ZnO粉末中无序激射现象时间分辨的研究

采用抽运-探测时间分辨方法实验研究了半导体材料ZnO纳米颗粒粉末中的无序激射现象.在2 67nm激光的抽运下，通过精确控制抽运光的能量和样品表面的抽运面积，获得了宽度小于1n m的单模无序激射光谱和多峰的多模无序激射光谱.时间分辨的抽运-探测结果显示，此时样 品的上能级寿命仅为几个皮秒，证明了ZnO粉末的单模无序光谱是受激辐射的结果. 关键词： 高散射介质 多重散射 抽运-探测 无序激射     

Effect of particle size and shape on nonresonant random laser action of dye-doped polymer random media

We present an experimental study of the light emission from dye-doped polymer random media dispersed with TiO₂ particles of various sizes, shapes, and structures. Random lasing with nonresonant feedback, similar to that for spherically shaped particles that are used for conventional random lasers, is observed for almost all types of particles and aggregates. The efficiency of random lasing for each medium is analyzed using the relationship between the emission spectrum and the transport mean free path (TMFP), which is measured by enhanced backscattering experiments. Results show that the peak emission intensity depends strongly on the particle shape and structure, whereas the spectral linewidth is governed by the TMFP.     

Linear and nonlinear optics,dynamics, and lasing in ZnO bulk and nanostructures

In linear optics, we report on measurements of the absolute external quantum efficiency of bulk ZnO and powders using an integrating sphere. At low temperature the near band edge emission efficiency can reach 0.15 in the best samples. For deep center luminescence this value may be even higher. When going to room temperature (RT) the quantum efficiency drops by about one order of magnitude. From time resolved luminescence measurements we deduce the lifetime of the free and bound excitons to be in the sub ns regime and find for the latter a systematic increase with increasing binding energy.Concerning lasing, we discuss the role of excitonic processes and the recombination in an inverted electron–hole plasma (EHP). While excitonic processes seem well justified at lower temperatures and densities, doubts arise concerning the concept of excitonic lasing at RT in ZnO. The densities at laser threshold at RT are frequently close to the Mott density or above but below the density at which population inversion in an EHP is reached. We suggest alternative processes which can explain stimulated emission in this density regime in an EHP at RT.     

染料掺杂聚合物薄膜中金纳米颗粒增强的随机激光

基于金属纳米结构而获得随机激光的增强,其独特的性质及其潜在的应用价值具有重要的研究意义,在表面增强荧光、光学开关器件、表面等离子激元激光等方面实现了较多应用。报道一种快捷有效的制备纳米颗粒的手段并基于该纳米颗粒结构分析了染料掺杂聚合物薄膜涂覆的随机激光现象和规律。利用离子溅射沉积和高温热处理在石英基底上制备了Au纳米颗粒,改变溅射时间Au纳米颗粒的尺寸发生可控变化,该方法便捷、工艺简单。研究采用40,80和120 s三种不同的时间进行Au膜溅射并在650 ℃下高温处理,得到粒径尺寸不同的Au纳米颗粒,随着溅射时间延长Au纳米颗粒的尺寸逐渐变大。通过涂覆有机荧光染料DCJTB掺杂的PMMA聚合物薄膜构建光致激射系统,利用纳秒脉冲激光对样品进行激发,得到随机激光并研究其出射光强度和阈值的变化规律特征。40,80和120 s三种溅射时间下所得Au纳米颗粒的平均粒径尺寸分别为230,250和390 nm,在532 nm激光激发下产生随机激光的阈值分别为20.5,17.5和12.5 μJ·pulse-1。Au纳米颗粒尺寸越大、粒子间距越小时,光子散射的平均自由程越短,光在金属颗粒之间可以多次有效散射,从而显著提高散射效率,产生较低阈值的激光发射;Au纳米颗粒的吸收峰与染料的荧光峰恰好匹配时,将会显著增强染料的荧光效应,激发更多染料分子发生能级跃迁,增加光子态密度,获得峰值更高、阈值更低的激射现象;泵浦光不破坏染料分子的情况下,可以多次循环泵浦获得激光,染料分子的发光效率随着多次激发略有降低,有助于随机激光器件的研究开发。实验研究结果与理论分析相一致,进一步明确了Au纳米颗粒对光子散射和等离子共振对光吸收增强的随机激光发射机理。该研究以Au纳米结构对光子的强散射效应为增益,通过理论分析和实验测量获得随机激光,为实现高效率、低阈值的随机激光研究提供了一种便捷的技术手段,有望促进随机激光器件的开发和应用。     

