Stimulated globular scattering of laser radiation in photonic crystals: Temperature dependences

The characteristics of stimulated globular scattering such as the frequency shift, threshold, and conversion efficiency are studied in photonic crystals (synthetic opal matrices and opal nanocomposites) at different temperatures. The results are compared with the study of stimulated Raman scattering in calcite single crystals. In both cases, a decrease in temperature from +20° C to −196° C resulted in an increase in the energy of stimulated scattering energy and its redistribution into the higher-order components.     

Modified cascade model of resonant Raman scattering: a case study of UV Raman scattering in Zn1−xMnxO thin films

The cascade model of inelastic resonant Raman scattering considers real electronic states in the conduction band (CB) as intermediaries to explain multiple longitudinal optical (LO) Stokes‐shifted lines in the emission spectra. In this study, we report modification in the cascade model under conditions where the scattered photons after multiple transitions have energy lower than the bandgap (E_g) and give rise to higher order n‐LO lines. The higher order n‐LO lines involve electron transition between the trap levels, which are created by impurities or defects in the forbidden energy gap, and are analogous to the real electronic states in CB, depending on the density of defects or impurities in the lattice. The presence of traps in the forbidden gap (1) acts as virtual intermediate states giving rise to higher order n‐LO modes and (2) tends to decrease the radiative recombination probability leading to quenching of the luminescence emission and line width (full‐width at half‐maximum) broadening. Ultraviolet Raman scattering in Mn‐doped ZnO (Zn_1−xMn_xO) thin films were investigated and the experimental observations analyzed in the domain of the modified cascade model. Copyright © 2011 John Wiley & Sons, Ltd.     

Raman and Hyper-Rayleigh Scattering in Lithium Tetraborate Crystals

Experimental studies of Raman scattering and the infrared reflection spectra of lithium tetraborate crystals were carried out within a broad temperature range with various polarization geometries. The crystals studied are characterized by record values of radiation resistance, transparence within a broad spectral range including the ultraviolet region, and nonlinear optical properties. A group-theoretical analysis of the vibrational spectra of this crystal was performed and fundamental vibrational terms were assigned to the symmetry types of the point group as well as the polarizations of the corresponding modes. The effective Raman cross section was measured and was found to be one order of magnitude higher than those of the known crystals, in which the stimulated Raman scattering (SRS) was observed. The nonlinear optical and electrooptical coefficients were evaluated and were found to be consistent with the results of independent measurements. The effect of a drastic increase in the intensity of quasi-elastic light scattering at 253 K was registered. It was associated with the phase transition that consists of the disordering of lithium ions with respect to the rigid skeleton. The formation energy for Frenkel defects in the lithium sublattice and the activation energy of the ionic conduction when heating the sample were calculated from the obtained temperature dependences of the intensity of quasielastic and hyper-Rayleigh light scattering.     

Structure of light scattering spectra in opal photonic crystals

Spectra of light losses are studied at a fixed angle of incidence of a collimated beam on the surface of an opal anisotropic photon crystal at various observation angles. It is shown that the structure of the forward-and backscattered light spectra is connected with the existence of several directional photonic forbidden bands. It is demonstrated that back scattering is enhanced and forward scattering is suppressed in the frequency region of photonic forbidden bands. It is suggested that a scattering band associated with photon localization at the photonic gap edge is observed.     

Raman spectroscopy in GaS: Zone boundary phonon interactions

Summary A complete polarization analysis of the GaS Raman spectrum, for excitation energies below the indirect energy gap, is reported. In order to assign second-order combinations and defect-induced forbidden modes, that appear in the spectra besides the six well-known Γ-phonons, also IR transmittance and reflectance measurements, for bothE⊥c andE‖c, have been performed. All the available selection rules are applied to both Raman and IR data, allowing to identify the high-symmetry points of phonons involved in the scattering and, when possible, to ascribe the main non-Γ structures of the spectra to the knownK andM point modes. This analysis brings to several new attributions, also ruling out some previous assignments, based on the separate study of either Raman or IR spectra. Work partially supported by M.P.I.     

