Luis Cerdán

Amplified spontaneous emission and optical gain measurements from pyrromethene 567--doped polymer waveguides and quasi-waveguides.

Amplified spontaneous emission from planar waveguides and quasi-waveguides based on Pyrromethene 567-doped poly(methyl methacrylate) thin films deposited onto quartz and glass substrates is investigated. Films with different thickness were prepared and pumped optically at 532 nm with pulses of up to 8 MW/cm(2). Pump thresholds for the onset of ASE emission, optical gains and losses were assessed. Net gain coefficients were estimated by fitting the data provided by variable stripe length measurements with a theoretical expression which takes into account saturation. In this way, net gain coefficients of up to 56 +/- 9 cm(-1) at a pump intensity of 5.3 MW/cm(2) for quasi-waveguides and up to 20.6 +/- 2.7 cm(-1) at a pump intensity of 3.4 MW/cm2 for waveguides, were obtained. Loss coefficients in the waveguides were estimated to be 3.8 +/- 0.4 cm-1 and 6.1 +/- 1.3 cm(-1) for 15 microm and 5 microm thick films, respectively. The results obtained seem to indicate a stronger self-mode-restriction capability in the quasiwaveguides than in conventional total internal-reflection waveguides.

First Highly Efficient and Photostable E and C Derivatives of 4,4‐Difluoro‐4‐bora‐3a,4a‐diaza‐s‐indacene (BODIPY) as Dye Lasers in the Liquid Phase, Thin Films, and Solid‐State Rods

A new library of E- and C-4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (BODIPY) derivatives has been synthesized through a straightforward protocol from commercially available BODIPY complexes, and a systematic study of the photophysical properties and laser behavior related to the electronic properties of the B-substituent group (alkynyl, cyano, vinyl, aryl, and alkyl) has been carried out. The replacement of fluorine atoms by electron-withdrawing groups enhances the fluorescence response of the dye, whereas electron-donor groups diminish the fluorescence efficiency. As a consequence, these compounds exhibit enhanced laser action with respect to their parent dyes, both in liquid solution and in the solid phase, with lasing efficiencies under transversal pumping up to 73 % in liquid solution and 53 % in a solid matrix. The new dyes also showed enhanced photostability. In a solid matrix, the derivative of commercial dye PM597 that incorporated cyano groups at the boron center exhibited a very high lasing stability, with the laser emission remaining at the initial level after 100 000 pump pulses in the same position of the sample at a 10 Hz repetition rate. Distributed feedback laser emission was demonstrated with organic films that incorporated parent dye PM597 and its cyano derivative. The films were deposited onto quartz substrates engraved with appropriate periodical structures. The C derivative exhibited a laser threshold lower than that of the parent dye as well as lasing intensities up to three orders of magnitude higher.

New perylene-doped polymeric thin films for efficient and long-lasting lasers

We establish an efficient strategy to optimize the performance of dye-doped host materials consisting of analyzing in a systematic way the dependence of their Amplified Spontaneous Emission (ASE) efficiency and photostability on the composition and structure of the matrices, selected to specifically avoid the thermal and/or chemical (photooxidation) processes, main mechanisms of dye photodegradation. For this study, a number of experimental polyimides have been chosen as a host matrix and their behavior has been compared with that of poly(methyl methacrylate) (PMMA). We correlate the optical properties with the oxygen permeation and thermal properties of the different polymeric hosts doped with perylene dyes to deepen the understanding of the photodegradation mechanism predominant in these dyes and to minimize its influence. We demonstrate high efficiency and photostable ASE from waveguides based on polymeric materials doped with Perylene Orange (PO), Perylene Red (PR), and mixtures of both. This enhancement in the optical properties allows reaching high gain and long-lasting distributed feedback (DFB) laser emission based on PO doped polymer matrices, even when operating in an unoptimised resonator.

Laser emission from mirrorless waveguides based on photosensitized polymers incorporating POSS

Laser emission from leaky waveguides based in dye-doped organic gain media incorporating Polyhedral Oligomeric Silsesquioxanes (POSS) nanoparticles is reported. The samples consist of thin film gain media deposited onto glass substrate defining a planar asymmetric slab waveguide, which does not incorporate any resonant substructure. The presence of POSS results in additional amplified spontaneous emission (ASE) spectral narrowing, and conditions have been found for which directional multimode laser emission is achieved. The spectral narrowing is ascribed to the photon path enlargement caused by a non-resonant feedback mechanism provided by individual scatterers, which enhances incoherently the magnitude of the amplification process. On the contrary, the appearance of multimode lasing is attributed to coherent random lasing from a many scatterers collective effect.

