Organic laser sources offer the opportunity to integrate flexible and widely tunable lasers in polymer waveguide circuits, e.g. for Lab-on-Foil applications. Therefore, it is necessary to understand gain and degradation processes for long-term operation. In this paper we address the challenge of life-time (degradation) measurements of photoluminescence (PL) and optical gain in thin-film lasers. The well known guest-host system of aluminum-chelate Alq3 (Tris-(8-hydroxyquinoline)aluminum) as host material and the laser dye DCM2 (4-(Dicyanomethylene)-2- methyl-6-julolidyl-9-enyl-4H-pyran) as guest material is employed as laser active material. Sample layers have been built up by co-evaporation in an ultrahigh (UHV) vacuum chamber. 200nm thick films of Alq3:DCM2 with different doping concentrations have been processed onto glass and thermally oxidized silicon substrates. The gain measurements have been performed by the variable stripe length (VSL) method. This measurement technique allows to determine the thin-film waveguide gain and loss, respectively. For the measurements the samples were excited with UV irradiation (ƛ = 355nm) under nitrogen atmosphere by a passively Q-switched laser source. PL degradation measurements with regard to the optical gain have been done at laser threshold (approximately 3 μJ/cm2), five times above laser threshold and 10 times above laser threshold. A t50-PL lifetime of > 107 pulses could be measured at a maximum excitation energy density of 32 μJ/cm2. This allows for a detailed analysis of the gain degradation mechanism and therefore of the stimulated cross section. Depending on the DCM2 doping concentration C the stimulated cross section was reduced by 35 %. Nevertheless, the results emphasizes the necessity of the investigation of degradation processes in organic laser sources for long-term applications.
Harald Flügge, Alexander Rohr, Sebastian Döring, Charlotte Fléchon, Manuela Wallesch, Daniel Zink, Jochen Seeser, Jaime Leganés, Tatjana Sauer, Torsten Rabe, Wolfgang Kowalsky, Thomas Baumann, Daniel Volz
Phosphorescent OLEDs are now being used in first commercial products, mainly in displays. Typically, such devices
operate at low-to-moderate brightnes s (<500 cd m-2), while it would be beneficial for actual lighting applications to also
reach a very high luminance. However, a phenomenon called efficiency roll-off contradicts this aim. The reducing of the
device efficiency with rising triplet exciton concentration due to triplet-triplet annihilation (TTA) is the most relevant
factor causing roll-off for such compounds. Photophysically, this is reflected by strong concentration quenching in
concentrated samples of phosphorescent materials.
We present a potential solution for this issue. In this article we identify a copper(I) emitter showing thermally-activated
delayed fluorescence (TADF) that seems to be much more immune to concentration quenching than conventional
phosphorescent materials, even though triplet states are also populated in a similar manner.
Since organic laser materials offer broad optical gain spectra they are predestined for the realization of widely
tunable laser sources. Here we report on a compact organic laser device that allows for voltage controlled
continuously wavelength tuning in the visible range of the spectrum by external deformation. The device
consists of an elastomeric distributed feedback (DFB) laser and an electro-active elastomer actuator also
known as artificial muscle. Second order DFB lasing is realized by a grating line structured elastomer
substrate covered with a thin layer of dye doped polymer. To enable wavelength tuning the elastomer laser is
placed at the center of the electro-active elastomer actuator. Chosen design of the actuator gives rise to
homogeneous compression at this position. The voltage induced deformation of the artificial muscle is
transferred to the elastomer laser and results in a decrease of grating period. This leads to an emission
wavelength shift of the elastomer laser. The increase of actuation voltage to 3.25 kV decreased the emission
wavelength from 604 nm to 557 nm, a change of 47 nm or 7.8%.
Holographic surface relief gratings written in azobenzene containing films were studied for the use as masters for
polymeric thin film distributed feedback (DFB) lasers. Light induced mass transport driven by E-Z isomerization in
azobenzene containing materials have shown to be attractive for all optical and one-step fabrication of periodic surface
structures with varying parameters for different optical applications. Based on new azobenzene materials and their
holographic processing deep surface relief gratings were generated with grating pitches in the range of 400 nm as
resonant structures for second order DFB lasers emitting in the VIS range. Nanoimprint techniques enabled multiple
duplications of azobenzene master gratings in UV adhesives. The replicas were coated via spin casting with thin films of
red light emitting polymer layers to form DFB thin film lasers. These active layers are guest-host-systems consisting of
an UV-light absorbing conjugated polymer as host transferring its excitation via Förster resonant energy transfer to a red
emitting conjugated polymer. Simple adjustment of grating depth via controlling of illumination time allowed it to
investigate the influence of the corrugation depth and thereby the coupling of laser light and grating on the lasing
behavior of second order DFB lasers in the red region. For this purpose multiple surface structures with different
corrugation depths of up to 130 nm were generated holographically, duplicated and coated.
