Amplified Spontaneous Emission Wavelength Research Articles

End Cap Effect on Solution-Processable Deep Blue Lasing Materials with Low-Amplified Spontaneous Emission Thresholds.

Organic lasers have attracted increasing attention owing to their superior characteristics such as lightweight, low-cost manufacturing, high mechanical flexibility, and high emission-wavelength tunability. Recent breakthroughs include electrically pumped organic laser diodes and an electrically driven organic laser, integrated with an organic light-emitting diode pumping. However, the availability of efficient deep blue organic laser chromophores remains limited. In this study, we develop two novel rigid oligophenylenes, end-capped with carbazole and phenylcarbazole groups, to demonstrate exceptional optical and amplified spontaneous emission (ASE) properties. These oligophenylenes are not only solution processable but also exhibit remarkably high solution photoluminescence quantum yields (PLQYs) of 90% and high radiative rates of 1.35 × 109 s-1 in the deep blue range. Our theoretical calculations confirm that the carbazole and phenylcarbazole end groups play a pivotal role in enhancing the optical transitions of the oligophenylene laser chromophores, thereby elevating their emission oscillator strengths. Remarkably, these materials demonstrate low solid-state ASE threshold values of 1.0 and 1.5 μJ/cm2 (at 431 and 418 nm, respectively). To the best of our knowledge, these ASE thresholds represent the lowest reported at these specific ASE wavelengths in the literature, regardless of whether they are solution-processed or thermally evaporated films. Furthermore, they exhibit excellent thermal and photostability, low triplet quantum yields, as well as negligible overlap of excited-state absorption within the ASE emission region, making them excellent candidates for a new class of deep blue materials for organic lasers. By integrating insights from theoretical calculations and experimental validation, our study provides a comprehensive understanding of the design principles behind these high-performing organic laser chromophores, paving the way for the development of advanced organic lasers with enhanced performance characteristics.

Polymer optical fiber amplifier based on all-inorganic perovskite quantum dots

The proliferation of polymer optical fibers (POFs) has opened multiple avenues of optical-based networks and sensing applications in the visible spectral range. However, the lack of efficient amplifiers significantly hinders their utilization in practical scenarios. As emerging gain media, halide perovskites have attracted considerable attention in exploring their practical applications. In this Letter, we investigated the optical gain properties of cesium lead bromide quantum dots (CsPbBr3 QDs), and by facet dip-coating, we realized a polymer optical fiber amplifier. Under a 400-nm, 163-fs Ti:Sapphire laser pumping, the amplified spontaneous emission (ASE) thresholds of 1.6 and 20.1 μJ/cm2 were achieved through stripe pumping of a QDs-thin-film and end-pumping of a polymer-fiber facet dip-coated with the QDs, respectively. A gain coefficient of 232.2 ± 22.8 cm−1 was obtained using the variable stripe length method. By coupling a broadband continuous-wave light source into the POF as the signal, the optical gain behavior was studied with varying pump fluence and signal power density. More than 20 dB optical gain was achieved within the ASE wavelength region of 530–540 nm with a predicted theoretical maximum gain of 33.6 dB. The research verifies the feasibility of amplifying continuous-wave signals in the visible spectrum and potentially closing the research gap in visible-light optical-to-optical amplifiers. This opens the avenue for further research and innovations in practical polymer-based optical amplification for a plethora of applications, including all optical processing chips and short-range interconnects, as well as visible-light and underwater communications.

Propagation loss in polyfluorene waveguides due to nanometer-roughness at their interfaces, studied by amplified spontaneous emission measurements

The propagation loss in single-mode asymmetric waveguides due to interface nanometer-roughness was studied using amplified spontaneous emission (ASE) measurements. Poly(9,9-dioctylfluorene) (F8) was used as the organic gain medium and the structure of the asymmetric waveguide was quartz glass substrate/F8/air. The propagation loss was measured at the ASE wavelength (447 nm) of amorphous F8, and the surface roughness of the substrate and F8 was measured using an atomic force microscope. The propagation losses of F8 waveguides with different F8 slab thicknesses were in good agreement with those calculated using an analytical expression for single-mode asymmetric waveguides with nanometer-roughness interfaces. The results presented herein will be useful for the design of high-performance organic lasers and organic optoelectronic integration systems.

