Vertical Organic Thin-Film Transistors with an Anodized Permeable Base for Very Low Leakage Current.

The organic permeable base transistor (OPBT) is currently the fastest organic transistor with a transition frequency of 40 MHz. It relies on a thin aluminum base electrode to control the transistor current. This electrode is surrounded by a native oxide layer for passivation, currently created by oxidation in air. However, this process is not reliable and leads to large performance variations between samples, slow production, and relatively high leakage currents. Here, for the first time it is demonstrated that electrochemical anodization can be conveniently employed for the fabrication of high-performance OPBTs with vastly reduced leakage currents and more controlled process parameters. Very large transmission factors of 99.9996% are achieved, while excellent on/off ratios of 5 × 105 and high on-currents greater than 300 mA cm-2 show that the C60 semiconductor layer can withstand the electrochemical anodization. These results make anodization an intriguing option for innovative organic transistor design.

Elucidating the Role of Conjugated Polyelectrolyte Interlayers for High-Efficiency Organic Photovoltaics.

Despite the promising function of conjugated polyelectrolytes (CPEs) as an interfacial layer in organic photovoltaics (OPVs), the underlying mechanism of dipole orientation and the electrical characteristics of CPE interlayers remain unclear. Currently, the ionic functionality of CPEs (i.e., whether they are cationic or anionic) is believed to determine the interfacial dipole alignment and the resulting electron or hole extraction properties at the interface between an organic photoactive layer and a metal electrode. In this research, we find that in contrast to this common belief, the photovoltaic efficiency can be improved significantly by both cationic and anionic CPE layers regardless of the ion functionality of the CPE. This improvement occurs because the interfacial dipoles of cationic and anionic CPEs are realigned in the identical direction despite the different ionic functionality. The net dipole is determined not by the intrinsic molecular dipole of the CPE but by the ionic redistribution in the CPE layer and the resulting interfacial dipole at the intimate contact with adjacent layers. We also demonstrated that the energy level alignment and performance parameters of OPVs can be controlled systematically by the electrically poled CPE layers with the oriented interfacial dipoles; the distribution of positive and negative ions in the CPE layer was adjusted by applying an appropriate external electric field, and the energy alignment was reversible by changing the electric field direction. The anionic and cationic CPEs (PSBFP-Na and PAHFP-Br) based on the same π-conjugated backbone of fluorene-phenylene were each used as the electron extraction layer on a photoactive layer. Both anionic and cationic CPE interlayers improved the energy level alignment at the interface between the photoactive layer and the electrode and the resulting performance parameters, which thereby increased the power conversion efficiency to 8.3 %.

Bimolecular crystals with an intercalated structure improve poly(p-phenylenevinylene)-based organic photovoltaic cells.

The exciton dissociation, recombination, and charge transport of bulk heterojunction organic photovoltaic cells (OPVs) is influenced strongly by the nanomorphology of the blend, such as the grain size and the molecular packing. Although it is well known that polymers based on amorphous poly(p-phenylenevinylene) (PPV) have a fundamental limit to their efficiency because of low carrier mobility, which leads to increased recombination and unbalanced charge extraction, herein, we demonstrate that the issue can be overcome by forming bimolecular crystals of an amorphous PPV-based polymer:phenyl-C61 -butyric acid methyl ester (PCBM) intercalated structure. We used amorphous poly(2,5-dioctyloxy-p-phenylene vinylene-alt-2',5'-thienylene vinylene) (PPVTV), which has a simple chemical structure. A reasonably high power conversion efficiency (∼3.5 %) was obtained, although the material has an intrinsically amorphous structure and a relatively large band gap (2.0 eV). We demonstrate a correlation between a well-ordered bimolecular crystal of PPVTV:PCBM and an improved hole mobility of a PPVTV:PCBM film compared to a pristine PPVTV film by using 2 D grazing incidence XRD and space-charge-limited current measurements. Furthermore, we show that the bimolecular crystal structure in high-performance OPVs is related to an optimum molecular packing, which is influenced by the PPVTV:PCBM blending ratio, side-chain length, and molecular weight of the PPVTV polymer. Improved charge transport in PPVTV:PCBM bimolecular crystals leads to a fast sweep out of charges and thus suppression of nongeminate recombination under the operating conditions.

Boosting the power conversion efficiency of perovskite solar cells using self-organized polymeric hole extraction layers with high work function.

A self-organized hole extraction layer (SOHEL) with high work function (WF) is designed for energy level alignment with the ionization potential level of CH3 NH3 PbI3 . The SOHEL increases the built-in potential, photocurrent, and power conversion efficiency (PCE) of CH3 NH3 PbI3 perovskite solar cells. Thus, interface engineering of the positive electrode of solution-processed planar heterojunction solar cells using a high-WF SOHEL is a very effective way to achieve high device efficiency (PCE = 11.7% on glass).

