RESUMEN
Developing a new end group for synthesizing asymmetric small molecule acceptors (SMAs) is crucial for achieving high-performance organic photovoltaics (OPVs). Herein, an asymmetric small molecule acceptor, BTP-BO-4FO, featuring a new difluoro-methoxylated end-group is reported. Compared to its symmetric counterpart L8-BO, BTP-BO-4FO exhibits an upshifted energy level, larger dipole moment, and more sequential crystallinity. By adopting two representative and widely available solvent additives (1-chloronaphthalene (CN) and 1,8-diiodooctane (DIO)), the device based on PM6:BTP-BO-4FO (CN) photovoltaic blend demonstrates a power conversion efficiency (PCE) of 18.62% with an excellent open-circuit voltage (VOC) of 0.933 V, which surpasses the optimal result of L8-BO. The PCE of 18.62% realizes the best efficiencies for binary OPVs based on SMAs with asymmetric end groups. A series of investigations reveal that optimized PM6:BTP-BO-4FO film demonstrates similar molecular packing motif and fibrillar phase distribution as PM6:L8-BO (DIO) does, resulting in comparable recombination dynamics, thus, similar fill factor. Besides, it is found PM6:BTP-BO-4FO possesses more efficient charge generation, which yields better VOC-JSC balance. This study provides a new ending group that enables a cutting-edge efficiency in asymmetric SMA-based OPVs, enriching the material library and shed light on further design ideas.
RESUMEN
The central core in A-DA1 D-A-type small-molecule acceptor (SMAs) plays an important role in determining the efficiency of organic solar cells (OSCs), while the principles governing the efficient design of SMAs remain elusive. Herein, we developed a series of SMAs with pyrido[2,3-b]quinoxaline (PyQx) as new electron-deficient unit by combining with the cascade-chlorination strategy, namely Py1, Py2, Py3, Py4 and Py5. The introduction of chlorine atoms reduces the intramolecular charge transfer effects but elevates the LUMO values. Density functional theory (DFT) reveals that Py2 with ortho chlorine substituted PyQx and Py5 with two chlorine atoms yield larger dipole moments and smaller πâ â â π stacking distances, as compared with the other three acceptors. Moreover, Py2 shows the strongest light absorption capability induced by extended orbit overlap lengths and more efficient packing structures in the dimers. These features endow the best device performance of Py2 due to the better molecular packing and aggregation behaviors, more suitable domain sizes with better exciton dissociation and charge recombination. This study highlights the significance of incorporating large dipole moments, small πâ â â π stacking distances and extended orbit overlap lengths in dimers into the development of high-performance SMAs, providing insight into the design of efficient A-DA1 D-A-type SMAs for OSCs.
RESUMEN
To boost the stability of all-small-molecule (ASM) organic photovoltaic (OPV) blends, an insulator polymer called styrene-ethylene-butylene-styrene (SEBS) as morphology stabilizer is applied into the host system of small molecules BM-ClEH:BO-4Cl. Minor addition of SEBS (1 mg/ml in host solution) provides a significantly enhanced T80 value of 15000 hours (extrapolated), surpassing doping-free (0 mg/ml) and heavy doping (10 mg/ml) counterparts (900 hours, 30 hours). The material reproducibility and cost-effectiveness of the active layer will not be affected by this industrially available polymer, where the power conversion efficiency (PCE) can be well maintained at 15.02%, which is still a decent value for non-halogen solvent-treated ASM OPV. Morphological and photophysical characterizations clearly demonstrate SEBS's pivotal effect on suppressing the degradation of donor molecules and blend film's crystallization/aggregation reorganization, which protects the exciton dynamics effectively. This work pays meaningful attention to the ASM system stability, performs a smart strategy to suppress the film morphology degradation, and releases a comprehensive understanding of the mechanism of device performance reduction.
RESUMEN
Using two structurally similar polymer acceptors in constructing high-efficiency ternary all-polymer solar cells is a widely acknowledged strategy; however, the focus thus far has not been on how polymer acceptor(s) would tune the aggregation of polymer donors, and furthermore film morphology and device performance (efficiency and stability). Herein, it is reported that matching of the celebrity acceptor PY-IT and the donor PBQx-TCl results in enhanced H-aggregation in PBQx-TCl, which can be finely tuned by controlling the amount of the second acceptor PY-IV. Consequently, the efficiency-optimized PY-IV weight ratio (0.2/1.2) leads to a state-of-the-art power conversion efficiency of 18.81%, wherein light-illuminated operational stability is also enhanced along with well-protected thermal stability. Such enhancements in the efficiency and operational and thermal stabilities of solar cells can be attributed to morphology optimization and the desired glass transition temperature of the target active layer based on comprehensive characterization. In addition to being a high-power conversion efficiency case for all-polymer solar cells, these enhancements are also a successful attempt for using combined acceptors to tune donor aggregation toward optimal morphology, which provides a theoretical basis for the construction of other types of organic photovoltaics beyond all-polymer solar cells.