Linearly Manipulating Color Emission via Anion Exchange Technology for High Performance Amplified Spontaneous Emission of Perovskites.

The most attractive advantages of all-inorganic cesium lead halide perovskites are their optical gain over broad spectral ranges through the visible spectrum, so are well suited to use in tunable lasers or broadband amplifiers. Most reported anion exchange reactions face a challenge to achieve the desired halogen-variable perovskites due to rapid and uncontrollable reactions and difficulty to synthesize directly. In this study, a simple vapor/solid anion exchange strategy is demonstrated for controlling the reaction process and realizing a wide range tuning of band gap and amplified spontaneous emission (ASE) wavelength, which exhibits a temperature-dependent anion exchange rate. By optimizing the reaction temperature at 90°C, the ASE wavelength can be linearly manipulated by just controlling the reaction time. A clear quantitative relationship between ASE peak position and reaction time is achieved. Compares with the CsPbClBr2 film obtained via the liquid phase anion exchange method, the fabricated perovskite films obtained by vapor/solid anion exchange technology exhibit superior film quality and enhanced ASE performance. This work may have applications in the future using facile and controllable techniques to develop high-quality full-color visible lasers.

Surface Passivation for Promotes Bi-Excitonic Amplified Spontaneous Emission in CsPb(Br/Cl)3 Perovskite at Room Temperature.

Perovskite-type lead halides exhibit promising performances in optoelectronic applications, for which lasers are one of the most promising applications. Although the bulk structure has some advantages, perovskite has additional advantages at the nanoscale owing to its high crystallinity given by a lower trap density. Although the nanoscale can produce efficient light emission, its comparatively poor chemical and colloidal stability limits further development of devices based on this material. Nevertheless, bulk perovskites are promising as optical amplifiers. There has been some developmental progress in the study of optical response and amplified spontaneous emission (ASE) as a benchmark for perovskite bulk phase laser applications. Therefore, to achieve high photoluminescence quantum yields (PLQYs) and large optical gains, material development is essential. One of the aspects in which these goals can be achieved is the incorporation of a bulk structure of high-quality crystallization films based on inorganic perovskite, such as cesium lead halide (CsPb(Br/Cl)3), in polymethyl methacrylate (PMMA) polymer and encapsulation with the optimal thickness of the polymer to achieve complete surface coverage, prevent degradation, surface states, and surface defects, and suppress emission at depth. Sequential evaporation of the perovskite precursors using a single-source thermal evaporation technique (TET) effectively deposited two layers. The PL and ASEs of the bare and modified films with a thickness of 400 nm PMMA were demonstrated. The encapsulation layer maintained the quantum yield of the perovskite layer in the air for more than two years while providing added optical gain compared to the bare film. Under a picosecond pulse laser, the PL wavelength of single excitons and ASE wavelength associated with the stimulated decay of bi-excitons were achieved. The two ASE bands were highly correlated and competed with each other; they were classified as exciton and bi-exciton recombination, respectively. According to the ASE results, bi-exciton emission could be observed in an ultrastable CsPb(Br/Cl)3 film modified by PMMA with a very low excitation energy density of 110 µJ/cm2. Compared with the bare film, the ASE threshold was lowered by approximately 5%. A bi-exciton has a binding energy (26.78 meV) smaller than the binding energy of the exciton (70.20 meV).

Dual Amplified Spontaneous Emission and Lasing from Nanographene Films.