掺杂硅石纳米粉末的染料随机激光发射

针对染料随机激光器特性与应用研究,讨论了无序介质中荧光粒子和额外散射粒子的发光性质、浓度变化以及颗粒尺寸与随机激光发射阈值之间的关系。采用时域有限差分法直接求解Maxwell方程组及速率方程组的方法,模拟仿真出了相应的发射谱线及浓度变化与激光发射阈值的关系曲线。所设计的样品中Rh6G-SiO2的质量分数为4%,其阈值大小为8.5 J/pulse时,额外微小散射体TiO2的加入对该介质随机激光发射产生的影响很小,可忽略不计。在此基础上,通过进一步模拟分析了处于不同条件和背景下随机激光的阈值特性。     

Theoretical investigation on temporal properties of random lasers pumped by femtosecond-lasing pulses

Pulsing random lasing property has been investigated in both one- and two-dimensional random medium by numerically solving Maxwell’s equations and rate equations in which the pumping rate is described by a time function with duration of 10s or 100s of femtoseconds. The peak intensity, width and delay time of a random lasing pulse are traced with the variation of the peak intensity, duration, shape and numbers of a pumping pulse. Results show that the behavior of random lasing depends strongly on the pumping process, some of which are in agreement with previously reported experiments pumped by femtosecond-lasing pulses. The present work enriches the knowledge about random lasers, especially in temporal regime, and could offer more guidance for relevant experiments.     

Random laser action in ZnO

We report a direct evidence of random laser in optically pumped ZnO powder. Discrete lasing modes are observed above threshold. The laser emission spectra depend on the angle of observation and are random. The lasing action is attributed to the coherent feedback due to recurrent light scattering in the powder. The lasing threshold intensity depends on the excitation volume. Received: 15 September 1999 / Revised version: 2 February 2000 / Published online: 5 July 2000     

Synthesis, morphology and random laser action of ZnO nanostructures

Three-dimensional (3-D) ZnO random-wall nanostructures and one-dimensional (1-D) ZnO nanorods were prepared on silicon substrates by a simple solid-vapour phase thermal sublimation technique. Optical pumped random lasing has been observed in the ZnO random-wall arrays with a threshold intensity of 0.38 MW/cm² in the emission wavelength from 380 to 395 nm. The optical gain was attributed to the closed-loop scattering and light amplification of the ZnO random-wall. The experimental result suggests that the morphology of nanostructure is the key factor to effect random lasing.     

Identification of statistical regimes and crossovers in coherent random laser emission

We measure intensity statistics and identify statistical regimes and crossovers in random lasers based on nonresonant feedback. A single parameter extracted from an α-stable Levy fit is used to characterize the intensity distributions in all regimes. Measurements made over a range of scattering strengths, excitation energies, and sample sizes enable us to demarcate three regimes of intensity statistics and the corresponding crossovers. An initial subthreshold Gaussian regime abruptly transits into a Levy regime at the random lasing threshold, which is followed by a continuous gradual crossover toward a second Gaussian regime. We find that the prominence of the Levy regime depends upon the sample size.     

Random lasing in porous scattering medium

The spectrum behavior evolution and the threshold of random lasing depending on the way of photon walk randomization in an active random medium were investigated. The following three ways of photon walk randomization were implemented: multiple light scattering by corundum and silica particles embedded into a solid polymer solution of dye (astrafloxin), multiple light reflection at sub-millimeter extensive air pores (mean diameter 200 μm) produced in the medium, and the combined action of both these effects. The most effective lasing is observed in the case of an active medium with air pores and scattering particles in the interpore space. Such a combined porous scattering medium acts as a network of dielectric waveguides transmitting effectively the random light. This spatial structure of the random active medium significantly increases the photon path in the medium, thereby promoting photon multiplication due to stimulated emission. In this combined medium the random lasing reveals the narrowest spectrum, the lowest threshold, and the highest density of spectral energy in the spectrum maximum.     