可变晶格常数乙醇-二氧化硅胶质光子晶体中的Raman散射

制备了乙醇 二氧化硅三维胶质光子晶体，其晶格常数随着晶体高度的变化而变化.用皮秒 脉冲激光在不同高度激发光子晶体中乙醇产生Raman信号，得到了两个结果：1）即使Raman 信号的中心频率与光子晶体的带隙中心频率一致，在其禁带方向上测得的强度也没有被抑制 到与带隙深度同样的量级；2）尽管单纯的具有Raman信号频率的入射光的透过率随着高度的 变化而剧烈变化，但在光子晶体中产生的Raman信号强度却几乎不随高度的变化而变化，即 光子晶体的赝带隙几乎没有影响在禁带方向上测得的Raman信号强度.基于“光子晶体 关键词： 光子晶体 Raman散射 赝带隙 内部光源     

Stimulated Raman scattering in light and heavy water under picosecond laser excitation

The spectra of stimulated Raman scattering in ordinary and heavy water under excitation by second harmonic of a picosecond Nd:YAG laser were compared. It was shown that when stimulated Raman scattering is excited in water in cavities of a photonic crystal (synthetic opal matrix constructed of silica nanoglobules) or a photonic glass in the form of close-packed monodimensional millimeter-size amorphous-quartz balls, the efficiency of stimulated Raman scattering increases significantly compared to a uniform liquid medium.     

Stimulated Raman scattering of light in artificial opal filled by water

We investigate stimulated scattering of light in globular photonic crystals infiltrated by water. Excitation of stimulated scattering of light is realized using powerful ultrashort (70 ps) laser pulses with an energy of 35 mJ and a frequency repetition of 15 Hz. We use the second-harmonic generation (532 nm) of the master oscillator and amplifier with a wavelength of 1064 nm. The photonic crystals under study are artificial opals filled by water or ethanol. We characterize the sample structures employing an electronic microscope along with the fiber-optics reflectance-spectroscopy technique. Photonic crystals have a stop band near the spectral positions of the exciting line (532 nm) and the first satellite of stimulated Raman scattering of light in water (649 nm). We observe a substantial reduction of the threshold of stimulated Raman scattering of light in water-infiltrated artificial-opal matrices in comparison with that of pure water. Such a reduction is explained as the result of a sharp increase in the photonic density of states near the stop-band edges of investigated photonic crystals. The reduction in the threshold of stimulated Raman scattering of light in water-infiltrated artificial-opal matrices opens up the opportunity to observe stimulated Raman scattering in numerous water media, including water solutions, biological and medical samples, heavy waters, and others.     

Effect of isotope substitution and doping on the Raman spectrum of galena (PbS)

The Raman spectrum of natural PbS has been shown to exhibit features related to the IR-active (Raman forbidden) LO phonons and to allowed scattering by two phonons. In order to confirm the vibrational nature of these features, and their peculiar temperature dependence, we compare here the spectra obtained for natural samples (i.e. mineral as well as synthetic with the natural isotopic abundance) with those measured for crystals prepared from highly enriched ³⁴S. The observed isotopic shifts confirm the vibrational nature of the structures mentioned above. We have also measured the spectra of synthetic samples of PbS annealed at several different pressures of sulphur. Because of their non-stoichiometric sulphur content they have carrier concentrations (either electrons or holes) in the 1×10¹⁷-3×10¹⁸ carriers/cm³ range (as determined from their IR reflection spectra). The measured spectra, as well as their temperature dependence, do not depend on the bulk carrier concentration, a fact that must result from surface pinning of the Fermi level within the fundamental energy gap.We finally discuss the apparent paradox of why the IR spectra reveal coupled LO-phonon-plasmon modes whereas the Raman spectra exhibit the bare LO-phonons.     

Electronic Raman Scattering in Graphene

Linear dispersion near the Dirac points in the band structure of graphenes can give rise to novel physical properties. We calculate the electronic contribution to the Raman spectra in graphenes, which also shows novel features. In the clean limit, the Raman spectrum in the undoped graphene is linear （with a universal slope against impurity scattering） at low energy due to the linear dispersion near the Dirae points, and it peaks at a position corresponding to the van Hove singularity in the band structure. In a doped graphene, the electronic Raman absorption is forbidden up to a vertical inter-band particle-hole gap. Beyond the gap the spectrum follows the undoped case. In the presence of impurities, absorption within the gap （in the otherwise clean case） is induced, which is identified as the intra-band contribution. The Drude-like intra-band contribution is seen to be comparable to the higher energy inter-band Raman peak. The results are discussed in connection to experiments.     