Chemically synthesized zigzag-edged nanographenes (NG) have recently demonstrated great success as the active laser units in solution-processed organic distributed feedback (DFB) lasers. Here, we report the first observation of dual amplified spontaneous emission (ASE) from a large-size NG derivative (with 12 benzenoid rings) dispersed in a polystyrene film. ASE is observed simultaneously at the 685 and 739 nm wavelengths, which correspond to different transitions of the photoluminescence spectrum. Ultrafast pump-probe spectroscopy has been used to ascertain the underlying photophysical processes taking place in the films. DFB lasers, based on these materials and top-layer nanostructured polymeric resonators (i.e., one or two-dimensional surface relief gratings), have been fabricated and characterized. Lasers emitting close to either one of the two possible ASE wavelengths, or simultaneously at both of them, have been prepared by proper selection of the resonator parameters.

Kinetically Protected Carbon-Bridged Oligo(p-phenylenevinylene) Derivatives for Blue Color Amplified Spontaneous Emission

Abstract Carbon-bridged oligo(p-phenylenevinylene)s (COPVn with repeating unit n = 1–6) have demonstrated great success as laser dyes for thin-film organic lasers. The excellent photostability observed in the longer homologues is, however, not present in the blue-emitting shorter compounds COPV1 and COPV2, attributed to the unprotected terminal positions that can degrade by photoreaction in the excited state. Here we report the synthesis of various COPV1 and COPV2 derivatives functionalized at the terminal positions with two types of sterically bulky protecting substituents: Tip (2,4,6-triisopropylphenyl) and tert-butyl (t-Bu) groups. Such molecular designs aim at preventing such photodegradation processes and thus to improve their stability. The efficacy of kinetic isotope effect for stabilization is also examined for COPV2, by the addition at terminal positions of deuterium atoms. Absorption, photoluminescence (PL), including PL quantum yield, and amplified spontaneous emission (ASE) studies have been conducted in polystyrene films doped with each of the derivatives. Significant and slight improvements of the ASE photostability are observed for the compounds with Tip groups and deuterium, respectively. Installation of substituents slightly affects the ASE wavelength within the blue spectral region, that is 385–413 nm and 462–474 nm, for COPV1 and COPV2, respectively.

Charge Carrier Dynamics and Broad Wavelength Tunable Amplified Spontaneous Emission in ZnxCd1-xSe Nanowires.

ZnxCd1-xSe is regarded as a promising semiconducting material for optoelectronic devices. However, the tunable amplified spontaneous emission (ASE) properties and corresponding charge carrier recombination dynamics in ZnxCd1-xSe (0 ≤ x ≤ 1) nanowires (NWs) remain poorly understood. Herein, the charge carrier dynamics and ASE properties in ZnxCd1-xSe NWs were systematically investigated. In these NWs, the one/two-photon pumped ASE wavelength across the entire visible spectrum (480-725 nm) can be easily tuned via compositional engineering. The ASE threshold is closely related to the absorption coefficient and PL lifetime. At room temperature, free-carrier recombination is dominated in the low fluence pumped PL process. The ASE behavior is determined by exciton recombination in the high pump fluence (>1018 cm-3) region. These findings uncover the origin of the tunable PL/ASE properties in ZnxCd1-xSe NWs and establish them as having practical application as a series of lasing gain materials.

Efficient Optical Gain from Near‐Infrared Polymer Lasers Based on Poly[N‐9′‐heptadecanyl‐2,7‐carbazole‐alt‐5,5‐(4′,7′‐di‐2‐thienyl‐2′,1′,3′‐benzothiadiazole)

