Laser-assisted local patterning of ZnO-based spots for mirror-less lasing

ZnO is known as one of the best materials for the implementation of the random lasing effect, associated with mirror-less laser emission in a simultaneously amplifying and highly scattering medium. Normally, the fabrication of this medium requires a rather complicated procedure of deposition and thermal treatment of ZnO-based films on some specific substrates, yielding wurtzite-orientation ZnO nanocrystals. We demonstrate a rapid synthesis of highly efficient ZnO-based random lasing spots on a piece of Zn by employing the phenomenon of laser-induced air breakdown. Being ignited near the surface of a Zn target, plasma of the air breakdown serves as a local reactor to locally transform its properties and thus form a film of well-packed 20–40 nm ZnO nanospheres. Exhibiting extremely high amplification and scattering, this medium is capable of generating the random lasing effect within the exciton-based photoluminescent band.     

Lasing with guided modes in ZnO nanorods and nanowires

A vertically arranged nearly parallel array of ZnO nanorods and randomly oriented nanowires has been grown by low pressure chemical vapor deposition (CVD) on silica substrates and on stainless steel gauze woven from a wire with a diameter of 40 μm, respectively. The quality of the produced material is high enough to act as a gain medium for stimulated emission in the ultraviolet spectral region. Multiple sharp lasing peaks were realized from single hexagonal nanorods and arrays of hexagonal ZnO nanorods. The lasing peaks display successive onset and saturation with increasing excitation power density and fit well the expected resonance spectrum of guided modes in hexagonal nanorods. The behavior of lasing spectra from shot to shot of pumping in randomly oriented nanowires along with the independence of the lasing threshold on the excitation spot area suggest that the emission spectrum results from the superposition of lasing modes in individual nanowires, rather than from random lasing due to photon coherent scattering.     

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。     

Transition from amplified spontaneous emission to laser action in strongly scattering media

In an active random medium, the combination of multiple scattering with light amplification may lead to random laser action. However, it is crucial but sometimes difficult to distinguish between amplified spontaneous emission and lasing. By varying the amount of scattering in an amplifying random medium, we have observed the transition from amplified spontaneous emission to lasing with coherent feedback. We have found out when the transition occurs through the measurement of the scattering mean free path. Our numerical simulation based on the direct solution to Maxwell equations clearly illustrates the transition from light amplification to laser oscillation due to an increase of the amount of scattering in active random medium.     

Random lasing in ZnO nanocrystals

Nanocrystalline ZnO powders can act as gain and scattering medium in a random laser where the light emission can be strongly amplified. In this work, we compare the luminescence properties of samples with different particle sizes in the regime of linear and nonlinear optics. In the high-excitation regime random lasing is observed in all samples. Here, the lasing threshold depends strongly on the size distribution in the ensemble. Additional characterization of the samples has been done by determining the absolute quantum efficiency of the radiative processes in the powder. The values are in the 10% range and the near-edge luminescence is strongly influenced by the particle sizes. We show that by annealing the nanocrystals coalesce to larger polycrystalline grains, which results in a new emission band at 3.333 eV due to the grain boundaries. Furthermore, it is found that in the annealed samples the threshold for random lasing could be considerably decreased.     

基于TiO_2纳米粒子薄膜的低阈值随机激光器的动力学研究

本文利用共轭聚合物(MEH-PPV)覆盖TiO_2纳米粒子薄膜制作随机激光器。随机TiO_2纳米粒子薄膜的激光辐射阈值比平面MEH-PPV薄膜的放大自发辐射阈值缩小了9倍。这是由于TiO_2纳米粒子诱导的多重散射造成的。进一步的飞秒荧光上转换实验表明,随机激光器中,光在增益介质里的停留时间有所增加,这直接证实了光在随机激光器结构中的多重散射引起光的传播路径增加。因此,这会促进更多的光发生辐射,从而降低随机激光器的阈值。     

无序介质激光的方向效应

无序介质激光是由该介质的非周期-类结构与相匹配的泵浦光场相互作用时其整体多重散射的干涉效应产生的.因此其局域模不仅与无序介质被泵浦的功率、面积有关,而且与方向有关.本文以ZnO粉末激光为例,运用传输矩阵的方法计算模拟了其局域模谱的方向效应.     

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.     

Lasing in random media

A random laser is a non-conventional laser whose feedback mechanism is based on disorder-induced light scattering. Depending on whether the feedback supplied by scattering is intensity feedback or amplitude feedback, random lasers are classified into two categories: random lasers with incoherent feedback and random lasers with coherent feedback. A brief survey of random lasers with incoherent feedback is presented. It is followed by a review of our recent experimental work on random lasers with coherent feedback, including measurement of the lasing threshold, lasing spectra, emission pattern, dynamical response, photon statistics, speckle pattern and the investigation of relevant length scales. Large disorder leads to spatial confinement of the lasing modes, that is the foundation for the micro random laser. Some theoretical models of random lasers with coherent feedback are briefly introduced. The study of random lasers improves our understanding of the interplay between light localization and coherent amplification.     