光子晶体晶粒尺寸和排列结构对随机激光辐射特性的影响

研究了光子晶体对随机激光器的输出特性的调控,并分析了光子晶体的晶粒尺寸和排列结构等对调控作用的影响.对于同一随机介质而言,上下表面用同种材料不同晶粒尺寸的光子晶体覆盖,结果显示:晶粒尺寸合适的光子晶体会使光在系统中来回振荡从而得到很好的放大,使系统中的光与随机增益介质的相互作用加强,激光阈值降低;同时还对激光模式有较强的调制能力,能在一定程度上抑制自发辐射,使之向所需要的频率内辐射.但如果光子晶体的晶粒尺寸与随机增益介质结构匹配不当,则光子晶体对激光模式调制能力较弱,光场能量不能有效地被局域在系统中,系统 关键词： 有限时域差分法 光子晶体 随机激光 辐射特性     

Random lasing in an organic light‐emitting crystal and its interplay with vertical cavity feedback

The simultaneous vertical‐cavity and random lasing emission properties of a blue‐emitting molecular crystal are investigated. The 1,1,4,4‐tetraphenyl‐1,3‐butadiene samples, grown by physical vapour transport, feature room‐temperature stimulated emission peaked at about 430 nm. Fabry‐Pérot and random resonances are primed by the interfaces of the crystal with external media and by defect scatterers, respectively. The analysis of the resulting lasing spectra evidences the existence of narrow peaks due to both the built‐in vertical Fabry‐Pérot cavity and random lasing in a novel, surface‐emitting configuration and threshold around 500 μJ cm⁻². The anti‐correlation between different modes is also highlighted, due to competition for gain. Molecular crystals with optical gain candidate as promising photonic media inherently supporting multiple lasing mechanisms.     

Photoluminescence and time-resolved photoluminescence of star-shaped ZnO nanostructures

Optical properties of star-shaped ZnO nanostructures were studied. The temperature-dependent photoluminescence (PL) was examined up to fourth-order longitudinal optical (LO) phonon assisted emissions of free excitons and confirmed that the nature of the room temperature PL in ZnO is 1-LO phonon assisted emission of free excitons. Low threshold ultraviolet stimulated emissions (SE) were obtained for our powder samples at room temperature. Picosecond time-resolved PL measurements detected a bi-exponential decay behavior which is strongly dependent on the excitation intensity: the slow decay term decreased faster than the fast decay term as the excitation intensity increased and the emission decays were dominated by the fast one. We also found that the emission decays decreased super-linearly before the appearance of the SE. This behavior may be used to deduce the threshold of SE or lasing.     

Random lasing in dye-doped polymer dispersed liquid crystal film

A dye-doped polymer-dispersed liquid crystal film was designed and fabricated,and random lasing action was studied.A mixture of laser dye,nematic liquid crystal,chiral dopant,and PVA was used to prepare the dye-doped polymer-dispersed liquid crystal film by means of microcapsules.Scanning electron microscopy analysis showed that most liquid crystal droplets in the polymer matrix ranged from 30 μm to 40 μm,the size of the liquid crystal droplets was small.Under frequency doubled 532 nm Nd:YAG laser-pumped optical excitation,a plurality of discrete and sharp random laser radiation peaks could be measured in the range of 575–590 nm.The line-width of the lasing peak was 0.2 nm and the threshold of the random lasing was 9 m J.Under heating,the emission peaks of random lasing disappeared.By detecting the emission light spot energy distribution,the mechanism of radiation was found to be random lasing.The random lasing radiation mechanism was then analyzed and discussed.Experimental results indicated that the size of the liquid crystal droplets is the decisive factor that influences the lasing mechanism.The surface anchor role can be ignored when the size of the liquid crystal droplets in the polymer matrix is small,which is beneficial to form multiple scattering.The transmission path of photons is similar to that in a ring cavity,providing feedback to obtain random lasing output.     

Taming Random Lasers through Active Spatial Control of the Pump

Active control of the spatial pump profile is proposed to exercise control over random laser emission. We demonstrate numerically the selection of any desired lasing mode from the emission spectrum. An iterative optimization method is employed, first in the regime of strong scattering where modes are spatially localized and can be easily selected using local pumping. Remarkably, this method works efficiently even in the weakly scattering regime, where strong spatial overlap of the modes precludes spatial selectivity. A complex optimized pump profile is found, which selects the desired lasing mode at the expense of others, thus demonstrating the potential of pump shaping for robust and controllable single mode operation of a random laser.     

