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。     

Spatial confinement of laser light in active random media

We have observed spatial confinement of laser light in micrometer-sized random media. The optical confinement is attributed to the disorder-induced scattering and interference. Our experimental data suggest that coherent amplification of the scattered light enhances the interference effect and helps the spatial confinement. Using the finite-difference time-domain method, we simulate lasing with coherent feedback in the active random medium.     

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 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.     

Light transport and correlation length in a random laser

A random laser is a strongly disordered, laser‐active optical medium. The coherent laser feedback, which has been demonstrated experimentally to be present in these systems beyond doubt, requires the existence of spatially localized photonic quasimodes. However, the origin of these quasimodes has remained controversial. We develop an analytical theory for diffusive random lasers by coupling the transport theory of the disordered medium to the semiclassical laser rate equations, accounting for (coherent) stimulated and (incoherent) spontaneous emission. From the causality of wave propagation in an amplifying, diffusive medium we derive a novel length scale which we identify with the average mode radius of the lasing quasi‐modes. We show that truly localized modes do not exist in the system without photon number conservation. However, we find that causality in the amplifying medium implies the existence of a novel, finite intensity correlation length which we identify with the average mode volume of the lasing quasimodes. We show further that the surface of the laser‐active medium is crucial in order to stabilize a stationary lasing state. We solve the laser transport theory with appropriate surface boundary conditions to obtain the spatial distributions of the light intensity and of the occupation inversion. The dependence of the intensity correlation length on the pump rate agrees with experimental findings.     

Dynamic nonlinear effect on lasing in a random medium

We have studied both experimentally and numerically the dynamic effect of nonlinearity on lasing in disordered medium. The third-order nonlinearity not only changes the frequency and size of lasing modes, but also modifies the laser emission intensity and laser pulse width. When the nonlinear response time is longer than the lifetime of the lasing mode, the nonlinearity changes the laser output through modifying the size of the lasing mode. When the nonlinear response is faster than the buildup of the lasing mode, positive nonlinearity always extracts more laser emission from the random medium due to the enhancement of single particle scattering.     

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.     

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.     

Spontaneous-emission spectrum of the nonlasing supermodes in semiconductor laser arrays

It is shown that the interference between amplified spontaneous emission into the nonlasing supermode and the laser field of a semiconductor laser array causes spatial hole burning, which couples the dynamics of the amplified spontaneous emission with the laser field. In particular, phase locking between the amplified spontaneous emission and the lasing mode leads to the formation of a spectral triplet composed of in-phase relaxation oscillation sidebands and an out-of-phase line at the lasing frequency.     

Investigation of amplified spontaneous X-ray laser radiation using the equation for the transverse correlation function of the field

A physical model, based on the solution of the quasi-optics equation for the transverse correlation function (TCF) of the field amplitude, is developed for investigating the brightness, angular divergence, and spatial coherence of the amplified spontaneous emission in a laboratory X-ray laser. The model takes account of the spontaneous source of radiation, diffraction, regular refraction, regular amplification taking account of saturation, nonresonance absorption, scattering by small-scale fluctuations of the electron density and the gain, and scattering by random hose-like deviations of the extended plasma medium of the X-ray laser. It is established that the TCF method makes it possible to obtain the final result much more quickly than the basic Monte Carlo method for the parabolic equation for the field amplitude. As a result of the statistical linearization of the equation for the transverse correlation function in the presence of gain saturation, this method overestimates the absolute values of the average intensity of the amplified spontaneous radiation, but the maximum overestimation does not exceed 10%. It is found that fluctuations of the optical parameters of the medium of the X-ray laser degrade the quality of the amplified spontaneous radiation beam, and they are the analog of the nonresonance absorption from the standpoint of the effect on the brightness of the laser and therefore decrease the observed gain. For the characteristic conditions of an X-ray laser with a quasistationary generation scheme, the contribution of small-scale gain fluctuations and random hose-like deviations of the plasma filament of the laser to the scattering of the amplified spontaneous radiation is much smaller than the contribution of small-scale density fluctuations. Calculations of the amplified spontaneous radiation in an X-ray laser, which is produced by unilateral irradiation of a curved target and possesses an asymmetric plasma electron density profile in the gain zone, are performed. It is shown that in the gain saturation regime the coherence length and the coherent power of the amplified spontaneous radiation can be substantially increased, realizing in the gain zone a convex electron density profile instead of a typical concave profile. It is found that this improvement of the coherence occurs only under conditions such that the characteristic depth of the small-scale density fluctuations does not exceed several percent of the typical regular values of the density in the gain zone.     

