Speckle-Free, Angle-Free, Cavity-Free White Laser with a High Color Rendering Index.

The freedom from efficiency droop motivates monochromatic lasers to progress in general lighting applications due to the demand for more efficient and sustainable light sources. Still, a white light based on monochromatic lasers with high lighting quality, such as a high color rendering ability, an angle-independent output, and a speckle-free illumination, has not yet been fabricated nor demonstrated. Random lasers, with the special mechanism caused by multiple scattering, the angle-free emission, and the uncomplicated fabrication processes, inspire us to investigate the feasibility of utilizing them in general lighting. In this work, a white random laser with a high color rendering index (CRI) value, regardless of pumping energy and observing direction, was performed and discussed. We also investigated the stability of white RL as its CIE chromaticity coordinates exhibit negligible differences with increasing pump energy density, retaining its high-CRI measurement. Also, it exhibits angle-independent emission while having a high color rendering ability. After passing through a scattering film, it generated no speckles compared to the conventional laser. We demonstrated the advances in white laser illumination, showing that a white random laser is promising to be applied for high-brightness illumination, biological-friendly lighting, accurate color selections, and medical sensing.

1337 nm Emission of a Nd3+-Doped TZA Glass Random Laser.

Random lasers have been studied using many materials, but only a couple have used glass matrices. Here, we present a study of zinc tellurite and aluminum oxide doped with different percentages of neodymium oxide (4 wt.%, 8 wt.%, and 16 wt.%) and demonstrate for the first time random laser action at 1337 nm. Laser emission was verified and the laser pulse's rise time and input-output power slope were obtained. A cavity composed of the sample's pump surface and an effective mirror formed by a second, parallel layer at the gain-loss boundary was probably the main lasing mechanism of this random laser system. The reason for the absence of emission at 1064 nm is thought to be a measured temperature rise in the samples' active volume.

Fabry-Perot Oscillation and Resonance Energy Transfer: Mechanism for Ultralow-Threshold Optically and Electrically Driven Random Laser in Quasi-2D Ruddlesden-Popper Perovskites.

The recently emerged metal-halide hybrid perovskite (MHP) possesses superb optoelectronic features, which have obtained great attention in solid-state lighting, photodetection, and photovoltaic applications. Because of its excellent external quantum efficiency, MHP has promising potential for the manifestation of ultralow threshold optically pumped laser. However, the demonstration of an electrically driven laser remains a challenge because of the vulnerable degradation of perovskite, limited exciton binding energy (Eb), intensity quenching, and efficiency drop by nonradiative recombinations. In this work, based on the paradigm of integration of Fabry-Perot (F-P) oscillation and resonance energy transfer, we observed an ultralow-threshold (∼250 µWcm-2) optically pumped random laser from moisture-insensitive mixed dimensional quasi-2D Ruddlesden-Popper phase perovskite microplates. Particularly, we demonstrated an electrically driven multimode laser with a threshold of ∼60 mAcm-2 from quasi-2D RPP by judicious combination of a perovskite/hole transport layer (HTL) and an electron transport layer (ETL) having suitable band alignment and thickness. Additionally, we showed the tunability of lasing modes and color by driving an external electric potential. Performing finite difference time domain (FDTD) simulations, we confirmed the presence of F-P feedback resonance, the light trapping effect at perovskite/ETL, and resonance energy transfer contributing to laser action. Our discovery of an electrically driven laser from MHP opens a useful avenue for developing future optoelectronics.

Perovskite Random Lasers, Process and Prospects.

Random lasers (RLs) are a kind of coherent light source with optical feedback based on disorder-induced multiple scattering effects instead of a specific cavity. The unique feedback mechanism makes RLs different from conventional lasers. They have the advantages of small volume, flexible shape, omnidirectional emission, etc., and have broad application prospects in the fields of laser illumination, speckle-free imaging, display, and sensing. Colloidal metal-halide perovskite nanomaterials are a hot research field in light sources. They have been considered as desired gain media owing to their superior properties, such as high photoluminescence, tunable emission wavelengths, and easy fabrication processes. In this review, we summarize the research progress of RLs based on perovskite nanomaterials. We first present the evolution of the RLs based on the perovskite quantum dots (QDs) and perovskite films. The fabrication process of perovskite nano-/microstructures and lasers is discussed in detail. After that, the frontier applications of perovskite RLs are discussed. Finally, the challenges are discussed, and the prospects for further development are proposed.