Role of ultrathin metal fluoride layer in organic photovoltaic cells: mechanism of efficiency and lifetime enhancement.

Although rapid progress has been made recently in bulk heterojunction organic solar cells, systematic studies on an ultrathin interfacial layer at the electron extraction contact have not been conducted in detail, which is important to improve both the device efficiency and the lifetime. We find that an ultrathin BaF2 layer at the electron extraction contact strongly influences the open-circuit voltage (Voc ) as the nanomorphology evolves with increasing BaF2 thickness. A vacuum-deposited ultrathin BaF2 layer grows by island growth, so BaF2 layers with a nominal thickness less than that of single-coverage layer (≈3 nm) partially cover the polymeric photoactive layer. As the nominal thickness of the BaF2 layer increased to that of a single-coverage layer, the Voc and power conversion efficiency (PCE) of the organic photovoltaic cells (OPVs) increased but the short-circuit current remained almost constant. The fill factor and the PCE decreased abruptly as the thickness of the BaF2 layer exceeded that of a single-coverage layer, which was ascribed to the insulating nature of BaF2 . We find the major cause of the increased Voc observed in these devices is the lowered work function of the cathode caused by the reaction and release of Ba from thin BaF2 films upon deposition of Al. The OPV device with the BaF2 layer showed a slightly improved maximum PCE (4.0 %) and a greatly (approximately nine times) increased device half-life under continuous simulated solar irradiation at 100 mW cm(-2) as compared with the OPV without an interfacial layer (PCE=2.1 %). We found that the photodegradation of the photoactive layer was not a major cause of the OPV degradation. The hugely improved lifetime with cathode interface modification suggests a significant role of the cathode interfacial layer that can help to prolong device lifetimes.

Organic solar cells using CVD-grown graphene electrodes.

We report on the development of flexible organic solar cells (OSCs) incorporating graphene sheets synthesized by chemical vapor deposition (CVD) as transparent conducting electrodes on polyethylene terephthalate (PET) substrates. A key barrier that must be overcome for the successful fabrication of OSCs with graphene electrodes is the poor-film properties of water-based poly(3,4-ethylenedioxythiphene):poly(styrenesulfonate) (PEDOT:PSS) when coated onto hydrophobic graphene surfaces. To form a uniform PEDOT:PSS film on a graphene surface, we added perfluorinated ionomers (PFI) to pristine PEDOT:PSS to create 'GraHEL', which we then successfully spin coated onto the graphene surface. We systematically investigated the effect of number of layers in layer-by-layer stacked graphene anode of an OSC on the performance parameters including the open-circuit voltage (Voc), short-circuit current (Jsc), and fill factor (FF). As the number of graphene layers increased, the FF tended to increase owing to lower sheet resistance, while Jsc tended to decrease owing to the lower light absorption. In light of this trade-off between sheet resistance and transmittance, we determined that three-layer graphene (3LG) represents the best configuration for obtaining the optimal power conversion efficiency (PCE) in OSC anodes, even at suboptimal sheet resistances. We finally developed efficient, flexible OSCs with a PCE of 4.33%, which is the highest efficiency attained so far by an OSC with CVD-grown graphene electrodes to the best of our knowledge.

Controlling surface enrichment in polymeric hole extraction layers to achieve high-efficiency organic photovoltaic cells.

Hole extraction in organic photovoltaic cells (OPVs) can be modulated by a surface-enriched layer formed on top of the conducting polymer-based hole extraction layer (HEL). This tunes the surface work function of the HEL to better align with the ionization potential of the polymeric photoactive layer. Results show noticeable improvement in device power conversion efficiencies (PCEs) in OPVs. We achieved a 6.1 % PCE from the OPV by optimizing the surface-enriched layer.

Polyaniline-based conducting polymer compositions with a high work function for hole-injection layers in organic light-emitting diodes: formation of ohmic contacts.

It is a great challenge to develop solution-processed, polymeric hole-injection layers (HILs) that perform better than small molecular layers for realizing high-performance small-molecule organic light-emitting diodes (SM-OLEDs). We have greatly improved the injection efficiency and the current efficiency of SM-OLEDs by introducing conducting polymer compositions composed of polyaniline doped with polystyrene sulfonate and perfluorinated ionomer (PFI) as the HIL. During single spin-coating of conducting polymer compositions, the PFI layer was self-organized at the surface and greatly increased the film work function. It enhanced hole-injection efficiency and current efficiency by introducing a nearly ohmic contact and improving electron blocking. Our results demonstrate that solution-processed polyaniline HILs with tunable work functions are good candidates for reducing process costs and improving OLED performance.