RESUMEN
All-small-molecule organic solar cells with good batch-to-batch reproducibility combined with non-halogen solvent processing show great potential for commercialization. However, non-halogen solvent processing of all-small-molecule organic solar cells are rarely reported and its power conversion efficiencies are very difficult to improve. Herein, we designed and synthesized a small molecule donor BM-ClEH that can take advantage of strong aggregation property induced by intramolecular chlorine-sulfur non-covalent interaction to improve molecular pre-aggregation in tetrahydrofuran and corresponding micromorphology after film formation. Tetrahydrofuran-fabricated all-small-molecule organic solar cells based on BM-ClEH:BO-4Cl achieved high power conversion efficiencies of 15.0% in binary device and 16.1% in ternary device under thermal annealing treatment. In contrast, weakly aggregated BM-HEH without chlorine-sulfur non-covalent bond is almost inefficient under same processing conditions due to poor pre-aggregation induced disordered π-π stacking, indistinct phase separation and exciton dissociation. This work promotes the development of non-halogen solvent processing of all-small-molecule organic solar cells and provides further guidance.
RESUMEN
The exploration of high-performance and low-cost wide-bandgap polymer donors remains critical to achieve high-efficiency nonfullerene organic solar cells (OSCs) beyond current thresholds. Herein, the 1,2,3-benzothiadiazole (iBT), which is an isomer of 2,1,3-benzothiadiazole (BT), is used to design wide-bandgap polymer donor PiBT. The PiBT-based solar cells reach efficiency of 19.0%, which is one of the highest efficiencies in binary OSCs. Systemic studies show that isomerization of BT to iBT can finely regulate the polymers' photoelectric properties including i) increasing the extinction coefficient and photon harvest, ii) downshifting the highest occupied molecular orbital energy levels, iii) improving the coplanarity of polymer backbones, iv) offering good thermodynamic miscibility with acceptors. Consequently, the PiBT:Y6 bulk heterojunction (BHJ) device simultaneously reaches advantageous nanoscale morphology, efficient exciton generation and dissociation, fast charge transportation, and suppressed charge recombination, leading to larger VOC of 0.87 V, higher JSC of 28.2 mA cm-2, greater fill factor of 77.3%, and thus higher efficiency of 19.0%, while the analog-PBT-based OSCs reach efficiency of only 12.9%. Moreover, the key intermediate iBT can be easily afforded from industry chemicals via two-step procedure. Overall, this contribution highlights that iBT is a promising motif for designing high-performance polymer donors.
RESUMEN
Near-infrared (NIR) organic photodetectors (OPDs), particularly all-polymer-based ones, hold substantial commercial promise in the healthcare and imaging sectors. However, the process of optimizing their active layer composition to achieve highly competitive figures of merit lacks a clear direction and methodology. In this work, celebrity polymer acceptor PY-IT into a more NIR absorbing host system PBDB-T:PZF-V, to significantly enhance the photodetection competence, is introduced. The refined all-polymer ternary broadband photodetector demonstrates superior performance metrics, including experimentally measured noise current as low as 6 fA Hz-1/2, specific detectivity reaching 8 × 1012 Jones, linear dynamic range (LDR) of 145 dB, and swift response speed surpassing 200 kHz, striking a fair balance between sensitivity and response speed. Comprehensive morphological and photophysical characterizations elucidate the mechanisms behind the observed performance enhancements in this study, which include reduced trap density, enhanced charge transport, diminished charge recombination, and balanced electron/hole mobilities. Moreover, the practical deployment potential of the proof-of-concept device in self-powered mode is demonstrated through their application in a machine learning-based cuffless blood pressure (BP) estimation system and in high-resolution computational imaging across complex environments, where they are found to quantitatively rival commercial silicon diodes.
