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

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 < 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 < 350 nm, lowest thresholds and highest slopes efficiencies were obtained with the shallower gratings; and (ii) for h > 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.

An efficient, low-cost, and highly photostable second-order distributed feedback ͑DFB͒ laser, fabricated by thermal nanoimprint lithography and based on a polymer active film containing a perylenediimide derivative, is reported. It shows a photostability half-life of 3.1ϫ 10 5 pump pulses ͑Ͼ8h ͒, when pumped at the same spot of the film. This value is the highest reported to date for organic DFB lasers measured under ambient conditions. The device emits at 573 nm, matching the second low-loss transmission window of poly͑methylmethacrylate͒͑ 460-590 nm͒, thus offering potential for applications in data communications based on polymer optical fibers.

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