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1.
Nat Commun ; 6: 7081, 2015 May 08.
Artículo en Inglés | MEDLINE | ID: mdl-25953105

RESUMEN

Solution-processed planar perovskite devices are highly desirable in a wide variety of optoelectronic applications; however, they are prone to hysteresis and current instabilities. Here we report the first perovskite-PCBM hybrid solid with significantly reduced hysteresis and recombination loss achieved in a single step. This new material displays an efficient electrically coupled microstructure: PCBM is homogeneously distributed throughout the film at perovskite grain boundaries. The PCBM passivates the key PbI3(-) antisite defects during the perovskite self-assembly, as revealed by theory and experiment. Photoluminescence transient spectroscopy proves that the PCBM phase promotes electron extraction. We showcase this mixed material in planar solar cells that feature low hysteresis and enhanced photovoltage. Using conductive AFM studies, we reveal the memristive properties of perovskite films. We close by positing that PCBM, by tying up both halide-rich antisites and unincorporated halides, reduces electric field-induced anion migration that may give rise to hysteresis and unstable diode behaviour.

2.
Adv Mater ; 27(1): 53-8, 2015 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-25359103

RESUMEN

A new method to deposit perovskite thin films that benefit from the thickness control and conformality of atomic layer deposition (ALD) is detailed. A seed layer of ALD PbS is place-exchanged with PbI2 and subsequently CH3 NH3 PbI3 perovskite. These films show promising optical properties, with gain coefficients of 3200 ± 830 cm(-1) .

3.
ACS Appl Mater Interfaces ; 6(1): 83-93, 2014 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-24024545

RESUMEN

Poly(silafluorene)s (PSFs) are promising light-emitting materials with brilliant solid-state blue luminescence, high quantum efficiency, excellent solubility, and improved thermal and chemical stability. PSFs are reported to have high electron affinity and conductivity originating from σ*-π* conjugation between the σ*-antibonding orbital of the exocyclic Si-C bond and the π* antibonding orbital of the butadiene fragment, a promising characteristic for improved charge carrier balance in OLEDs. In this paper, we present a protocol for photopatterning derivatives of poly(3,6-dimethoxy-9,9-dialkylsilafluorenes) with resolutions exceeding 10 µm. The procedure begins by converting polymers (Mn = 50-55 kg/mol, PDI = 1.8) with cyclohexenyl and norbornenyl containing side chains to their respective epoxides using the Prilezhaev reaction and m-chloroperoxybenzoic acid (m-CPBA). Using the I-line (365 nm) of a Karl Suss MA6 mask aligner, a 1 s UV light exposure of the photoacid generator (PAG) bis(4-tert-butylphenyl)iodonium hexafluoro-phosphate (DtBPI-PF6) generates sufficient protons to catalyze epoxide ring-opening and form a bridging network of covalent C-O bonds which renders the material insoluble in developing solvents such as toluene or THF. The resultant cross-linked material possess characteristic blue photoluminescence with solid state quantum yields >80%. Polymer films have excellent transparency (with a measured Eg ≈ 3.0 eV). Energy levels determined using cyclic voltammetry were -5.7 and -2.7 eV for HOMO and LUMO, respectively. Additionally, several device applications are demonstrated which incorporate cross-linked films. These include examples of solid state lasing in the region of 420-450 nm from cross-linked films on second order corrugated silica substrates (Λ = 200 nm). OLEDs were also prepared with a cross-linked emitting layer as part of a trilayer device which we report to have a maximum external quantum efficiency of 3.2% at 33 mA/cm(2) and a stable blue-violet emission with an electroluminescence maximum at 410 nm. Photopatternable PSF epoxides are also shown to be efficient hosts for Förster energy transfer and we provide examples of pattern layers incorporating small molecule emitters which emit in both the red and green while blue emission of the host is effectively suppressed.

4.
J Am Chem Soc ; 132(10): 3236-7, 2010 Mar 17.
Artículo en Inglés | MEDLINE | ID: mdl-20180567

RESUMEN

Cross-linked conductive polymer networks that mediate chemical, electronic, optical, and mechanical signals are enticing materials from which to construct actuators and sensors as well as more complex polymer-fiber-based structures capable of emulating natural cytoskeletal stress fibers such as actin. In this work we have synthesized and characterized a novel class of high molecular weight electroactive polyferrocenylsilane (PFS) that has been functionalized with pendant alkoxysilane groups and which can be conveniently gelled by sulfonic acid catalyzed condensation of the cross-linkable alkoxysilanes. These PFS electroactive gels are capable of converting an electrical signal to mechanical stress and strain as a result of a change in dimension in response to electrochemical oxidation or reduction coupled with transport of charge balancing ions and solvent molecules in PFS. Electrospinning of these polymer solutions is possible using a 5 kV voltage applied between a needle and indium tin oxide (ITO) substrate on to which fibers are collected. ITO substrates with collected fibers thereupon are incorporated into miniature electrochemical cells containing lithium triflate/gamma-butyrolactone electrolyte and examined using optical microscopy. Applying 1.5-2.0 V anodic potential to the ITO results in immediate oxidation of PFS fibers followed by strain induced buckling. This buckling occurs in many cases as regular sinusoid perturbations along the fiber. Application of cathodic 2.0 V potential causes most of the distorted fibers to return to their initial form. Such inherent shape memory is potentially useful in creating microswitches, microactuators, and micromanipulators.

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