High-efficiency inverted polymer solar cells via dual effects of introducing the high boiling point solvent and the high conductive PEDOT:PSS layer

Polymer solar cells (PSCs) are of great interest in the past decade owing to their potentially low-cost in the manufacturing by the solution-based roll to roll method. In this paper, a novel inverted device structure was introduced by inserting a high conductive PEDOT:PSS (hcPEDOT:PSS) layer between the Au nanoparticles (NPs)-embedded hole transport layer (PEDOT:PSS) and the top electrode layer. Power conversion efficiency (PCE) initially reached up to 4.51%, illustrating ∼10% higher compared with the device similarly enhanced by Au NPs plasmonics where only one PEDOT:PSS layer with the embedded Au NPs was used in single bulk heterojunction inverted PSCs based on the poly(3-hexylthiophene):[6,6]-phenyl C61-butyric acid methylester (P3HT:PCBM). The PCE was further improved from 4.51% to 5.01% by adding the high-boiling point solvent of 1,8-diiodooctane (DD) into the active layer, presenting ∼20% enhancement in PCE through dual effects of introducing the high boiling point solvent and the high conductive PEDOT:PSS layer. Morphologies of the active layers were characterised by SEM and AFM separately in the paper.     

Photolithographic patterning of PEDOT:PSS with a silver interlayer and its application in organic light emitting diodes

A patterning scheme for poly(3,4-ethylenedioxythio-phene):poly(styrenesulfonate) (PEDOT:PSS) is reported. With a silver interlayer, the conductive PEDOT:PSS film can be patterned down to micrometer scales by traditional photolithography, and this patterning scheme can be applied on large-area flexible substrates. Through systematical investigations, the patterning processes have no obvious influence on both the bulk and surface properties of PEDOT:PSS films. Efficient organic light emitting diodes (OLEDs) are realized based on this patterned PEDOT:PSS anode, and they show comparable performance to those devices with an indium tin oxide (ITO) anode. High-resolution OLED pixel arrays are also demonstrated. Our interlayer approach here has an advantage of patterning PEDOT:PSS with high resolution and large scale, and it is also compatible with traditional photolithographic processes which substantially save the capital cost. Results indicate that the photographically patterned conductive PEDOT:PSS film becomes a promising candidate for eletrical eletrode material in organic electronic applications.     

Benzodithiophene and benzotrithiophene-based conjugated polymers for organic thin-film transistors application: Impact of conjugated- and acyl-side chain

A series of benzodithiophene (BDT) and benzotrithiophene (BTT)-based conjugated polymers (P1–P4), with/without conjugated- and acyl-side chain, have been synthesized by Stille cross-coupling reaction. Their thermal, photophysical, electrochemical properties, devices performances, and microstructure have been investigated. Conjugated-side chain can significantly raise the thermal stability and acyl-side chain can lower HOMO/LUMO energy levels. Organic thin-film transistors (OTFTs) based on conjugated polymers were fabricated and the transistor electrical characterization showed the device performance was sensitive to the conjugated- and acyl-side chain substituent of polymers. A maximum hole mobility of 1.70 × 10⁻³ cm² V⁻¹ s⁻¹ was obtained for P1-based devices, which is an order of magnitude higher than those of P3 and P4-based devices. The corresponding microstructures were investigated by grazing-incidence X-ray diffraction (GIXD) to correlate with conjugated- and acyl-side chain dependent carrier mobility of P1–P4. The results showed that the conjugated- and acyl-side chain have an impact on the polymer packing models and device performances.     

Design rules for semi-transparent organic tandem solar cells for window integration

For window integration of semi-transparent solar cells in living and working areas, color neutral transparency perception and good color rendering are of pivotal importance. In order to tune the optical device properties, we simulate a parallel tandem configuration with two different absorber materials. Within a regime of convenient transparency perception, the transparency can be adjusted between 20% and 40% by choosing the right absorber layer thickness combination. From the optical field in the tandem devices we calculate the charge carrier generation profile and subsequently correlate the optical properties with the electrical device properties as derived from drift-diffusion modelling – altogether allowing for a comprehensive assessment of the transparency, the transparency perception and the device performance and their interdependencies.     

Growth behavior and improved water–vapor-permeation-barrier properties of 10-nm-thick single Al2O3 layer grown via cyclic chemical vapor deposition on organic light-emitting diodes

We have investigated the growth behavior and water vapor permeation barrier properties of cyclic chemical vapor deposition (C-CVD)-grown 10-nm-thick single layer of Al₂O₃. Al₂O₃ layers grown by C-CVD showed a high density of 3.298 g/cm³ and were amorphous without grain boundaries. A deposition rate of 0.46 nm/cycle was obtained. The C-CVD system was self-limiting, as in the case of atomic layer deposition, which enables precise control of the thickness of the Al₂O₃ layer. A water vapor transmission rate of 1.51 × 10⁻⁵ (g/m²)/day was obtained from a Ca degradation test performed at 85 °C and 85% relative humidity. Moreover, the performance of organic light-emitting diodes, passivated by a C-CVD-grown 10-nm-thick Al₂O₃ single layer, was not affected after 24,000 h of turn-on time; this is strong evidence that C-CVD-grown Al₂O₃ layers effectively prevent water vapor from diffusing into the active organic layer.     

