9 Search Results

Abstract The short exciton diffusion length associated with most classical organic semiconductors used in organic photovoltaics (5-20 nm) imposes severe limits on the maximum size of the donor and acceptor domains within the photoactive layer of the cell. Identifying materials that are able to transport excitons over longer distances can help advancing our understanding and lead to solar cells with higher efficiency. Here, we measure the exciton diffusion length in a wide range of nonfullerene acceptor molecules using two different experimental techniques based on photocurrent and ultrafast spectroscopy measurements. The acceptors exhibit balanced ambipolar charge transport and surprisingly long exciton diffusionmore » lengths in the range of 20 to 47 nm. With the aid of quantum-chemical calculations, we are able to rationalize the exciton dynamics and draw basic chemical design rules, particularly on the importance of the end-group substituent on the crystal packing of nonfullerene acceptors.« less

Abstract Due to a general paucity of suitable characterization methods, the internal orientational ordering of polymer fibrils has rarely been measured despite its importance particularly for semi‐conducting polymers. An emerging tool with sensitivity to bond orientation is polarized resonant soft X‐ray scattering (P‐RSoXS). Here, P‐RSoXS reveals the molecular arrangement within fibrils (if type I or type II fibrils), the extent of orientation in the fibril crystal, and an explicit crystal‐amorphous interphase. Neat films as well as binary blends with a fullerene derivative are characterized for three different polymers, that are prototypical materials widely used in organic electronics applications. Anisotropic P‐RSoXSmore » patterns reveal two different fibril types. Analysis of the q ‐dependence of the anisotropy from simulated and experimental scattering patterns reveal that neat polymer fibrillar systems likely comprise more than two phases, with the third phase in addition to crystal and amorphous likely being an interphase with distinct density and orientation. Intriguingly, the fibril type correlates to the H‐ or J‐aggregation signature in ultraviolet‐visible (UV–vis) spectroscopy, revealing insight into the fibril formation. Together, the results will open the door to develop more sophisticated structure‐function relationships between chemical design, fibril type, formation pathways and kinetics, interfacial ordering, and eventually device functions.« less

Abstract To achieve semiconducting materials with high electron mobility in organic field‐effect transistors (OFETs), low‐lying energy levels (the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO)) and favorable molecular packing and ordering are two crucial factors. Here, it is reported that the incorporation of pyridine and selenophene into the backbone of a diketopyrrolopyrrole (DPP)‐based copolymer produces a high‐electron‐mobility semiconductor, PDPPy‐Se. Compared with analogous polymers based on other DPP derivatives and selenophene, PDPPy‐Se features a lower LUMO that can decrease the electron transfer barrier for more effective electron injection, and simultaneously a lower HOMO that, however, canmore » increase the hole transfer barrier to suppress the hole injection. Combined with thermal annealing at 240 °C for thin film morphology optimization to achieve large‐scale crystallite domains with tight molecular packing for effective charge transport along the conducting channel, OFET devices fabricated with PDPPy‐Se exhibit an n‐type‐dominant performance with an electron mobility (μ _e ) as high as 2.22 cm ² V ⁻¹ s ⁻¹ and a hole/electron mobility ratio (μ _h /μ _e ) of 0.26. Overall, this study demonstrates a simple yet effective approach to boost the electron mobility in organic transistors by synergistic use of pyridine and selenophene in the backbone of a DPP‐based copolymer.« less

Abstract Solution‐processed Cu(In,Ga)(S,Se) ₂  (CIGS) has a great potential for the production of large‐area photovoltaic devices at low cost. However, CIGS solar cells processed from solution exhibit relatively lower performance compared to vacuum‐processed devices because of a lack of proper composition distribution, which is mainly instigated by the limited Se uptake during chalcogenization. In this work, a unique potassium treatment method is utilized to improve the selenium uptake judiciously, enhancing grain sizes and forming a wider bandgap minimum region. Careful engineering of the bandgap grading structure also results in an enlarged space charge region, which is favorable for electron–hole separationmore » and efficient charge carrier collection. Besides, this device processing approach has led to a linearly increasing electron diffusion length and carrier lifetime with increasing the grain size of the CIGS film, which is a critical achievement for enhancing photocurrent yield. Overall, 15% of power conversion efficiency is achieved in solar cells processed from environmentally benign solutions. This approach offers critical insights for precise device design and processing rules for solution‐processed CIGS solar cells.« less

