RESUMEN
Effective charge separation is essential in plasmon-mediated photochemistry and is usually achieved by constructing plasmon-semiconductor interfaces, which is usually challenging. In this work, by monitoring the plasmon-mediated silver oxidation with in situ Raman spectroscopy, we demonstrate that the adsorbed thiophenol molecules could modulate the rate of photochemical reactions by tuning the charge separation at the plasmon-molecule interfaces. It is found that the thiophenol molecules with strong electron-withdrawing or donating functional groups could accelerate or decelerate the rate of plasmon-mediated silver oxidation, respectively. Owing to the easy tuning of the electronic structures of organic molecules via substitution, our method provides a versatile and convenient approach for the fine modulation of plasmon-mediated photochemical reactions.
RESUMEN
Emerging intrinsically flexible fully π-conjugated polymers (FπCPs) are a promising functional material for flexible optoelectronics, attributed to their potential interchain interpenetration and entanglement. However, the challenge remains in obtaining elastic-plastic FπCPs with intrinsic robust optoelectronic property and excellent long-term and cycling deformation stability simultaneously for applications in deep-blue flexible polymer light-emitting diodes (PLEDs). This study, demonstrates a series of elastic-plastic FπCPs (P1-P4) with an excellent energy dissipation capacity via side-chain internal plasticization for the ultra-deep-blue flexible PLEDs. First, the freestanding P1 film exhibited a maximum fracture strain of 34.6%. More interestingly, the elastic behavior is observed with a low strain (≤10%), and the stretched film with a high deformation (>10%) attributed to plastic processing revealed the robust capacity to realize energy absorption and release. The elastic-plastic P1 film exhibits outstanding ultra-deep-blue emission, with an efficiency of 56.38%. Subsequently, efficient PLEDs are fabricated with an ultra-deep-blue emission of CIE (0.16, 0.04) and a maximum external quantum efficiency of 1.73%. Finally, stable and efficient ultra-deep-blue electroluminescence are obtained from PLEDs based on stretchable films with different strains and cycling deformations, suggesting excellent elastic-plastic behavior and deformation stability for flexible electronics.
RESUMEN
A new non-conjugated polymer (PVCz-OMeDAD) with good solution processability was developed to serve as an efficient dopant-free hole-transporting material (HTM) for perovskite solar cells (PSCs). PVCz-OMeDAD was simply prepared by the free-radical polymerization of vinyl monomers, which were synthesized from low-cost raw materials through three high-yield synthesis steps. The combination of the flexible non-conjugated polyvinyl main chain and hole-transporting methoxydiphenylamine-substituted carbazole side chains endowed PVCz-OMeDAD with excellent film-forming ability, a suitable energy level, and high hole mobility. As a result, by using an ultra-thin (≈30â nm) PVCz-OMeDAD film as cost-effective dopant-free polymer HTM, the conventional n-i-p-type PSCs demonstrated a power conversion efficiency (PCE) up to 16.09 %, suggesting the great potential of the polymer film for future low-cost, large-scale, flexible PSCs applications.
Asunto(s)
Compuestos de Calcio/química , Suministros de Energía Eléctrica , Óxidos/química , Polímeros/química , Energía Solar , Titanio/química , Polimerizacion , TemperaturaRESUMEN
Control of the hierarchical molecular organization of polydiarylfluorenes by synthetic strategies is significant for optimizing photophysical properties as well as the performance of light-emitting devices. Herein, for the suppression of molecular aggregation and enhancement of luminescence efficiency, a series of steric units were introduced into polydiarylfluorenes by copolymerization, with the aim of integrating the advantages of the steric-hindrance effect and of the ß-phase. Optical and Raman spectroscopies revealed a ß-phase conformation for a polymer copolymerized with spiro[fluorene-9,9'-xanthene] (SFX), with photoluminescence (PL) peaks at 454, 482, and 517 nm. Moreover, the morphological stability and electroluminescence (EL) stability were also improved without compromising the performance of the polymer light-emitting diodes (PLEDs). Furthermore, three steric-hindrance-functionalized copolymers showed significantly decreased thresholds for amplified spontaneous emission (EthASE) and enhanced stability following thermal annealing treatment. These results indicate that steric-hindrance functionalization is a superior approach to improve the overall stability and optoelectronic properties for blue-light-emitting π-conjugated polymers.