Review of Open Cavity Random Lasers as Laser-Based Sensors.

In this review, the concept of open cavity lasing for ultrasensitive sensing is explored, specifically in driving important innovations as laser-based biosensors─a field mostly dominated by fluorescence-based sensing. Laser-based sensing exhibits higher signal amplification and lower signal-to-noise ratio due to narrow emission lines as well as high sensitivity due to nonlinear components. The versatility of open cavity random lasers for probing analytes directly which is ultrasensitive to small changes in chemical composition and temperature fluctuations paves the path of utilizing narrow emission lines for advanced sensing. The concept of random lasing is first explained followed by a comparison of the different lasing threshold that has been reported. This is followed by a survey of reports on laser-based sensing and more specifically as biosensors. Finally, a perspective on the way forward for open cavity laser-based sensing is put forth.

Plasmonically Enhanced Colloidal Quantum Dot/Graphene Doped Polymer Random Lasers.

An improvement in random lasers based on a colloidal quantum dot (QD)/graphene-doped polymer was observed and attributed to multiple light-scattering and graphene surface plasmon resonance. The emission characteristics of quantum dots doped with graphene oxide and reduced graphene oxide were compared. The QD/reduced graphene oxide hybrid exhibited a lower laser emission threshold (~460 µJ/cm2). The emission modes and thresholds were strongly dependent on both the graphene doping concentration and the external temperature. Decreased plasmon coupling was the primary reason for lower QD/graphene laser emission with increasing temperature. The optimum reduced graphene oxide concentration was 0.2 wt.%. This work provides a practical approach to optimizing the threshold and stability of random laser devices, with potential applications in displays, sensors, and anti-counterfeiting labels.

Direct Measurement of the Reduced Scattering Coefficient by a Calibrated Random Laser Sensor.

The research in optical sensors has been largely encouraged by the demand for low-cost and less or non-invasive new detection strategies. The invention of the random laser has opened a new frontier in optics, providing also the opportunity to explore new possibilities in the field of sensing, besides several different and peculiar phenomena. The main advantage in exploiting the physical principle of the random laser in optical sensors is due to the presence of the stimulated emission mechanism, which allows amplification and spectral modification of the signal. Here, we present a step forward in the exploitation of this optical phenomenon by a revisitation of a previous experimental setup, as well as the measurement method, in particular to mitigate the instability of the results due to shot-to-shot pump energy fluctuations. In particular, the main novelties of the setup are the use of optical fibers, a reference sensor, and a peristaltic pump. These improvements are devoted to: eliminating optical beam alignment issues; improving portability; mitigating the variation in pump energy and gain medium performances over time; realizing an easy and rapid change of the sensed medium. The results showed that such a setup can be considered a prototype for a portable device for directly measuring the scattering of liquid samples, without resorting to complicated numerical or analytic inversion procedures of the measured data, once the suitable calibration of the system is performed.

Stability-Enhanced Emission Based on Biophotonic Crystals in Liquid Crystal Random Lasers.

A new design of a bio-random laser based on a butterfly wing structure and ITO glass is proposed in this article. Firstly, the butterfly wing structure was integrated in a liquid crystal cell made of ITO glass. The integrated liquid crystal cell was injected with liquid crystal and dye to obtain a bio-random laser. A non-biological random laser was obtained with a capillary glass tube, liquid crystal and dye. The excitation spectra and thresholds were recorded to evaluate the performance of the biological and non-biological random lasers. The results show that the excitation performance stability of the bio-random laser is improved and the number of spikes in the spectra is reduced compared with the non-biological random laser. Finally, the equivalent cavity length of the biological and non-biological random lasers was compared and the optical field distribution inside the butterfly wing structure was analyzed. The data show that the improvement of the excitation performance stability of the bio-random laser is related to the localization of the optical field induced by the photonic crystal structure in the butterfly wing.