Layered perovskites have been shown to improve the stability of perovskite solar cells while its operation mechanism remains unclear. Here we investigate the process for the conversion of light to electrical current in high performance layered perovskite solar cells by examining its real morphology. The layered perovskite films in this study are found to be a mixture of layered and three dimensional (3D)-like phases with phase separations at micrometer and nanometer scale in both vertical and lateral directions. This phase separation is explained by the surface initiated crystallization process and the competition of the crystallization between 3D-like and layered perovskites.more » We further propose that the working mechanisms of the layered perovskite solar cells involve energy transfer from layered to 3D-like perovskite network. The impact of morphology on efficiency and stability of the hot-cast layered perovskite solar cells are also discussed to provide guidelines for the future improvement.« less

Abstract The high crystallinity and ability to harvest near‐infrared photons make diketopyrrolopyrrole (DPP)‐based polymers one of the most promising donors for high performing organic solar cells (OSCs). However, DPP‐based OSC devices still suffer from the trade‐off between energetic loss ( E _loss ) and maximum external quantum efficiency (EQE _max ), which significantly hinders their potential. Thus far, the replacement of fullerenes with small molecule acceptors did not wisdom the performance development of DPP‐donor‐based solar cells due to severe charge recombination issues. In this work, efficient DPP‐based solar cells are reported using low bandgap fused ring electron acceptor, IEICO‐4F. PBDTT‐DPP:IEICO‐4Fmore » OSC devices deliver a champion power conversion efficiency of 9.66% with successful interface engineering along with low E _loss of 0.57 eV and a high EQE _max (>70%).« less

Two-dimensional perovskites have emerged as more intrinsically stable materials for solar cells. Chemical tuning of spacer organic cations has attracted great interest due to their additional functionalities. However, how the chemical nature of the organic cations affects the properties of two-dimensional perovskites and devices is rarely reported. Here we demonstrate that the selection of spacer cations (i.e., selective fluorination of phenethylammonium) affects the film properties of two-dimensional perovskites, leading to different device performance of two-dimensional perovskite solar cells (average n = 4). Structural analysis reveals that different packing arrangements and orientational disorder of the spacer cations result in orientational degeneracymore » and different formation energies, largely explaining the difference in film properties. This work provides key missing information on how spacer cations exert influence on desirable electronic properties and device performance of two-dimensional perovskites via the weak and cooperative interactions of these cations in the crystal lattice.« less

Abstract N‐type organic small molecules (SMs) are attracting attention in the organic electronics field, due to their easy purification procedures with high yield. However, only a few reports show SMs that perform well in both organic field‐effect transistors (OFETs) and organic solar cells (OSCs). Here, the synthesis and characterization of an n‐type small molecule with an indacenodithieno[3,2‐b]thiophene (IDTT) core unit and linear alkylated side chain (C ₁₆ ) (IDTTIC) are reported. Compared to the state‐of‐the‐art n‐type molecule IDTIC, IDTTIC exhibits smaller optical bandgap and higher absorption coefficient, which is due to the enhanced intramolecular effect. After mixing with the polymermore » donor PBDB‐T, IDTIC‐based solar cells deliver a power conversion efficiency of only 5.67%. In stark contrast, the OSC performance of IDTTIC improves significantly to 11.2%. It is found that the superior photovoltaic properties of PBDB‐T:IDTTIC blends are mainly due to reduced trap‐assisted recombination and enhanced molecular packing coherence length and higher domain purity when compared to IDTIC. Moreover, a significantly higher electron mobility of 0.50 cm ² V ⁻¹ s ⁻¹ for IDTTIC in OFET devices than for IDTIC (0.15 cm ² V ⁻¹ s ⁻¹ ) is obtained. These superior performances in OSCs and OFETs demonstrate that SMs with extended π‐conjugation of the backbone possess a great potential for application in organic electronic devices.« less