The development of organic thin film lasers has seen tremendous progress over the past few years. Only a few
materials are necessary to allow for continuous wavelength tunability in the spectral region from the UV to the
near IR. At the same time, the lasing thresholds of organic thin film lasers have been reduced considerably both
due to improved low-loss distributed feedback (DFB) resonator structures and highly efficient gain materials
based on guest-host energy transfer. Aside from the as yet open issue of electrical operation of organic lasers,
which we will address briefly in this paper, there are numerous applications (e.g. in biotechnology, spectroscopy)
where optically driven organic lasers may be the more cost effective and versatile solution. In this context, tunable
polymer lasers pumped by compact and inexpensive InGaN laser diodes will be shown. These lasers are based on a
modified poly(9,9'-dioctylfluorene) derivative (BN-PFO) containing 12% of -6,6'-(2,2'-octyloxy-1,1'-binaphthyl)
spacer groups doped with a few wt% of the stilbene dye 1,4-Bis(2-(4-(N,N-di(p-tolyl)amino)phenyl)vinyl-benzene
(DPAVB). With the same host polymer (BN-PFO) quasi continuous wave operation (up to 5 MHz) can be
demonstrated. Highly repetitive lasers are especially desirable for many spectroscopic applications. This regime
of operstion is found to be impeded by the photo-physics in doped organic systems where the accumulation of
absorptive species in the gain medium leads to piled-up absorption losses and consequently to termination of the
lasing process. The presence of the dopand molecules seems to strongly promote the formation and stabilization of
the species which we relate to triplet excitons. Therefore, the concentration of the dopand affects the feasibility of
quasi-cw operation of thin-film organic lasers. Strategies and results to achieve highly repetitive operation in low-threshold
guest-host systems BN-PFO:DPAVB or BN-PFO:poly[2-methoxy-5-(2'-ethylhexyloxy)-1,4-phenylene
vinylene] (MEH-PPV) will be presented.
At high current densities, the characteristics of organic laser diode structures are strongly influenced by a variety
of loss processes such as bimolecular annihilations, field-induced exciton dissociation and induced absorptions
due to polarons and triplet excitons. Here, we investigate a TE2-mode organic double-heterostructure laser diode
by numerical simulation. The electrical properties are described using a numerical drift-difusion model and the
optical characteristics are modeled using a transfer matrix method. When annihilation processes are included,
a threshold current density of 8.5 kA/cm2 is derived for the considered device. Laser operation is not achieved
when field-induced exciton dissociation is considered. For induced absorptions, maximum relative cross sections
of 9.6 × 10-8 for polarons and 1.4 × 10-4 for triplet excitons have been calculated, which would still allow laser
operation. For higher relative absorption cross sections, laser operation is suppressed for all current densities.
Furthermore, the impact of field quenching is analyzed and the separation of singlet excitons from polarons and
triplet excitons in the time domain is studied.
In this paper we investigate the optical gain in organic thin film waveguides using the variable stripe length
method (VSL). As active medium the guest-host system containing Tris-(8-hydroxy-chinolinato)-aluminium
(Alq3) doped by 10-(2-benzothiazolyl)-2,3,6,7-tetrahydro-1,1,7,7-tetramethyl-1H,5H,11H- (1)-benzopyropyrano-
(6,7-8-i,j)quinolizin-11-one (C545T) is studied. The doping concentration is varied over a wide range and the
gain coefficient is measured at different excitation densities to analyze the behavior of the differential gain. The
F¨orster energy transfer is responsible for the occupation of the exited state of the coumarin molecules. For
low doping concentrations with an inefficient host-guest energy transfer a low stimulated cross section can be
observed. At optimal doping concentrations (3.7-6.4 wt%) we obtain a cross section of σ =6.8x10-17 cm2 and a
high material gain of gmat ≈500 cm-1 at an excitation density Eex of Eex ≈300 μJ/cm2. A further increased
doping concentration (15 wt%) leads to a reduced cross section, due the onset of concentration quenching in
the guest-host system. Furthermore, at high excitation densities we observe a strong saturation effect of the
maximum gain which depends strongly on the doping concentration.
Compared to well established liquid based dye lasers, amplifying media based on amorphous organic thin films allow the realisation of versatile, cost effective and compact lasers. Aside from that, the materials involved are organic semiconductors, which in principle allow the fabrication of future electrically driven organic laser diodes. A highly promising, low-loss resonator geometry for these lasers is the distributed feedback (DFB) structure, which is based on a periodic modulation of the refractive index in the waveguide on the nanometer scale. By variation of the grating period Λ one may tune the laser emission within the gain spectrum of the amplifying medium. We will demonstrate organic lasers spanning the entire spectral region from 360-715 nm. Tuning ranges as large as 115 nm (λ = 598-713 nm) in the red spectral region and more than 30 nm (λ = 362-394 nm) in the UV render these novel lasers highly attractive for various spectroscopic applications. As the grating period Λ is typically between 100 nm and 400 nm the DFB resonators are fabricated by e-beam lithography. These gratings may, however, be used as masters to obtain an arbitrary amount of copies by nanoimprint lithography into plastic substrates. Therefore these lasers are very attractive even for single-use applications (e.g. in medicine and biotechnology). Today, the key challenge in the field is the realisation of the first electrically driven organic laser. Key pre-requisites are highly efficient amplifying material systems which allow for low threshold operation and charge transport materials that bring about the stability to sustain the necessary current densities, several orders of magnitude higher than in OLEDs. We will demonstrate diode structures operated electrically under pulsed conditions at current densities up to 760 A/cm2 with a product of the current density and the external quantum effciency (J×ηext) of 1.27 A/cm2. Mechanisms deteriorating the quantum efficieny at elevated current densities will be discussed.
Inverted organic light-emitting diodes showing light emission from
the top are discussed. Top-emitting organic light-emitting diodes
are required for next-generation active-matrix organic
light-emitting displays , as Si-driving circuitry has to be
incorporated into the display itself. We focus on hybrid anodes,
thereby giving a simple model for spin-coating of PEDOT:PSS on top
of an organic layer-stack, LiF-based cathodes and phosphorescent
emitters, allowing for highly efficient inverted organic light
emitting diodes. A maximum current efficiency of 55.4 cd/A at
140 cd/m2 and a maximum luminous efficiency of 17.2 lm/W at
50 cd/m2 has been obtained.
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