Tailoring the Random Lasing Properties by Controlled Phase Separation Process in PMMA:PVK Dye-Doped Polymeric Blends.

This article describes the random lasing (RL) phenomenon obtained in a dye-doped, polymeric double-phase system composed of PMMA and PVK polymers. It shows how relative concentrations between mentioned macromolecules can influence lasing parameters of the resulting blends, including obtained emission spectra and threshold conditions. We describe the influence of lasers' composition on their morphologies and link them with particular RL properties. Our studies reveal that the disorder caused by phase separation can support the RL phenomenon both in the waveguiding and quasi-waveguiding regimes. Changing the relative concentration of polymers enables one to switch between both regimes, which significantly influences threshold conditions, spectral shift, number of lasing modes, and ability to support extended and/or localized modes. Finally, we show that a simple phase separation technique can be used to fabricate efficient materials for RL. Moreover, it enables the tailoring of lasing properties of materials in a relatively wide range at the stage of the laser material fabrication process in a simple way. Therefore, this technique can be seen as a fast, cheap, and easy to perform way of random lasers fabrication.

Large-Area Biocompatible Random Laser for Wearable Applications.

Recently, wearable sensor technology has drawn attention to many health-related appliances due to its varied existing optical, electrical, and mechanical applications. Similarly, we have designed a simple and cheap lift-off fabrication technique for the realization of large-area biocompatible random lasers to customize wearable sensors. A large-area random microcavity comprises a matrix element polymethyl methacrylate (PMMA) in which rhodamine B (RhB, which acts as a gain medium) and gold nanorods (Au NRs, which offer plasmonic feedback) are incorporated via a spin-coating technique. In regards to the respective random lasing device residing on a heterogenous film (area > 100 cm2), upon optical excitation, coherent random lasing with a narrow linewidth (~0.4 nm) at a low threshold (~23 µJ/cm2 per pulse) was successfully attained. Here, we maneuvered the mechanical flexibility of the device to modify the spacing between the feedback agents (Au NRs), which tuned the average wavelength from 612.6 to 624 nm under bending while being a recoverable process. Moreover, the flexible film can potentially be used on human skin such as the finger to serve as a motion and relative-humidity sensor. This work demonstrates a designable and simple method to fabricate a large-area biocompatible random laser for wearable sensing.

Perovskite random lasers: a tunable coherent light source for emerging applications.

Metal halide perovskites have attracted increasing attention due to their superior optical and electrical characteristics, flexible tunability, and easy fabrication processes. Apart from their unprecedented successes in photovoltaic devices, lasing action is the latest exploitation of the optoelectronic performance of perovskites. Among the substantial body of research on the configuration design and light emission quality of perovskite lasers, the random laser is a very interesting stimulated emission phenomenon with unique optical characteristics. In this review article, we first comprehensively overview the development of perovskite-based optoelectronic devices and then focus our discussion on random lasing performance. After an introduction to the historical development of versatile random lasers and perovskite random lasers, we summarize several synthesis methods and discuss their material configurations and stability in synthesized perovskite materials. Following this, a theoretical approach is provided to explain the random lasing mechanism in metal halide perovskites. Finally, we propose future applications of perovskite random lasers, presenting conclusions as well as future challenges, such as quality stability and toxicity reduction, of perovskite materials with regard to practical applications in this promising field.

Investigation of the Optical Properties of a Novel Class of Quinoline Derivatives and Their Random Laser Properties Using ZnO Nanoparticles.

