Solution-processed organic photovoltaics (OPV) offer the attractive prospect of low-cost, light-weight and environmentally benign solar energy production. The highest efficiency OPV at present use low-bandgap donor polymers, many of which suffer from problems with stability and synthetic scalability. They also rely on fullerene-based acceptors, which themselves have issues with cost, stability and limited spectral absorption. Here we present a new non-fullerene acceptor that has been specifically designed to give improved performance alongside the wide bandgap donor poly(3-hexylthiophene), a polymer with significantly better prospects for commercial OPV due to its relative scalability and stability. Thanks to the well-matched optoelectronic and morphological properties of these materials, efficiencies of 6.4% are achieved which is the highest reported for fullerene-free P3HT devices. In addition, dramatically improved air stability is demonstrated relative to other high-efficiency OPV, showing the excellent potential of this new material combination for future technological applications.
A novel small molecule, FBR, bearing 3-ethylrhodanine flanking groups was synthesized as a nonfullerene electron acceptor for solution-processed bulk heterojunction organic photovoltaics (OPV). A straightforward synthesis route was employed, offering the potential for large scale preparation of this material. Inverted OPV devices employing poly(3-hexylthiophene) (P3HT) as the donor polymer and FBR as the acceptor gave power conversion efficiencies (PCE) up to 4.1%. Transient and steady state optical spectroscopies indicated efficient, ultrafast charge generation and efficient photocurrent generation from both donor and acceptor. Ultrafast transient absorption spectroscopy was used to investigate polaron generation efficiency as well as recombination dynamics. It was determined that the P3HT:FBR blend is highly intermixed, leading to increased charge generation relative to comparative devices with P3HT:PC60BM, but also faster recombination due to a nonideal morphology in which, in contrast to P3HT:PC60BM devices, the acceptor does not aggregate enough to create appropriate percolation pathways that prevent fast nongeminate recombination. Despite this nonoptimal morphology the P3HT:FBR devices exhibit better performance than P3HT:PC60BM devices, used as control, demonstrating that this acceptor shows great promise for further optimization.
We report a general light processing strategy for organic solar cells (OSC) that exploits the propensity of the fullerene derivative PC60BM to photo-oligomerize, which is capable of both stabilizing the polymer:PC60BM active layer morphology and enhancing the device stability under thermal annealing. The observations hold for blends of PC60BM with an array of benchmark donor polymer systems, including P3HT, DPP-TT-T, PTB7, and PCDTBT. The morphology and kinetics of the thermally induced PC60BM crystallization within the blend films are investigated as a function of substrate and temperature. PC60BM nucleation rates on SiOx substrates exhibit a pronounced peak profile with temperature, whose maximum is polymer and blend-composition dependent. Modest illumination (<10 mW/cm(2)) significantly suppresses nucleation, which is quantified as function of dose, but does not affect crystalline shape or growth, in the micrometer range. On PEDOT:PSS substrates, thermally induced PC60BM aggregation is observed on smaller (≈ 100 nm) length scales, depending upon donor polymer, and also suppressed by light exposure. The concurrent thermal dissociation process of PC60BM oligomers in blend films is also investigated and the activation energy of the fullerene-fullerene bond is estimated to be 0.96 ± 0.04 eV. Following light processing, the thermal stability, and thus lifetime, of PCDTBT:PC60BM devices increases for annealing times up to 150 h. In contrast, PCDTBT:PC70BM OSCs are found to be largely light insensitive. The results are rationalized in terms of the suppression of PC60BM micro- and nanoscopic crystallization processes upon thermal annealing caused by photoinduced PC60BM oligomerization.