On the role of aggregation effects in the performance of perylene-diimide based solar cells

A model bulk-heterojunction of a perylene diimide (PDI) monomeric derivative is studied for interrogating the role of PDI aggregates in the photocurrent generation efficiency (η_PC) of PDI-based organic photovoltaic (OPV) devices. Blend films of the PDI derivative and the poly(indenofluorene) (PIF) polymer annealed between room temperature and 220 °C, are used as the photoactive layers for the fabrication of OPVs. The positive effect of thermal annealing is assigned to the evolution of PDI aggregates in the amorphous PIF matrix. Annealing increases the electron mobility by three orders of magnitude. In contrast, owned to the thermally inert PIF matrix used, hole mobility increases only by a factor of six. High resolution cross-sectional scanning electron microscopy suggests that η_PC in PDI-based OPVs is not limited by the PDI aggregates but by their improper alignment. In situ Raman spectra and density functional theory calculations identify a marker for monitoring the strength of π–π stacking interactions between PDI monomers. It s further demonstrated that the electron-collecting electrode of the PIF:PDI devices dictates their performance. The use of Al is found to impede charge extraction and this is attributed to an unidentified product of the reaction between PDI and Al that leads to the formation of an electron-blocking layer. Device performance rectifies when a Ca/Al electrode is used and the power conversion efficiency is increased by a factor of four.     

Intrinsic difference in Schottky barrier effect for device configuration of organic thin-film transistors

Schottky barrier effect for n-channel organic thin-film transistors (OTFTs) with bottom-gate, top-contact (TC) and bottom-gate, bottom-contact (BC) configuration was examined by using device simulation with a thin-film organic transistor advanced simulator (TOTAS). A thermionic field emission (TFE) model which addresses tunneling of thermally excited electrons was applied as a carrier injection model of OTFTs. Simulation results reveal that the BC configuration is affected by Schottky barrier more severely than the TC configuration under the same condition for device parameters, and that this discrepancy in device characteristics can be completely alleviated by contact-area-limited doping, where highly-doped semiconducting layers are prepared in the neighborhood of contact electrodes. Moreover, the existence of an intrinsic Schottky barrier is indicated even though an ohmic-contact condition is assumed, which becomes more prominent for lower bulk carrier concentration in organic semiconductor. This work suggests the availability of the TFE model for simulating realistic OTFT devices with Schottky contacts. From the simulation results, intrinsic differences in device performance for the TC and BC configurations are discussed.     

Evolution in crystal structure and electrical performance of thiophene-based polymer field effect transistors: A remarkable difference between thermal and solvent vapor annealing

We report the various conformational structures of long pendant side-chains, and the effects of thermal and solvent vapor annealing (SVA) with the corresponding charge carrier mobilities of thiophene-based conjugated polymers, poly[5,5′-bis(3-dodecyl-2-thienyl)-2,2′-bithiophene] (PQT-12) and poly(4,4′-bis-decyloxymethylquaterthiophene) (POQT), by correlated study of their extraordinary polymorphic crystal structures. In substitution for alkyl chains in polythiophenes, ether alkyl chains induce a favorable non-covalent interaction between the oxygen and sulfur atoms and help the polymer chains planar with lower torsion angles between conjugated backbone units showing a reduced π–π stacking distance. However, the flexibility and conformational freedom with such long side-chains dominantly induce polymorphic crystallites from bent and extended side-chains. Especially, POQT exhibit two polymorphic crystallite phases in a similar ratio probably due to the increased freedom of ether alkyl chains. Therefore, the field effect mobility of POQT is decreased gradually with the increase of annealing temperature from 0.024 (at 80 °C) to 3.96 × 10⁻⁴ cm²/V s (at 170 °C). Contrary to the thermal annealing method, solvent-vapor-annealed POQT films show highly ordered and single-phase crystallites with edge-on orientation to the substrate, which ultimately provides an effectively improved charge carrier mobility from 0.023 (pristine) to 0.076 cm²/V s after adequate solvent vapor exposure.     

Thermal buffer materials for enhancement of device performance of organic light emitting diodes fabricated by laser imaging process

Laser Induced Thermal Imaging (LITI) is a laser addressed thermal patterning technology with unique advantages such as an excellent uniformity of transfer film thickness, a capability of multilayer stack transfer and a possibility to fabricate high resolution as well as large-area display. Nevertheless, it has been an obstacle to use such a laser imaging process as a commercial technology so far because of serious deterioration of the device performances plausibly due to a re-orientation of the molecular stacking especially in the emitting layer during thermal transfer process. To improve device performances, we devised a new concept to suppress the thermal degradation during such kind of thermal imaging process by using a high molecular weight small molecular species with large steric hindrance as well as high thermostability as a thermal buffer layer to realize highly efficient LITI devices. As a result, we obtained very high relative efficiency (by EQE) up to 91.5% at 1000 cd/m² from the LITI devices when we utilize 10-(naphthalene-2-yl)-3-(phenanthren-9-yl)spiro[benzo[ij]tetraphene-7,9′-fluorene] as a thermal buffer material.     

High efficiency organic photovoltaic cells based on inverted SubPc/C60/ITO cascade junctions

Conventional heterojunction organic photovoltaic cells typically involve the deposition of the electron donor layer (or donor–acceptor blend) on top of a transparent anode, with the cathode deposited last. Inverting the structure and deposition sequence usually worsens the performance characteristics, except device lifetime. We compare conventional (SubPc/C₆₀) and inverted (C₆₀/SubPc) junctions, the latter exhibiting a power conversion efficiency of 3.5%. We also find a significant trade-off between the open circuit voltage and short circuit photocurrent, potentially attributable to the formation of a C₆₀/ITO Schottky junction, and a change from exciton-quenching to exciton-blocking behavior of the SubPc:MoO_X interface in inverted devices.