Quinoline Schiff bases display potential applications in optoelectronics and laser fields because of their unique optical properties that arise from extensive delocalization of the electron cloud, and a high order of non-linearity. In this context, a new class of conjugated quinoline-derivative viz. N-(quinolin-3-ylmethylene)anilines were synthesized from 2-hydroxyquinoline-3-carbaldehyde in two good yielding steps. The ability of these imines to accept an electron from a donor is denoted by their electron acceptor number and sites, which is calculated using density functional theory (DFT). The optical properties such as FT-IR, Raman, UV-VIS, and EDS spectra were calculated using TD-DFT, which also provided the energy gap, HOMO-LUMO structure. The optical properties of the synthesized imino quinolines were experimentally studied using photoluminescence and absorption spectroscopy. The properties such as Stokes shift and quantum yield were calculated using experimental data. Furthermore, the compound bearing a methyl group on the aryl ring and ZnO nanoparticles (hydrothermally synthesized) were dissolved in toluene, and optically excited with a 355 nm nanosecond laser, which produced a random laser.

Anderson Localization Enabled Spectrally Stable Deep-Ultraviolet Laser Based on Metallic Nanoparticle Decorated AlGaN Multiple Quantum Wells.

Random lasers exhibit many exotic properties, including chaotic behavior, light localization, broad angular emission, and cost-effective fabrication, which enable them to attract both scientific and industrial interests. However, before the realization of their potential applications, several challenges still remain including the underlying mechanism and controllability due to their inherent multidirectional and chaotic fluctuations. Through more than two decades of collaborative efforts, the discovery of Anderson localization in random lasers provides a plausible route to resolve the difficulties, which enables one to tailor the number of lasing modes and stabilize the emission spectra. However, the related studies are rather rare and only restricted to limited wavelengths. In this study, based on enhanced Anderson localization assisted by surface plasmon resonance, spectrally stable deep-ultraviolet lasing action in AlGaN multiple quantum wells (MQWs) is demonstrated. Our work serves as firm evidence to demonstrate the underlying mechanism of stabilized deep-ultraviolet random laser action that multiple scattering of a light beam in a disordered medium can induce Anderson localization similar to electron behavior. This feature covers the whole spectral range, and it is a universal phenomenon of an electromagnetic wave. Notably, stabilized deep-ultraviolet random laser action has not been demonstrated in all previous studies, even though it has great academic interest and potential application in many areas from environmental protection to biomedical engineering.

Advances in Random Fiber Lasers and Their Sensing Application.

Compared with conventional laser, random laser (RL) has no resonant cavity, reducing the requirement of cavity design. In recent years, the random fiber laser (RFL), a novel kind of RL, has made great progress in theories and experiments. The RFL has a simpler structure, a more flexible design, and higher reliability. It has valuable applications for earth sciences, biological life sciences, and national defense security, due to these unique properties. This paper reviews the development of RFLs in the last decade, including their configurations based on various optical fibers and their output properties, especially the method of control. Moreover, we also introduce their applications in the optical fiber sensing system, which is a very important and practical orientation to study. Finally, this paper presents the prospects of RFLs.

Multifunctional Random-Laser Smart Inks.

With the superiority of laser-level intensity, narrow spectral line width, and broad-angular emission, random lasers (RLs) have drawn considerable research interests for their potential to carry out a variety of applications. In this work, the applications associated with optical-encoded technologies, including security printing, military friend or foe identification (FFI), and anticounterfeiting of documents are highlighted, and the concept of a transient RL "smart ink" has been proposed. The proof-of-concept was demonstrated as invisible signatures, which encoded the messages through the spectral difference of spontaneous emission and RL under specified conditions. Next, the possibility of encoding the data with multibit signals was further confirmed by exploiting the threshold tunability of RLs. Moreover, the transient characteristic of this smart ink and its capability to be attached on freeform surfaces of different materials were also shown. With the advantages of a facile manufacturing process and multiple purposes, it is expected that this ink can soon be carried out in a variety of practical utilities.

Grain Boundary Induced Ultralow Threshold Random Laser in a Single GaTe Flake.

