable detail in both scattering geometries. The experimental data are interpreted in terms of a model according to which the major contribution to the observed patterns is due to Bragg diffraction of light from (111)-type closely packed layers of the face-centered cubic opal lattice. The model takes into account the disorder in the alternation of the (111) layers along the sample growth axis; this disorder gives rise, in particular, to twinning of the fcc opal lattice.     

High Miller-index photonic bands in synthetic opals

We present a detailed study of high Miller-index (h k l) photonic bands in a-SiO₂ synthetic opals. Polarized light transmission spectra of opals were studied in a wide wavelength range for all high symmetry directions on the Brillouin zone (BZ) in the face-centered cubic (fcc) lattice. It is shown that under the conditions of low dielectric contrast the dispersion of high Miller-index photonic bands is described well by the calculated dependences of Bragg wavelengths diffracted from the (h k l) crystallographic planes of the fcc lattice.     

In and Si distribution in synthetic opals

An X-ray photoelectric absorption by samples of synthetic opals (SO) loaded by In and Si has yielded filler distribution profiles over thickness. The SO+In sample exhibited a uniform filling of SO voids throughout the sample thickness (on average, 16.9% of each large void). The SO+Si sample, besides the near-surface region where large voids are completely filled, revealed a region with variable Si concentration in the SO, where the Si content decreases linearly down to a depth where pure SO is found. Fiz. Tverd. Tela (St. Petersburg) 40, 1373–1375 (July 1998)     

Sound velocity in single crystals of synthetic opals

The [111] longitudinal sound velocity (v _L) in a single-crystal synthetic opal has been measured at a frequency of 10 MHz in the temperature range 4.2–300 K. At 300 K, v _L=2.1×10⁵ cm/s. The quantity dv _L/v _{300 K}(T) (where v _T,K?v_{300 K}) in the ranges 4.2–200 and 200–300 K behaves in the way typical of amorphous and crystalline solids, respectively.     

Specific features in the thermal conductivity of synthetic opals

Data on the thermal conductivity ϰ _ph of the cluster lattice of synthetic opals are analyzed. All opals are divided into two groups according to the temperature dependence of their ϰ _ph. These are opals-1, whose thermal conductivity behaves like ϰ _ph(T) of quasi-crystalline materials, and opals-2, with a ϰ _ph(T) dependence typical of classical amorphous solids. Possible reasons for this difference are considered. An attempt is made to explain the complex temperature hysteresis in ϰ _ph(T) observed earlier in opals-2. Fiz. Tverd. Tela (St. Petersburg) 39, 392–398 (February 1997)     

Spectroscopy of the photonic stop band in synthetic opals

The photonic band gap of opals has been studied experimentally from their optical transmission spectra as a function of the incident beam orientation in the opal crystal lattice. The measurements were carried out for all high-symmetry points on the surface of the Brillouin zone of an fcc lattice. The experimental dependence of the energy position of the photonic band gap on the light wave vector direction is well described by the set of theoretical relations developed for the stop bands originating from the Bragg diffraction of light on {111}-type planes of the twinned fcc lattice of synthetic opals.     

Structural modification of synthetic opals during thermal treatment

The density and porosity of synthetic opals with spheres 315 and 1000 nm in diameter were measured in relation to the annealing temperature. At annealing temperatures of up to 500°C, the seeming density and porosity remain almost unchanged. Then, at temperatures of up to 950°C, the density increases gradually and, accordingly, the porosity decreases due to the collapse of nanopores caused by the sphere substructure. As the annealing temperature increases further, the opal density increases sharply up to 2.22 g/cm³ (which corresponds to the density of amorphous silica) and the open microporosity due to the voids between spheres disappears. Differential thermal and thermogravimetric analyses showed that SiO₂ powders with particles with average size of 315 and 1000 nm can have, respectively, two-and three-level systems of micro-and nanopores.     

Solid state broadening in Auger spectra

Some Auger spectra in the gas phase show extremely sharp lines and a great deal of fine structure while the Auger spectra of solids, even at high resolution, lack this detailed fine structure and generally have much broader peaks. In an effort to understand the broadening processes which occur on condensation of a gas or vapour to the solid phase, several solids for which high resolution gas phase data exists have been studied. The result of measurements of the M₄₅N₄₅N₄₅ Auger spectrum of cadmium are reported and comparison is made with the vapour phase data. Although the solid data contains considerable quasi-atomic fine structure the lines are broader than the vapour phase and by matching computer broadened vapour phase data to the experimental data an estimate of the individual line widths may be made. The relative intensities of the lines in the simulation agree closely with the solid data if loss processes are considered. Measurements have also been made on the same Cd transition in CdS and in this material the Auger lines are much broader than in Cd metal and the fine structure has almost disappeared. Results are also reported of measurements of the Auger spectra of solid rare gases made with the aid of a UHV cryostat capable of operating at temperatures down to 10 K. The gases studied were Xe, Ar and Kr and again comparison with computer broadened gas data enable the broadening of individual Auger lines to be estimated. Measurements of the line breadths have been made at various temperatures and the results of these experiments will be discussed in terms of lifetime and lattice vibrational broadening.     

Selective control of light beams in diffraction experiments on synthetic opals

This paper reports on an experimental and theoretical investigations of the possibility of selectively controlling the intensity of {hkl} diffraction reflections in synthetic opals. The calculations of the photonic stop-band width for low-contrast multi-component photonic crystals argue for a selective pattern of the vanishing of various {hkl} stop bands (and, accordingly, of the various {hkl} diffraction reflections) under variation of the dielectric permittivity of one of the components. Optical diffraction patterns have been studied visually and recorded in various scattering geometries with bulk opal samples illuminated by white unpolarized light. The experiments have made use of immersion spectroscopy, a method reducing essentially to successive measurements of diffraction patterns under variation of the dielectric permittivity of the liquid filler of the opal matrix. The {111} and {220} Bragg reflections have been observed to weaken noticeably at the filler permittivities matching very well with the values derived earlier from an analysis of transmission spectra.     