AbstractState‐of‐the‐art near‐infrared lasers based on poly[N‐9′‐heptadecanyl‐2,7‐carbazole‐alt‐5,5‐(4′,7′‐di‐2‐thienyl‐2′,1′,3′‐benzothiadiazole)] (PCDTBT) and poly(9,9‐dioctylfluorene‐alt‐benzothiadiazole) (F8BT) blends are reported. Polymer light‐emitting diodes (PLEDs) based on PCDTBT/F8BT blends with 30 wt% PCDTBT content exhibit a maximum radiance of 64.3 W sr−1 m−2 and external quantum efficiency of 2.11% with Commission Internationale de L'Eclairage (CIE) coordinates (x = 0.69, y = 0.30). Using an optimal blend ratio of 15 wt% PCDTBT in F8BT, a maximum gain value of 28.2 cm−1 at 710 nm is achieved, a remarkable value given that PCDTBT is a low emissive polymer extensively employed as donor polymer in organic photovoltaics. The lowest amplified spontaneous emission (ASE) and laser thresholds exhibited by the blends are 590 nJ pulse−1 (21 µJ cm−2) and 63.1 nJ pulse−1 (201 µJ cm−2). Transient absorption spectroscopy confirms efficient Förster resonant energy transfer from F8BT to PCDTBT which, together with the large miscibility of PCDTBT in F8BT, enables PCDTBT emission enhancement and optical gain. Furthermore, a ternary blend system composed of F8BT, PCDTBT, and poly(3‐hexylthiophene) is demonstrated, in which the ASE wavelength can be tuned in a 60 nm range from 650 to 710 nm at a very low threshold level via control of the blend content ratio.

A Temperature-Tunable Thiophene Polymer Laser.

This paper reports a temperature-tunable conjugated polymer poly[3-(2-ethyl-isocyanato-octadecanyl)-thiophene] (TCP) laser working in superradiant (SR)—or amplified spontaneous emission (ASE)—mode. The absorption spectra indicated the aggregate (mostly dimer) formation upon increasing concentration and/or decreasing temperature. Amplified spontaneous emission (ASE) was observed at suitable concentration, temperature, and pump energy values. The efficiency of the ASE from the TCP polymer was improved by energy transfer from an oligomer 9,9,9′,9′,9″,9″-hexakis(octyl)-2,7′,2′,7″-trifluorene (HOTF). Moreover, the ASE wavelength can be tuned between 550 and 610 nm by changing the temperature of the solution from 60 to 10 °C. To the best of our knowledge, this is the first report of a high-power, temperature-tunable, and conjugated polymer laser.

Amplified Spontaneous Emission Based on 2D Ruddlesden–Popper Perovskites

Abstract2D Ruddlesden–Popper perovskites (RPPs) are a class of quantum‐well (QW) materials, composed of layered perovskite QWs encapsulated between two hydrophobic organic layers. Different from widely investigated 3D‐perovskites with free carriers at room temperature, 2D‐RPPs exhibit strongly bound electron–hole pairs (excitons) for high‐performance solar cells and light emitting diodes (LEDs). Herein, it is reported that self‐organized multiple QWs in 2D‐RPP thin films naturally form an energy cascade, which enables an ultrafast energy transfer process from higher energy‐bandgap QWs to lower energy‐bandgap QWs. Therefore, photoexcitations are concentrated on lower‐bandgap QWs, facilitating the build‐up of population inversion. Room‐temperature amplified spontaneous emission (ASE) from 2D‐RPP thin films is achieved at dramatically low thresholds, with gain coefficients as high as >300 cm−1, and stoichiometrically tunable ASE wavelengths from visible to near‐infrared spectral range (530–810 nm). In view of the high efficiency reported for LEDs, these solution‐processed 2D‐RPP thin films may hold the key to realize electrically driven lasers.

Low threshold Amplified Spontaneous Emission properties in deep blue of poly[(9,9-dioctylfluorene-2,7-dyil)-alt-p-phenylene] thin films

Amongst the different optoelectronic applications of conjugated polymers, the development of new active materials for optically pumped organic lasers is still an open question particularly in the blue-near UV spectral range. We investigate the emission properties of poly[(9,9-dioctylfluorene-2,7-dyil)- alt-p-phenylene] (PFP) neat films under nanosecond pump. We demonstrate that thanks to the introduction of a phenylene moiety between two fluorene units it is possible to obtain Amplified Spontaneous Emission (ASE) with a lower threshold and a blue shifted wavelength with respect to poly(9,9-dioctylfluorene) (PFO). We demonstrate efficient ASE with a minimum threshold as low as 23 μJcm−2 and a minimum ASE wavelength of 436 nm. A maximum net optical gain of about 26 cm−1 is measured at an excitation density of 0.23 mJcm−2. These results make the PFP a good active material for optically pumped deep blue organic lasers.