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应用多光子非线性Compton散射模型和时域有限差分法,对Compton散射对时变非磁化等离子体光子晶体禁带的影响进行了研究,提出了将多光子非线性Compton散射电磁波和入射电磁波作为等离子体光子晶体产生光子禁带的新机制,给出了电磁场的Maxwell方程组和叠代方程的修正方程,并进行了数值模拟。结果表明,Compton散射使等离子体禁带宽随等离子体上升时间的增大比散射前有明显减小而最后趋于定值,均匀等离子体透射率峰值比线性等离子体增大得更多,利用Compton散射可实现对光子禁带的控制。     

Stimulated Raman scattering in three-dimensional photonic crystals

The results of experimental studies of stimulated Raman scattering of light (SRS) excited in three-dimensional photonic crystals — synthetic opal matrices infiltrated with Raman active media are presented. It is shown that the SRS threshold in such structures decreases with respect to the SRS threshold in Raman active bulk materials. The influence of the photonic-band structure of the active materials used on the SRS properties is estimated.     

一种可精确控制粒径的SiO2微球合成方法

用改进的种子法合成SiO₂微球. 微球生长过程中连续缓慢添加正硅酸乙酯,使用动态光散射法实时监控微球粒径的增长过程,调节正硅酸乙酯的添加,实现对粒径的精确控制. 为制备禁带位置位于1000 nm 的光子晶体,合成粒径为446 nm的SiO₂微球,微球粒径在4 h内从193 nm 增长到446 nm,远远快于传统种子法,微球粒径与目标粒径偏差为±5 nm. 制得的SiO₂微球被组装为光子晶体,其禁带位置恰好位于1000 nm.     

含有多缺陷的一维光子晶体的完全透射及应用

计算了具有多缺陷且相对中间缺陷具有镜像对称结构的一维光子晶体的透射谱。在光子晶体的禁带中得到了多个完全透射峰且对称性地分布于禁带中心频率两侧。缺陷相距较近时，禁带中心不存在透射峰。所有透射峰都敏感地依赖于中间缺陷的折射率。     

Compton散射对非均匀等离子体光子晶体光子带隙的影响

应用多光子非线性Compton散射模型和时域有限差分法,对多光子非线性Compton散射对非均匀等离子体光子晶体光子带隙特性的影响进行了研究,提出将入射和散射光作为形成光子带隙的新机制,对电磁波方程进行了修正.结果表明:与Compton散射前相比,散射使电磁波幅值衰减更快|随等离子体密度增加,透射谱禁带宽度几乎无变化,其中心频率向高频方向有明显移动,向上的峰值有较大增加,反射谱向下的峰值有明显减小|随温度增加,透射谱禁带宽明显减小,向上的峰值略有减小,透射能量有所降低|随两种介质介电系数比增加,光子禁带数增加,且带隙间距显著减小.     

Probe Raman spectroscopy in photon traps

It was found that the use of multifiber probes and photon traps allows contactless measurement of Raman scattering spectra for small amounts (～1 µg) of organic and inorganic compounds at exposures of 1–16 s. The possibility of improving the sensitivity of Raman scattering spectrum measurement using globular photonic crystals as matrices or substrates carrying analyzed compounds was studied.     

Engineering disorder in three-dimensional photonic crystals

We demonstrate the effect of introducing controlled disorder in self-assembled three-dimensional photonic crystals. Disorders are induced through controlling the self-assembling process using an electrolyte of specific concentrations. Structural characterization reveals increase in disorder with increase in concentrations of the electrolyte. Reflectivity and transmittance spectra are measured to probe the photonic stop gap at different levels of controlled disorder. With increase in disorder the stop gap is vanished and that results in a fully random photonic nanostructure where the diffuse scattered intensity reaches up to 100%. The estimated scattering mean free path shows significant reduction for photonic crystals with 100% controlled disorder as compared to those with 0% controlled disorder. Our random photonic nanostructure is unique in which all scatters have the same size and shape. Therefore, we observe the resonant characteristics in the multiple scattering of light.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed. The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together. Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

Spontaneous Raman scattering spectra of ADP and DADP crystals in different polarization schemes

Spontaneous Raman-scattering spectra of light in ADP and DADP crystals were obtained in four polarization schemes, the widths of some Raman lines were measured. The presence of a strong and sharp Raman line corresponding to the totally symmetric vibration of the phosphate group and a strong diffuse Raman satellite corresponding to the totally symmetric vibration of the ammonium group in the spontaneous scattering spectra of both (ADP and DADP) crystals was observed. According to the theory, such lines are preferable for the stimulated Raman scattering.