The combination of efficient light emission and high charge-carrier mobility has thus far proved elusive for polymer semiconductors, with high mobility typically achieved by cofacial pi-electron system to pi-electron system interactions that quench exciton luminescence. We report a new strategy, comprising the introduction of a limited number of more effective hopping sites between otherwise relatively isolated, and thus highly luminescent, polyfluorene chains. Our approach results in polymer films with large mobility (mu approximately 3-6 x 10(-2) cm2 V-1 s-1) and simultaneously excellent light-emission characteristics. These materials are expected to be of interest for light-emitting transistors, light-emitting diode sources for optical communications and may offer renewed hope for electrically pumped laser action. In the last context, optically pumped distributed feedback lasers comprising one-dimensional etched silica grating structures coated with polymer have state-of-the-art excitation thresholds (as low as 30 W cm(-2) (0.1 nJ per pulse or 0.3 microJ cm-2) for 10 Hz, 12 ns, 390 nm excitation) and slope efficiencies (up to 11%).
Rational molecular design allows
for manipulating the chain conformations
of polymer semiconductors by cooperative arrangement of bulky groups
with steric hindrance effect and supramolecular groups with noncovalent
attractions. Herein, a model polyfluorene with β-phase, poly[4-(octyloxy)-9,9-diphenylfluoren-2,7-diyl]-co-[5-(octyloxy)-9,9-diphenylfluoren-2,7-diyl] (PODPF),
has been synthesized successfully via key Baeyer–Villiger rearrangement
reaction. Its thin film exhibited excellent spectral stability without
green band emission after thermal annealing at 200 °C under air
and nitrogen ambients. The β-phases of PODPF in the concentrated
toluene solution, organogels, and films have been characterized and
confirmed by UV absorption and PL spectra as well as grazing-incidence
X-ray scattering. The results suggest that the octyloxy substituents
enable backbone planarization via van der Waals forces of the in-plane
alkyl chains to overcome intrachain repulsion between fluorene monomers.
Organic lasers using β-phase PODPF exhibit lower threshold than
those of poly(9,9-dioctylfluorene), suggesting promising optical gain
media. This observation suggested that supramolecular steric hindrance
(SSH) is a promising molecular design of polymer semiconductors, and
supramolecular steric polymers are one kind of model to get insight
into the structure–function relationships for electrically
pumped organic lasers in organic electronic and photonics.
Nonradiative
recombination, the main energy loss channel for open
circuit voltage (V
oc), is one of the crucial
problems for achieving high power conversion efficiency (PCE) in inverted
perovskite solar cells (PSCs). Usually, grain boundary passivation
is considered as an effective way to reduce nonradiative recombination
because the defects (uncoordinated ions) on grain boundaries are passivated.
We added the hydroxyl and carbonyl functional groups containing carbon
quantum dots (CQDs) into a perovskite precursor solution to passivate
the uncoordinated lead ions on grain boundaries. Higher photoluminescence
intensity and longer carrier lifetime were demonstrated in the perovskite
film with the CQD additive. This confirmed that the addition of CQDs
can reduce nonradiative recombination by grain boundary passivation.
Additionally, the introduction of CQDs could increase the thickness
of the perovskite film. Consequently, we achieved a champion device
with a PCE of 18.24%. The device with CQDs retained 73.4% of its initial
PCE after being aged for 48 h under 80% humidity in the dark at room
temperature. Our findings reveal the mechanisms of how CQDs passivate
the grain boundaries of perovskite, which can improve the efficiency
and stability of PSCs.
We report the fabrication of optically pumped solid‐state polymer lasers based on the semiconducting polymer poly(9,9‐dioctylfluorene) (PFO) using resonator structures that offer one‐ and two‐dimensional distributed feedback. The lasers are readily fabricated by solution deposition of thin polymer films on top of suitable grating microstructures etched into fused silica substrates. The devices operate in the blue spectral region, are highly efficient (slope efficiencies as high as 7.8 % are demonstrated), and exhibit very low threshold energies for oscillation (0.8 nJ per pulse). The operating characteristics of the lasers are investigated in detail. The transverse mode profiles and divergence of the output beams are measured and correlated with the internal lasing modes and the feedback mechanism present in the resonators. Additionally, broadband tuning of the emission wavelength over a range of ∼ 40 nm is demonstrated by controlling the supported resonant frequency of the laser cavities.
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