A highly sensitive chemosensor for solution based on organic semiconductor laser gain media

Laser has been widely applied in the scientific and engineering areas including communications, medical treatment, industry, and military due to its extremely strict monochromaticity, high coherence and high energy density. Organic laser based on solution processable polymer gain media has attracted considerable attention in various applications due to its easy fabrication, compact system and flexibility. At present, the chemosensors based on organic semiconductor laser have been widely developed. It has been reported to achieve solution monitoring by organic DFB (distributed feedback) laser. Although the method has its own advantages, there are still many operability and craftsmanship problems to be resolved. In this paper we introduce a new type of the real-time monitoring for various solution. The monitor is realized by using amplified spontaneous emission (ASE) from optically pumped organic semiconductor gain media. The gain media comprising blends of poly(9, 9-dioctylfluorene-co-benzothiadiazole) (F8BT) and poly(3-hexylthiophene) (P3HT) at a ratio of 15:85 wt.% is dissolved into toluene (25 mg/mL). Thin films (90 nm thickness) of P3HT/F8BT are obtained by spin coating (2000 rpm) from solution onto pre-cleaned quartz substrates. The P3HT/F8BT film demonstrates the absorption peak at 471 nm, the PL peak at 622 nm, and the ASE peak at 661 nm with FWHM (full-width-at-half-maximum) linewidth of ～ 10 nm under the stripe laser pumping. The thin films are, then, covered by droplet of solution to form planar waveguide structure with variable effective refractive index. Upon analyte binding, a change in refractive index at the P3HT/F8BT film surface results in a change in the effective refractive index of the planar waveguide and in turn induces shift of the ASE mode wavelength and variation of ASE threshold of the organic gain media. The changes in ASE wavelength and threshold can be monitored for sensing. The red shift of 4.5 nm in the ASE spectrum is from 661 to 665.5 nm and the threshold increases from 0.579 J/pulse to 1.447 J/pulse which can be detected with the concentration of sodium chloride increasing from 0 to 25 wt.% in pure water. Our experimental results show that this method is easy to detect the concentration grads of 1 wt.% sodium chloride solution. The measurement sensitivity of solution reaches 97.8 nm/RIU (refractive index unit), and accuracy reaches 141.9 nm/RIU. Furthermore, we demonstrate that the chemosensor could be used for detecting different kinds of solution in the same concentration. The ASE peak position and threshold display clearly different when the droplet 10 wt.% sodium, chloride solution and hydromel solution onto P3HT/F8BT film. Our study suggests that the organic gain media films have potentiality to be developed as a high sensitivity and high accuracy chemosensor to detect solution due to the high sensitivity of the ASE peak position and threshold to the refractive index of the solution.

Thickness dependence of amplified spontaneous emission in low-absorbing organic waveguides

The effect of varying film thickness (h) on the amplified spontaneous emission (ASE) properties of 0.5 wt.% perylenediimide-doped polystyrene waveguides is reported. The threshold dependence on h, not previously investigated in detail, is analyzed in terms of the film absorption and photoluminescence, the confinement of the fundamental waveguide mode (TE0), and the presence of high-order modes. For h<400 nm and down to 150 nm, the ASE wavelength blueshifts, while the linewidth and threshold increase. The detrimental ASE operation in very thin films is due to the low absorption as well as to the poor confinement of the TE0 mode.