Nonfullerene solar cells have increased their efficiencies up to 13%, yet quantum efficiencies are still limited to 80%. Here we report efficient nonfullerene solar cells with quantum efficiencies approaching unity. This is achieved with overlapping absorption bands of donor and acceptor that increases the photon absorption strength in the range from about 570 to 700 nm, thus, almost all incident photons are absorbed in the active layer. The charges generated are found to dissociate with negligible geminate recombination losses resulting in a short-circuit current density of 20 mA cm−2 along with open-circuit voltages >1 V, which is remarkable for a 1.6 eV bandgap system. Most importantly, the unique nano-morphology of the donor:acceptor blend results in a substantially improved stability under illumination. Understanding the efficient charge separation in nonfullerene acceptors can pave the way to robust and recombination-free organic solar cells.
A key challenge to the commercialization of organic bulk heterojunction solar cells is the achievement of morphological stability, particularly under thermal stress conditions. Here we show that a low-level light exposure processing step during fabrication of blend polymer:PC 60 BM solar cells can result in a 10-fold increase in device thermal stability and, under certain conditions, enhanced device performance. The enhanced stability is linked to the light-induced oligomerization of PC 60 BM that effectively hinders their diffusion and crystallization in the blend. We thus suggest that light processing may be a promising, general and cost-effective strategy to optimize fullerene-based solar cell performance. The low level of light exposure required suggests not only that this may be an easily implementable strategy to enhance performance, but also that light-induced PC 60 BM oligomerization may have inadvertently influenced previous studies of organic solar cell device behaviour.
Despite the rapid developments in all‐polymer solar cells (all‐PSCs) due to the progress of polymerized small molecular acceptors (PSMA), the effect of linkage unit conjugation on the polymer acceptor (PA) is not well understood and PAs with high efficiency, good stability, and thickness‐insensitivity are rarely seen. Herein, two novel PSMAs, named PJTVT and PJTET are designed, by incorporating conjugated thienylene‐vinylene‐thienylene (TVT) and unconjugated thienylene–ethyl–thienylene (TET) units, respectively. Results show that the energy levels, energy losses, and energy offset of the two PSMAs have little difference (<≈0.03 eV). However, due to the π‐extended coplanar backbone of PJTVT, when blended with polymer donor JD40, a more ordered π–π stacking and enhanced face‐on orientation morphology is observed, which contributes to enhanced exciton dissociation, superior charge transport, and faster charge extraction, leading to a record power conversion efficiency of 16.13% (10.93% for JD40:PJTET). Impressively, the JD40:PJTVT device shows superior thickness‐insensitivity and long‐term stability, both of which make it an ideal choice for industrialization. These results demonstrate that molecular modulation in the linking unit is a promising strategy to construct PSMAs for high‐performance thick‐film all‐PSCs with superior long‐term stability, and shows the superiority of conjugated backbones for PSMAs.
Cost-effective, solution-processable organic photovoltaics (OPV) present an interesting alternative to inorganic silicon-based solar cells. However, one of the major remaining challenges of OPV devices is their lack of long-term operational stability, especially at elevated temperatures. The synthesis of a fullerene dumbbell and its use as an additive in the active layer of a PCDTBT:PCBM-based OPV device is reported. The addition of only 20 % of this novel fullerene not only leads to improved device efficiencies, but more importantly also to a dramatic increase in morphological stability under simulated operating conditions. Dynamic secondary ion mass spectrometry (DSIMS) and TEM are used, amongst other techniques, to elucidate the origins of the improved morphological stability.
The photochemistry and stability of fullerene films is found to be strongly dependent upon film nanomorphology. In particular, PCBM blend films, dispersed with polystyrene, are found to be more susceptible to photobleaching in air than the more aggregated neat films. This enhanced photobleaching correlated with increased oxygen quenching of PCBM triplet states and the appearance of a carbonyl FTIR absorption band indicative of fullerene oxidation, suggesting PCBM photo-oxidation is primarily due to triplet-mediated singlet oxygen generation. PCBM films were observed to undergo photo-oxidation in air for even modest (≤40 min) irradiation times, degrading electron mobility substantially, indicative of electron trap formation. This conclusion is supported by observation of red shifts in photo- and electro-luminescence with photo-oxidation, shown to be in agreement with time-dependent density functional theory calculations of defect generation. These results provide important implications on the environmental stability of PCBM-based films and devices.
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