High‐Performance Organic Solar Cells with Spray‐Coated Hole‐Transport and Active Layers

In this study, we report high performance organic solar cells with spray coated hole‐transport and active layers. With optimized ink formulations we are able to deposit films with controlled thickness and very low surface roughness (<10 nm). Specifically we deposit smooth and uniform 40 nm thick films of poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as well as films composed of a mixture of poly(3‐hexyl thiophene) (P3HT) and the C₆₀‐derivative (6,6)‐phenyl C61‐butyric acid methyl ester (PCBM) with thicknesses in the range 200–250 nm. To control film morphology, formation and thickness, the optimized inks incorporate two solvent systems in order to take advantage of surface tension gradients to create Marangoni flows that enhance the coverage of the substrate and reduce the roughness of the film. Notably, we achieve fill factors above 70% and attribute the improvement to an enhanced P3HT crystallization, which upon optimized post‐drying thermal annealing results in a favorable morphology. As a result, we could extend the thickness of the layer to several hundreds of nanometers without noticing a substantial decrease of the transport properties of the layer. By proper understanding of the spreading and drying dynamics of the inks we achieve spray coated devices with power conversion efficiency of 3.75%, with fill factor, short circuit current and open circuit voltage of 70%, 9.8 mA cm^?2 and 550 mV, respectively.     

p‐Doping of Copper(I) Thiocyanate (CuSCN) Hole‐Transport Layers for High‐Performance Transistors and Organic Solar Cells

The ability to tune the electronic properties of soluble wide bandgap semiconductors is crucial for their successful implementation as carrier‐selective interlayers in large area opto/electronics. Herein the simple, economical, and effective p‐doping of one of the most promising transparent semiconductors, copper(I) thiocyanate (CuSCN), using C₆₀F₄₈ is reported. Theoretical calculations combined with experimental measurements are used to elucidate the electronic band structure and density of states of the constituent materials and their blends. Obtained results reveal that although the bandgap (3.85 eV) and valence band maximum (?5.4 eV) of CuSCN remain unaffected, its Fermi energy shifts toward the valence band edge upon C₆₀F₄₈ addition—an observation consistent with p‐type doping. Transistor measurements confirm the p‐doping effect while revealing a tenfold increase in the channel's hole mobility (up to 0.18 cm² V^?1 s^?1), accompanied by a dramatic improvement in the transistor's bias‐stress stability. Application of CuSCN:C₆₀F₄₈ as the hole‐transport layer (HTL) in organic photovoltaics yields devices with higher power conversion efficiency, improved fill factor, higher shunt resistance, and lower series resistance and dark current, as compared to control devices based on pristine CuSCN or commercially available HTLs.     

Tuning Hole Transport Layer Using Urea for High‐Performance Perovskite Solar Cells

Interface engineering is critical to the development of highly efficient perovskite solar cells. Here, urea treatment of hole transport layer (e.g., poly(3,4‐ethylene dioxythiophene):polystyrene sulfonate (PEDOT:PSS)) is reported to effectively tune its morphology, conductivity, and work function for improving the efficiency and stability of inverted MAPbI₃ perovskite solar cells (PSCs). This treatment has significantly increased MAPbI₃ photovoltaic performance to 18.8% for the urea treated PEDOT:PSS PSCs from 14.4% for pristine PEDOT:PSS devices. The use of urea controls phase separation between PEDOT and PSS segments, leading to the formation of a unique fiber‐shaped PEDOT:PSS film morphology with well‐organized charge transport pathways for improved conductivity from 0.2 S cm^?1 for pristine PEDOT:PSS to 12.75 S cm^?1 for 5 wt% urea treated PEDOT:PSS. The urea‐treatment also addresses a general challenge associated with the acidic nature of PEDOT:PSS, leading to a much improved ambient stability of PSCs. In addition, the device hysteresis is significantly minimized by optimizing the urea content in the treatment.     

Cover Picture: Solution‐Processed Organic Tandem Solar Cells (Adv. Funct. Mater. 14/2006)

The fabrication of a solution‐processed polymer tandem cell by stacking two single cells in series is reported by de Boer and co‐workers on p. 1897. The bottom and top cell are complementary with respect to their absorption spectra and the layer thickness of the bottom cell was optimized in order to create an optical cavity that efficiently transmits the required wavelength for the top cell. The combination of this tandem architecture with more efficient small‐bandgap materials will enable the realization of highly efficient organic solar cells. A solution‐processed polymer tandem cell fabricated by stacking two single cells in series is demonstrated. The two bulk‐heterojunction subcells have complementary absorption maxima at λ_max ～ 850 nm and λ_max ～ 550 nm, respectively. A composite middle electrode is applied that serves both as a charge‐recombination center and as a protecting layer for the first cell during spin‐coating of the second cell. The subcells are electronically coupled in series, which leads to a high open‐circuit voltage of 1.4 V, equal to the sum of each subcell. The layer thickness of the first (bottom) cell is tuned to maximize the optical absorption of the second (top) cell. The performance of the tandem cell is presently limited by the relatively low photocurrent generation in the small‐bandgap polymer of the top cell. The combination of our tandem architecture with more efficient small‐bandgap materials will enable the realization of highly efficient organic solar cells in the near future.     

Solar Cells: Performance Optimization of Polymer Solar Cells Using Electrostatically Sprayed Photoactive Layers (Adv. Funct. Mater. 20/2010)

Polymer solar cells (PSCs) are fabricated using a novel film deposition method, the electrostatic spray (e‐spray) technique. Stable atomization and uniform deposition of the polymer blend by e‐spray are achieved by manipulating the solution concentration, the solvent composition, and the electric field. The performance of PSCs is primarily influenced by the inherent film morphology of the e‐sprayed polymer‐blend active layers, which is significantly different from that of the conventional films that are formed using the spin‐coating (SC) method. The intrinsically formed interfacial boundaries between the e‐sprayed blend pancakes resist charge transport, which unfavorably influences device efficiency. The internal series resistance (R_S) of the PSCs that are formed using the e‐spray method (e‐spray‐PSC) is significantly reduced by a solvent vapor soaking (SVS) treatment in addition to the conventional thermodynamic nanomorphology controls. The detailed relationship between the morphologies (film morphology and internal nanomorphology) and the R_S is revealed using impedance spectroscopy. The performance of the e‐spray‐PSCs is comparable to those of the PSCs that are fabricated using the SC method under identical conditions. Therefore, the e‐spray method can be used to fabricate ultralow‐cost PSCs, because of the performance results combined with the intrinsic advantages that the e‐spray method is simple and has a low materials loss.     

PEDOT:PSS‐Assisted Exfoliation and Functionalization of 2D Nanosheets for High‐Performance Organic Solar Cells

Here, a facial and scalable method for efficient exfoliation of bulk transition metal dichalcogenides (TMD) and graphite in aqueous solution with poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) to prepare single‐ and few‐layer nanosheets is demonstrated. Importantly, these TMD nanosheets retain the single crystalline characteristic, which is essential for application in organic solar cells (OSCs). The hybrid PEDOT:PSS/WS₂ ink prepared by a simple centrifugation is directly integrated as a hole extraction layer for high‐performance OSCs. Compared with PEDOT:PSS, the PEDOT:PSS/WS₂‐based devices provide a remarkable power conversion efficiency due to the “island” morphology and benzoid–quinoid transition. This study not only demonstrates a novel method for preparing single‐ and few‐layer TMD and graphene nanosheets but also paves a way for their applications without further complicated processing.