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     

Extremely selective modal oscillation of random lasing induced by strong multiple scattering

We report on a new physical aspect of random lasing, an extremely selective modal oscillation by using a two-dimensional calculation model. The developed model consists of two theoretical subsystems, two-dimensional scattering model for describing multiple scattering process and rate equation model for describing lasing process. Using this model, we show how emission spectrum behaves as the scattering state of photons inside the system changes. It is shown that specific and strong modal oscillation takes place in a closed loop path of emitted photons, efficiently supported by the background multiple scattering. With the increase of multiple scattering events around the closed loop path, the system starts to oscillate with an extremely strong mode without any ASE (amplified spontaneous emission) noise.     

蒙特卡罗法计算无序激光器的阈值

提出了计算无序激光器阈值增益的模型,提出了已知平均自由程和散射强度分布得到分布函数及相应的随机变量的方法.对各向同性的光散射,导出了各分布函数,并在每次散射中得到相应的随机变量.运用蒙特卡罗法模拟光子在无序介质中的随机行走,得到了无序激光器的阈值.讨论了阈值增益与光子平均自由程、增益区半径、增益区深度、非增益区光吸收系数的关系,提出了降低阈值的方法.理论结果与实验数据是符合的. 关键词： 激光物理 阈值 蒙特卡罗 散射     

Effect of Pump Area on Lasing Modes in Active Random Media

We investigate the effect of pump area on lasing modes in an active random medium. Considering the structure characteristics in a real experimental system, the random medium is divided into two regions, i.e. pump and non-pump areas. The dependence of lasing modes on the pump area is qualitatively explained by means of the model in which the lasing is ascribed to the interaction of the complex localized modes in the active random medium with local aperiodic quasi-structure with appropriate pump light. There exist different pump sizes for lasing with different modes. As the pump size decreases in this random system, the pump threshold of the lasing modes increases. There are different lasing modes in different excitation regions in this random system. This gives us some information about the dependence of lasing modes on pump areas in active random media.     

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。     

Photon localization laser: low-threshold lasing in a random amplifying layered medium via wave localization

We demonstrate low-threshold lasing in random amplifying layered medium via photon localization. Lasing is facilitated by resonant excitation of localized modes at the pump laser wavelength, which are peaked deep within the sample with greatly enhanced intensity. Emission occurs into long-lived localized modes overlapping the localized gain region. This mechanism overcomes a fundamental barrier to reducing lasing thresholds in diffusive random lasers, in which multiple scattering restricts the excitation region to the proximity of the sample surface.     

Numerical study of random lasing in three dimensional amplifying disordered media

In this paper, the lasing action in three-dimensional active random systems has been numerically investigated. Here, random systems of spherical dielectric particles imbedded in an active medium are considered. The quasi steady state approximation for the population inversion of the active medium is applied to solve three dimensional governing equations. Results show that when the density of particles increases to an upper limit, the intensity of lasing modes is enhanced. Also, the effects of pumping rate and particle size on the number of lasing modes and their intensity are studied. Lasing threshold of laser modes in different disordered systems is calculated and it is shown that by an appropriate selection of the central frequency of gain line-shape, the output power intensity of random lasers increases. These results are in agreement with the experimental results observed by others.     

二维随机介质中的能量分布和频谱特性

研究了二维随机介质中能量的空间分布和一些特定区域的频谱特性.结果显示介质中能量呈局域化分布,其分布与介质中颗粒的随机分布有关,还与激发光的波长有密切的关系,介质中能量聚集的区域和介质的准封闭区域有一定关系但并非一一对应.所考察的各准封闭区域的频谱均随时间变化,在同一激发光的激励下各准封闭区域的频谱均不相同,而同一区域在不同的激发光的激励下频谱也不相同.当激发波长与准封闭区域的结构参数偏差较大时,频谱中谱峰会出现此消彼涨的模式竞争现象,而且能量衰减得较快;而当激发波长与该结构参数较接近时,相应的频谱中存在一 关键词： 激光物理 有限时域差分法 局域化 频谱特性     

Backscattering of laser light from colloidal silica

Light-scattering experiments gained prominence as potential applications of quantum optics, non-linear optics, and photon localization. The possibility of the realization of lasing action in random media has created much interest in the study of the coherent structure of the backscattered light from disordered media. Backscattering (BS) studies are carried out to analyze the possibilities of photon localization in colloidal silica. The scattering enhancement is best associated with the density of the scatterers. The width of the BS cone and, hence, the mean-free path is related to the concentration of the medium. The dependence of the photon wavelength on the possible characteristics of the scattering is presented.     

Discrete Green's Function for Lattice Random Walk

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Discrete Green's Function for Lattice Random Walk

A lattice random walk model based on particles scattering on discrete lattice of homogenous space is introduced. The discrete Green's function (DFG) for two-dimensional and three-dimensional lattice random walk of photon is found and proved by mathematical induction. The convolution theorem of photon lattice random walk is presented. They can be used with the method of images to calculate the photon density distribution in semi-infinite and finite slab homogenous turbid media such as tissue.