Polarization anisotropy of optical transmission in opals and Langmuir-Blodgett crystals

The transmission spectra of thin-film colloidal photonic crystals with three-dimensional and one-dimensional-two-dimensional photonic energy band structures, i.e., opals and Langmuir-Blodgett crystals with a refractive index contrast of ∼1.5: 1.0, have been measured in linearly polarized light. It has been demonstrated that the polarization anisotropy in the light transmitted through the crystal is uniquely related to the diffraction resonance and that the degree of polarization can exceed 90%. A higher degree of polarization is provided by lattices that are characterized by a smaller attenuation of light polarized in the plane of incidence. It has been revealed that the diffraction resonances from the crystal planes for which the dispersions are in anticrossing with the dispersion of the growth planes acquire the same anisotropy. The general character of the results obtained has been confirmed by the fact that the polarization anisotropy identically manifests itself in colloidal crystals that have different symmetries and lattice orderings.     

Disorder broadening of alloy Auger spectra

Auger spectroscopy promises the means to separate initial and final state contributions to the disorder broadening of core XPS spectra in disordered alloys. Auger disorder broadening, deduced from recent ab initio results, is predicted to be greater than XPS disorder broadening for Cu₅₀Pd₅₀ and Ag₅₀Pd₅₀ alloys. Simulations are used to assess whether this effect is observable experimentally despite the greater lifetime broadening of Auger spectra. A number of cases where narrow core–core–core Auger transitions should allow clear experimental identification of this effect are identified. The prospects for determining environment-resolved Auger spectra using APECS have been investigated.     

Low-temperature heat capacity and heat conductivity of single-crystal synthetic opals

The heat capacity at constant pressure (in the range 3–50 K) and the lattice heat conductivity (from 5 to 75 K) of a single-crystal synthetic opal are measured. It is shown that the heat capacity of the opal behaves at these temperatures in a way similar to porous amorphous materials. The data on the heat conductivity suggest that single-crystal opals can be related to a class of semicrystalline (partially crystallized amorphous) materials. However, because of specific features of their crystal structure, the opals form a nonstandard type of semicrystalline material which we termed semiamorphous.     

Acoustic properties of globular photonic crystals based on synthetic opals

Acoustic properties of globular photonic crystals based on synthetic opals and composed of closely packed SiO₂ globules about 200 nm in diameter are theoretically investigated. Dispersion characteristics of the investigated samples are numerically simulated, and the group velocity of acoustic waves and the effective mass of acoustic phonons are found. It is shown that phononic bandgaps in these photonic crystals are within the gigahertz frequency range. The effective mass of the acoustic phonons corresponding to the edges of the bandgaps is found, and a possibility that bound states of acoustic phonon pairs, biphonons, manifest themselves in the light scattering spectra is discussed.     

Multiple Bragg diffraction in low-contrast photonic crystals based on synthetic opals

The phenomenon of multiple Bragg diffraction in low-contrast photonic crystals based on synthetic opals has been studied both experimentally and theoretically. The transmission and reflection spectra of opal films near the K point of the Brillouin zone of the face-centered cubic lattice in s-polarization exhibit the effect of anticrossing of dispersion curves corresponding to the (111) and ([`1]11)(\bar 111) photonic stop bands. The effect of quasi-Brewster suppression of stop bands is clearly pronounced in p-polarization. The experimental data are analyzed using the calculation of the band structure of opal with the inclusion of the polarization of incident light.     

Secondary radiation of synthetic opals loaded by the sodium nitrite ferroelectric

This paper reports on a comparison of transmission, reflection, and secondary radiation spectra of unloaded synthetic opals and samples filled with the sodium nitrite ferroelectric (NaNO₂). The radiation is provided by semiconductor light-emitting diodes operating in the ultraviolet and visible spectral regions. Selective excitation of slow electromagnetic waves in a photonic crystal, an effect observed when the exciting radiation frequency approaches the stop-band edge, is studied.     

Optical characterization of natural and synthetic opals by Bragg reflection spectroscopy

The Bragg reflection of light from natural and synthetic opals was studied experimentally, and the samples were characterized by atomic-force microscopy. The reflection spectra were theoretically calculated within the model of a planar, periodically layered medium. A comparison of the experimental and calculated data made it possible to determine the parameters of the crystal structure of synthetic opals (lattice constants and sintering coefficients of a-SiO₂ particles). It was concluded that the pores in the structure of natural opals are filled by a material with a refractive index close to that of a-SiO₂.     

Stochastic broadening of signals in distorsionless transmission lines

The paper presents a theory of a stochastic continuous transmission line in which the series inductanceLΔ[1+l(x)], series resistanceRΔ[1+r(x)], shunt capacitanceCΔ[1+c(x)], and shunt conductanceGΔ[1+g(x)] are defined as Gaussian random functions. (The continuous line is considered as a limiting case of a lumped transmision line.) The non-negative random functionsL(x),R(x),C(x), andG(x) are chosen as delta-correlated, i.e. their correlation function is of the formΘδ(x′ −x″) whereΘ is a 4×4 positive definedx-independent matrix. Propagation of a signal of Gaussian shape is analyzed. A special attention is devoted to the so-called distorsionless lines defined by the deterministic conditionR/L=G/C. As a consequence of the stochasticity of the functionsl(x),r(x),c(x), andg(x), transmitted signals do become distorted: they become broadened. An explicit formula for this broadening is derived. This work has been supported by the Slovak Grant Agency VEGA under contract No. 1/4319/97.