Femtosecond laser ablation of ZnO nanorods for two-photon-pumped random lasing and optical data storage

Femtosecond laser ablation based on two-photon absorption was employed to cut ZnO nanorods into uniform ZnO nanoparticles of deep subwavelength size. The fabricated ZnO nanoparticles possess a shorter mean transport length for photons at the emission wavelength and a much smaller scattering cross section at the pump wavelength, leading to highly efficient two-photon-pumped random lasing with a low threshold of ??8?mJ/cm². It was demonstrated that the significant enhancement in two-photon luminescence after the irradiation of femtosecond laser pulses could also be utilized for realizing optical data storage.     

Random laser in one dimension

We present an analytical approach to random lasing in a one-dimensional medium, consistent with transfer matrix numerical simulations. It is demonstrated that the lasing threshold is defined by transmission through the passive medium and thus depends exponentially on the size of the system. Lasing in the most efficient regime of strong three-dimensional localization of light is discussed. We argue that the lasing threshold should have anomalously strong fluctuations from probe to probe, in agreement with recent measurements.     

随机性对部分随机介质激光器阈值的影响

基于速率方程和Maxwell方程相结合的模型，采用时域有限差分法(FDTD)研究了介质的随机性和层数对部分随机介质激光器阈值的影响.模拟结果显示，当抽运速率超过阈值时，出现一个或者多个振荡模；随机性或者系统的尺度增加时，振荡模数量也增加；部分随机介质激光器的阈值在一定的随机强度和层数下将达到最小值，它与完全随机情况下的结论有所不同.对所得到的结论给出了物理解释.这些结果对于制作随机激光器和光集成潜在应用价值. 关键词： 激光物理 随机激光器 阈值 时域有限差分法     

Tailoring of random lasing characteristics in dye-doped nematic liquid crystals

Amplified spontaneous emission and random lasing are investigated in random systems with dye-doped nematic liquid crystals. And that temporal stability of random lasing is analyzed. The influence of pumping polarization as well as the multiple scattering and reflection between boundaries on the emission behavior and the formation of coherent feedback is investigated in detail. For freely suspended samples, certain emission wavelength can be obtained by changing the pump wavelength. This feature is useful in making wavelength-tunable lasers. Moreover, as the pumping thickness of wedge sample increases, the emission spectrum is red shifted and the average spacing of adjacent spikes decreases. This property can be applied in laser mode selection, i.e., the number of modes within certain wavelength range can be chosen.     

基于多形貌银纳米颗粒的多波长相干随机激光研究

采用溶剂热法分别制备了球形银纳米颗粒和多形貌银纳米颗粒,其中球形银纳米颗粒具有400 nm的窄带等离激元共振峰,而多形貌银纳米颗粒的共振区间在400～700 nm之间,将它们分别掺入R6G与PVP的混合溶液中,利用旋涂法在玻璃基板上制备银纳米颗粒嵌入染料掺杂聚合物薄膜随机激光器。采用纳秒脉冲激光进行随机激光泵浦实验,实验结果表明球形银纳米颗粒染料掺杂聚合物薄膜只有自发辐射峰,而多形貌银纳米颗粒染料掺杂聚合物薄膜具有线宽<0.8 nm的相干随机激光发射光谱,其阈值为1.9 mJ·cm-2, 这可能是由于银纳米颗粒的等离激元共振区间与R6G的发射光谱重叠,支持局域等离激元效应的形成,明显的局域场增强有效地改善了与附近分子的相互作用,从而激发了更多的辐射光子,促进了高增益的形成。进一步,利用多形貌银纳米颗粒在银纳米颗粒染料掺杂聚合物薄膜中随机分布的特性,通过改变泵浦位置,实现了20 nm范围内的随机激光输出波长的调控,具体输出范围为590.1～610.4 nm。认为这是由于多形貌银纳米颗粒在不同位置的组成和分布不同,改变了表面等离激元的相互作用和光子的散射能力,从而形成不同的增益效应和不同的封闭光振荡路径。此外,考虑到多形貌银纳米颗粒的共振波长较宽,探究了其用于输出其他颜色光的可能性。以与上述银纳米颗粒R6G染料掺杂聚合物薄膜相似的制备方法,制备了多形貌银纳米颗粒掺杂DCJTB染料聚合物薄膜,并且进行随机激光泵浦实验。结果表明,可以有效的产生波长为675 nm,半高宽<0.8 nm的相干红光随机激光,并且阈值仅为0.98 mJ·cm-2。研究结果在宽带可调谐随机激光器研究以及多色随机激光器研究领域具有重要的参考价值。