Lasing from colloidal InP/ZnS quantum dots

High-quality InP/ZnS core-shell nanocrystal quantum dots (NQDs) were synthesized as a heavy-metal-free alternative to the gain media of cadmium-based colloidal nanoparticles. Upon UV excitation, amplified spontaneous emission (ASE) and optical gain were observed, for the first time, in close-packed InP/ZnS core-shell NQDs. The ASE wavelength can be selected by tailoring the nanocrystal size over a broad range of the spectrum. Moreover, the optical gain profile of InP/ZnS NQDs was matched to the second order feedback of holographic polymer-dispersed liquid crystal gratings, leading to the very first demonstration of an optically-pumped, nanocrystal laser based on InP/ZnS core-shell NQDs.

Amplified spontaneous emission in α-phase and β-phase polyfluorene waveguides

Amplified spontaneous emission (ASE) of α- and β-phase poly(9,9-dioctylfluorene) (F8) based waveguides has been studied and ASE wavelengths have been determined as 451 nm and 468 nm, respectively. β-phase waveguides are found to be with higher net gain and lower light propagation loss as compared to α-phase waveguides. Such important improvement of ASE properties, making β-phase waveguides superior over α-phase counterparts is shown to be achieved at the expense of higher refractive index and photoluminescence quantum efficiency of β-phase F8.

Propagation characteristics and wavelength tuning of amplified spontaneous emission from dye-doped polymer

The propagation characteristics of amplified spontaneous emission (ASE) through a rhodamine 6 G-doped polymethyl methacrylate freestanding film waveguide were studied. This was done by shifting the excitation stripe horizontally along a transversely pumped waveguide. By this method, we could tune the ASE wavelength. The maximum tunability thus obtained was approximately 18 nm with a pump stripe length of 6 mm.

Amplified spontaneous emission from fluorene-based copolymer wave guides

Amplified spontaneous emission (ASE) from optically pumped thin film wave guides of a fluorene-based copolymer, poly(2,7-(9,9-di- n-octylfluorene)-alt-(1,4-phenylene-((4-sec-butylphenyl)imino)-1,4-phenylene)) (TFB), which has a high hole mobility and a low ionization potential in comparison with those of fluorene-based copolymers, has been observed. The net gain spectra and the loss coefficient of TFB wave guides are measured as gain media for use in solid-state organic lasers. A maximum net gain of 15.5 cm −1 and a low loss coefficient of 12.1 cm −1 are obtained at the ASE wavelength of 459 nm.

Semiconducting polyfluorenes as materials for solid-state polymer lasers across the visible spectrum

We report a detailed study of the gain properties of three polyfluorenes: poly(9,9-dioctylfluorene- co-9,9-di(4-methoxyphenyl)fluorene (F8DP), poly(9,9-dioctylfluorene- co-benzothiadiazole) (F8BT), and a Dow proprietary copolymer, Dow Red F. The emission spectra of these conjugated polymers span the full visible spectrum from 400 to 800 nm. We observe amplified spontaneous emission (ASE) with peak wavelengths at 452, 576 and 685 nm for F8DP, F8BT and Red F, respectively. Low stimulated emission thresholds in the region of 0.1–0.45 μJ per pulse are demonstrated for planar asymmetric waveguides. Variable stripe length gain measurements at the peak ASE wavelengths show large net gains up to 66 cm −1. Very low loss coefficients, in the range of 3.2–14.8 cm −1, were also found.

Fluorene-based polymer gain media for solid-state laser emission across the full visible spectrum

We report a study of the optical gain properties of three polyfluorenes with chemically tuned emission characteristics that span 400–800 nm. We demonstrate low threshold light amplification in the blue, green, and red spectral ranges via amplified spontaneous emission (ASE) in optically pumped planar asymmetric waveguides. Gain and loss measurements at the peak ASE wavelengths show large net gains, 22⩽g⩽66 cm−1, and low losses, 15⩾α⩾3 cm−1. Our findings establish fluorene-based polymers as an attractive family of materials for use in tuneable solid-state lasers that emit at wavelengths across the whole visible spectrum.