Random lasing is a lasing phenomenon realized in random media, and it has attracted a great deal of attention in recent years. An essential requirement for strong random lasing is to achieve strong and recurrent scattering among grain boundaries of a disordered structure. Herein, we report a random laser (RL) based on individual polycrystalline GaTe microflakes (MFs) with a lasing threshold of 4.15 kW cm-2, about 1-2 orders of magnitude lower than that of the reported single GaN microwire random laser. The strongly enhanced light scattering and trapping benefit from the reduced grain size in the polycrystalline GaTe MF, resulting in a ultralow threshold. We also investigate the dependence of spatially localized cavities' dimension on the pumping intensity profile and temperature. The findings provide a feasible route to realize RL with a low threshold and small size, opening up a new avenue in fulfilling many potential optoelectronic applications of RL.

Tailoring Whispering Gallery Lasing and Random Lasing in A Compound Cavity.

A compound cavity was proposed to achieve both whispering gallery mode (WGM) lasing and random lasing. The WGM-random compound cavity consisted of a random structure with an annular boundary, which was fabricated by a method combining both inkjet printing and metal-assisted chemical etching methods. An ultrathin polymer membrane was attached to the WGM-random compound cavity, forming a polymer laser device. A transformation from WGM lasing to random lasing was observed under optical pumping conditions. The laser performance could be easily tailored by changing the parameter of the WGM-random compound cavity. These results provide a new avenue for the design of integrated light sources for sensing applications.

Lotus-Leaf-Inspired Flexible and Tunable Random Laser.

We describe herein a flexible and tunable random laser made from a flexible poly(dimethylsiloxane) substrate. The substrate is prepared by casting via soft lithography from a lotus leaf to produce a micropapilla surface structure similar to that of a lotus leaf. The micropapilla provides efficient multiple scattering for the photons generated in the gain medium, and random lasing emerges because photons undergo closed-loop paths by scattering from three equilaterally arranged micropapillae. Given the diverse distribution of microscale features on the soft substrate, the random laser spectrum can be tuned by as much as 26.0 nm by changing the pump position. Furthermore, the random laser can be easily tuned by about 14 nm by flexing it, which modifies the micropapilla density and thereby changes the reabsorption strength of the laser dye. The photostability of the random laser is ensured by sealing the gain medium (i.e., dye solution) in a closed system. The results provide a promising method to realize a variety of laser-based applications such as optical biosensors on chips, microscale structural alteration detectors, flexible wearable devices, and multicolor (even white) random lasers.

A corona modulation device structure and mechanism based on perovskite quantum dots random laser pumped using an electron beam.

Although laser pumping using electroN beam (EB) has high transient power output and easy modulation based on perovskite quantum dot (PQD) film, its lasing emitting direction is the same as the pumped EB's direction. Thus, realizing the conventional direct device structure through the film lasing mechanism is extremely difficult. Therefore, using the random lasing principle, herein, we proposed a corona modulation device structure based on PQDs random laser pumped using an EB. We discussed and stimulated the optimized designed method of the device in terms of parameters of the electronic optical device and the utilization ratio of output power and its modulation extinction ratio, respectively. According to the simulation results, this type of device structure can effectively satisfy the new random lasing mechanism in terms of high-speed and high-power modulation.

Surface-Emitting Perovskite Random Lasers for Speckle-Free Imaging.

Random lasers have been ideal illumination sources for speckle-free and high-speed imaging. Despite their successes, the real applications of random lasers are facing a long-standing challenge, i.e., the cumbersome size of the illuminating system. Herein, we demonstrate perovskite-based surface emitting random lasers (SERLs) and explore their applications in speckle-free imaging. The random lasers are generated by multiple scattering in a perovskite polycrystalline film sandwiched by two distributed Bragg reflectors. Owing to the tight confinement in vertical direction and large number of random resonances, the wavevectors of random lasers are dominated by their vertical components, and thus, multimode SERLs with a divergence angle of ∼3-5° and low spatial coherence are produced. By directly illuminating the patterns with the SERLs, the notable speckle noises of conventional optical images have been dramatically suppressed. This research shall provide a strategy toward the integrated spectral-free imaging systems.