A borane laser

Emission from electronically excited species forms the basis for an important class of light sources-lasers. So far, commercially available solution-processed blue-emitting laser materials are based on organic compounds or semiconductor nanocrystals that have significant limitations: either low solubility, low chemical- and/or photo-stability and/or uncompetitive prices. Here we report a novel and competitive alternative to these existing laser materials that is based on boron hydrides, inorganic cluster compounds with a rich and diverse chemistry. We demonstrate that solutions of the borane anti-B18H22 show, under pulsed excitation, blue laser emission at 406 nm with an efficiency (ratio of output/input energies) of 9.5%, and a photostability superior to many of the commercially available state-of-the-art blue laser dyes. This demonstration opens the doors for the development of a whole new class of laser materials based on a previously untapped resource for laser technology-the boranes.

Straightforward synthetic protocol for the introduction of stabilized c nucleophiles in the BODIPY core for advanced sensing and photonic applications

A straightforward synthetic protocol to directly incorporate stabilized 1,3-dicarbonyl C nucleophiles to the meso position of BODIPY (4,4-difluoro-4-bora-3a,4a-diaza-s-indacene) is reported. Soft nucleophiles generated by deprotonation of 1,3-dicarbonyl derivatives smoothly displace the 8-methylthio group from 8-(methylthio)BODIPY analogues in the presence of Cu(I) thiophenecarboxylate in stoichiometric amounts at room temperature. Seven highly fluorescent new derivatives are prepared with varying yields (20-92%) in short reaction times (5-30 min). The excellent photophysical properties of the new dyes allow focusing on applications never analyzed before for BODIPYs substituted with stabilized C nucleophiles such as pH sensors and lasers in liquid and solid state, highlighting the relevance of the synthetic protocol described in the present work. The attainment of these dyes, with strong UV absorption and highly efficient and stable laser emission in the green spectral region, concerns to one of the greatest challenges in the ongoing development of advanced photonic materials with relevant applications. In fact, organic dyes with emission in the green are the only ones that allow, by frequency-doubling processes, the generation of tunable ultraviolet (250-350 nm) radiation, with ultra-short pulses.

Chiral Organic Dyes Endowed with Circularly Polarized Laser Emission

The direct generation of efficient, tunable, and switchable circularly polarized laser emission (CPLE) would have far-reaching implications in photonics and material sciences. In this paper, we describe the first chiral simple organic molecules (SOMs) capable of simultaneously sustaining significant chemical robustness, high fluorescence quantum yields, and circularly polarized luminescence (CPL) ellipticity levels (|glum|) comparable to those of similar CPL-SOMs. All these parameters altogether enable efficient laser emission and CPLE with ellipticity levels 2 orders of magnitude stronger than the intrinsic CPL ones.

On the characteristic lengths in the variable stripe length method for optical gain measurements

Although the variable stripe length (VSL) method has been widely used to measure the optical gain in thin film active media, different nor totally rigorous criteria have yet been used to estimate two important characterization parameters, namely, threshold and saturation lengths, on which the method critically depends. Here we present a formalism which leads to analytical expressions to rigorously calculate these characteristic lengths from VSL data, providing a unique criterion for the estimation of the amplified spontaneous emission threshold and saturation points.

Laser Efficiency Enhancement Due to Non-Resonant Feedback in Dye-Doped Hybrid Materials: Theoretical Insights and Experiment

It has been recently shown that the presence of nanoscatterers up to a certain density, homogeneously distributed in gain media, instead of being detrimental to conventional two-mirror cavity laser efficiency and directionality, may result in an increase of the output energy due to an enlargement in the effective optical path. Here we present a theoretical model for the stimulated emission in very weak scattering active media and show that the aforementioned laser efficiency improvement owes to a contribution of non-resonant feedback due to Rayleigh scattering. The model reveals that a critical factor in the physics of the emission is the nanometric size of the scattering particles irrespective of their nature. Experiments are carried out and the results are shown to be in agreement with the predictions of the model.

Circularly polarized laser emission induced in isotropic and achiral dye systems

The production of efficient, tunable, and switchable circularly polarized laser emission would have far reaching implications in optical communications or biophotonics. In this work, it is demonstrated the direct generation of circularly polarized (CP) laser emission in achiral and isotropic dye laser systems without the use of extracavity polarizing elements, and without resorting to chiral dyes, chiral liquid crystal matrices, or interferometric methods. The origin of this ellipticity arises from the dynamic birefringence induced by the strong and polarized laser pumping and the subsequent orientation anisotropy of the excited molecular dipoles. A complete polarimetric characterization of the polarization state of conventional dye laser oscillators as a function of different experimental parameters is performed and it is shown that the generated light always possesses a certain level of circularity that changes in a distinctive way with pump energy and polarization. These results demonstrate that it is possible to generate and modulate CP laser light from efficient and photostable conventional laser dyes.