Thin film organic lasers represent a new generation of inexpensive, mechanically flexible devices for spectroscopy, optical communications and sensing. For this purpose, it is desired to develop highly efficient, stable, wavelength-tunable and solution-processable organic laser materials. Here we report that carbon-bridged oligo(p-phenylenevinylene)s serve as optimal materials combining all these properties simultaneously at the level required for applications by demonstrating amplified spontaneous emission and distributed feedback laser devices. A series of six compounds, with the repeating unit from 1 to 6, doped into polystyrene films undergo amplified spontaneous emission from 385 to 585 nm with remarkably low threshold and high net gain coefficients, as well as high photostability. The fabricated lasers show narrow linewidth (<0.13 nm) single mode emission at very low thresholds (0.7 kW cm−2), long operational lifetimes (>105 pump pulses for oligomers with three to six repeating units) and wavelength tunability across the visible spectrum (408–591 nm).

The aim of this work was to improve the laser performance, in terms of threshold and operational lifetime, of lasers based on polymer films doped with perylenediimide (PDI) derivatives as active media. For such purpose, we first investigated the amplified spontaneous emission (ASE) properties of perylene orange (PDI-O), when doped into polystyrene (PS) films. Lower ASE thresholds and larger photostabilities than those of similar films containing another PDI derivative (PDI-C6), recently reported in the literature, have been measured. Results have been interpreted in terms of the photoluminescence efficiency of the films, which depends on the type of 10 molecular arrangement, inferred with the help of nuclear magnetic resonance experiments. We also show that PS films have a better ASE performance, i.e. lower thresholds and larger photostabilities, than those based on poly(methyl methacrylate), which was recently highlighted as one of the best matrixes for PDI-O. Finally, a 1D second-order distributed feedaback laser using PS doped with PDI-O, was fabricated and characterized. This device has shown a threshold significantly lower (by around one order of magnitude) than that of a similar laser based on PDI-C6-doped PS.15

The aim of this work was to design strategies to improve the performance of solid-state lasers and amplifiers based on perylenediimide (PDI) derivatives as active materials. So, the effect of different types of modifications of the chemical structure of PDIs in their spectral, electrochemical, and laser properties in both solution and PDI-doped polystyrene films at various concentrations has been investigated. In particular, we focused on controlling the wavelength of emission in order to tune the laser wavelength as well as in increasing the amount of PDI in the films in order to decrease the laser thresholds, while keeping a good photostability. Three types of modifications of the chemical structure were investigated: (a) symmetrical substitution at the imide nitrogen positions (PDI 1); (b) substitution at the bay positions in the PDI core (PDI 4); and (c) modification in the dicarboximide group (PDI 5). All three derivatives were soluble and showed good n-type acceptor ability. Routes b and c led to red shifts in the absorption and photoluminescence (PL) emission, although the PL quantum yield decreased considerably. Amplified spontaneous emission (ASE) was observed in films doped with PDI 1 (λ ) 579 nm) and PDI 4 (λ ) 599 nm). The best performance, with an ASE threshold of 15 kW/cm 2 and a photostability halflife of 31 × 10 3 pump pulses, was obtained for films doped with 0.75 wt % of PDI 1 (route 1). PDI 1-based materials are among the most photostable reported in the literature and show very-reasonable thresholds. Moreover, these materials are particularly interesting in the field of data communications based on polymer optical fibers because they emit at wavelengths close to 570 nm, which constitutes the second low-loss transmission window in poly(methyl methacrylate).

We report on the preparation and characterization, under optical pump, of second-order one-dimensional distributed feedback (DFB) lasers based on polystyrene films doped with a perylenediimide derivative, as active media. The DFB gratings were engraved on the substrates (SiO2) by thermal nanoimprint lithography, followed by reactive ion etching. Laser emission wavelength was tuned from 554 to 583 nm by changing film thickness (h) between 240 and 1200 nm. The effect on the performance (emission wavelength, threshold, slope efficiency, number of modes, and spectral shape) of varying the grating depth (d) from 30 to 240 nm, for the whole range of h values, has been investigated. Although there is extensive work in the literature aiming to tune the emission wavelength of organic DFB lasers by h variation, the effect of changing d systematically has not been previously studied. Experimental results have been interpreted by models that take into account the presence of the grating by averaging either h or the effective refractive index. Single-mode emission (λ0) was observed for h &lt; 1000 nm, while for thicker films lasing appeared at two different wavelengths (λ0 and λ1). Models indicate that λ0 and λ1 correspond to the TE0 and TE1 waveguide modes, respectively. It was found that d plays an important role in determining the DFB thresholds and slope efficiencies for two h regimes: (i) For h &lt; 350 nm, lowest thresholds and highest slopes efficiencies were obtained with the shallower gratings; and (ii) for h &gt; 1000 nm, d affects significantly the losses associated with the TE1 mode, so single mode emission was achieved at λ0 or at λ1 for deep and shallow gratings, respectively. Finally, the shape of the emission spectra, both below and above threshold, has also been analyzed in order to clarify the physical mechanisms responsible for the existence of gain. Bragg dips were observed in the spectra below threshold only for devices with d/h larger than around 0.3 and their width increased with increasing d/h. In these cases, single-mode DFB emission appeared at the long-wavelength edge of the Bragg dip, indicating that index-coupling modulation contributes significantly to the gain process. On the other hand, for smaller d/h values, Bragg dips became too small to be detected, so gain coupling becomes the dominant mechanism accounting for the presence of gain.