Statistics of random lasing modes in weakly scattering systems

We investigated the statistics of random lasing modes in colloidal solutions with local pumping. The ensemble-averaged spectral correlation function of single-shot emission spectra exhibits regular oscillations. The statistical distribution of laser emission intensity follows a power-law decay, in comparison with an exponential decay of the statistical distribution of amplified spontaneous emission (ASE) intensity. The dramatic difference between the statistics of lasing peaks and that of the stochastic ASE spikes illustrates their distinct mechanisms.     

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。     

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.     

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.     

Effect of stimulated raman scattering on the formation of the random lasing spectrum of dyes

The nature of the line structure of the random lasing spectrum of vesicular films activated by dyes (rhodamine 6G, pyrromethene 597) has been analyzed. The spectral lines appear above the random lasing threshold and are manifested only within the spectrum of the amplified spontaneous radiation of dye molecules against the continuous-pedestal background. Their intensities are proportional to the product of the intensities of the pump and continuous spectrum at the frequencies of these lines, and the frequencies are exactly reproduced from pulse to pulse. The shifts of the lines are strongly correlated with the pump frequency and the frequencies of these lines coincide with the frequencies of the Raman scattering lines of dye molecules. Using these properties, it has been shown that the observed lines are due to stimulated resonant Raman scattering by dye molecules, which occurs simultaneously with the stimulated emission of these molecules. These two processes affect each other and jointly form a united nonlinear process where all of the oscillations active in Raman scattering are manifested.     

Room-temperature amplified spontaneous emission at 1300 nm in solution-processed PbS quantum-dot films

We report room-temperature amplified spontaneous emission and spectral narrowing at infrared wavelengths in solution-processed films made up of PbS quantum-dot nanocrystals. The results are relevant to optical amplification and lasing integrated upon a variety of substrates. The active optical medium operates at room temperature without any additional matrix material, providing an optical gain of 260 cm(-1) and a pump threshold of 1 mJ/cm(-2). Nanocrystals synthesized in an aqueous solution and stabilized by use of short ligands result in high quantum-dot volume fractions in solid films and in a redshift emission relative to absorption.     

Stimulated emission of argon dimers excited by a pulsed plasma-cathode discharge

Results are reported from a theoretical and experimental investigation aimed at obtaining lasing on transitions of an Ar₂ excimer laser pumped by a pulsed electric discharge. It is shown that by using a recently developed plasma-cathode discharge, quasi-cw excitation of the laser active medium can be achieved with a gain of around 0.1 cm⁻¹. The results of preliminary experiments performed using a model system indicate an effect wherein the duration of the spontaneous emission at the gl=126 nm transition of the Ar₂ dimer decreases monotonically as its peak intensity increases. This behavior, which is observed with increasing pump intensity, is evidence of a stimulated emission effect in the system. However, the measurements indicate that no amplification takes place in the active medium because of accidental impurities in the working gas. Zh. Tekh. Fiz. 67, 49–52 (November 1997)     

Transition of lasing modes in disordered active photonic crystals

The transition from a photonic band-edge laser to a random laser in two-dimensional active photonic crystals is described. The lasing modes in the active photonic crystals shift from the edge of the photonic bandgap to the bulk of the gap when a certain amount of position and size disorder is introduced. The shift of lasing modes is determined with various gain profiles. The results show that the modulation of lasing modes is significant when the lasing transition wavelength overlaps the photonic bandgap.     

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     

Fluorescence and amplified spontaneous emission of glass forming compounds containing styryl-4H-pyran-4-ylidene fragment

Potential of glassy films of newly synthesised low molecular weight organic molecules for light amplification and lasing applications has been investigated by analysing fluorescence, transient differential absorption and amplified spontaneous emission properties. These non-symmetric and symmetric molecules contain styryl-4H-pyran-4-ylidene fragment with three different electron acceptor groups: dicyanomethylene, barbituric acid, indene-1,3-dione. Fluorescence quantum yields of the investigated compounds in solutions are between 0.32 and 0.54, while they drop down by an order of magnitude in thin solid films. Incorporation of bulky side groups reduced excitonic interactions enabling manifestation of amplified spontaneous emission in the neat films of the investigated derivatives.