RESUMEN
Single-component organic solar cells based on double cable polymers have achieved remarkable performance, with DCPY2 reaching a high efficiency of over 13%. In this study, DCPY2 is further optimized with an efficiency of 13.85%, maintaining a high fill factor (FF) without compromising the short circuit current. Despite its intermixed morphology, DCPY2 shows a reduced recombination rate compared to their binary counterpart (PBDB-T:Y-O6). This slower recombination in DCPY2 is attributed to the reduced wavefunction overlap of delocalized charges, achieved by spatially separating the donor and acceptor units with an alkyl linker, thereby restricting the recombination pathways. Adding 1,8-diiodooctane (DIO) into DCPY2 further reduced the recombination rate by facilitating acceptor aggregation, allowing free charges to become more delocalized. The DIO-assisted aggregation in DCPY2 (5% DIO) is evidenced by an increased pseudo-pure domain size of Y-O6. Fine molecular control at the donor/acceptor interface in the double-cable polymer achieves reduced non-geminate recombination under efficient charge generation, increased mobility, and charge carrier lifetime, thereby achieving superior performance. Nevertheless, the FF is still limited by relatively low mobility compared to the blend, suggesting the potential for further mobility improvement through enhanced higher-dimensional packing of the double-cable material.
RESUMEN
All-polymer solar cells (All-PSCs) are considered the most promising candidate in achieving both efficient and stable organic photovoltaic devices, yet the field has rarely presented an in-depth understanding of corresponding device stability while efficiency is continuously boosted via the innovation of polymer acceptors. Herein, a ternary matrix is built for all-PSCs with optimized morphology, improved film ductility and importantly, boosted efficiency and better operational stability than its parental binary counterparts, as a platform to study the underlying mechanism. The target system PQM-Cl:PTQ10:PY-IT (0.8:0.2:1.2) exhibits an alleviated burn-in loss of morphology and efficiency under light soaking, which supports its promoted device lifetime. The comprehensive characterizations of fresh and light-soaked active layers lead to a clear illustration of opposite morphological and physical degradation direction of PQM-Cl and PTQ10, thus resulting in a delicate balance at the optimal ternary system. Specifically, the enlarging tendency of PQM-Cl and shrinking preference of PTQ10 in terms of phase separation leads to a stable morphology in their mixing phase; the hole transfer kinetics of PQM-Cl:PY-IT host is stabilized by incorporating PTQ10. This work succeeds in reaching a deep insight into all-PSC's stability promotion by a rational ternary design, which booms the prospect of gaining high-performance all-PSCs.
RESUMEN
With plenty of popular and effective ternary organic solar cells (OSCs) construction strategies proposed and applied, its power conversion efficiencies (PCEs) have come to a new level of over 19% in single-junction devices. However, previous studies are heavily based in chloroform (CF) leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component. Herein, we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy, named BTP-BO-3FO with enlarged bandgap, brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9, processed by CF and ortho-xylene (o-XY). With detailed analyses supported by a series of experiments, the best PCE of 19.24% for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif, which furthermore nourishes a favorable charge generation and recombination behavior. Likewise, over 19% PCE can be achieved by replacing spin-coating with blade coating for active layer deposition. This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance, hence, will be instructive to other ternary OSC works in the future.
RESUMEN
Laboratory-scale all-polymer solar cells (all-PSCs) have exhibited remarkable power conversion efficiencies (PCEs) exceeding 19%. However, the utilization of hazardous solvents and nonvolatile liquid additives poses challenges for eco-friendly commercialization, resulting in the trade-off between device efficiency and operation stability. Herein, an innovative approach based on isomerized solid additive engineering is proposed, employing volatile dithienothiophene (DTT) isomers to modulate intermolecular interactions and facilitate molecular stacking within the photoactive layers. Through elucidating the underlying principles of the DTT-induced polymer assembly on molecular level, a PCE of 18.72% is achieved for devices processed with environmentally benign solvents, ranking it among the highest record values for eco-friendly all-PSCs. Significantly, such superiorities of the DTT-isomerized strategy afford excellent compatibility with large-area blade-coating techniques, offering a promising pathway for industrial-scale manufacturing of all-PSCs. Moreover, these devices demonstrate enhanced thermal stability with a promising extrapolated T80 lifetime of 14 000 h, further bolstering their potential for sustainable technological advancement.
RESUMEN
Currently, nearly all high-efficiency organic photovoltaic devices use donor polymers based on the benzo-dithiophene (BDT) unit. To diversify the choices of building blocks for high-performance donor polymers, the use of benzo-difuran (BDF) units is explored, which can achieve reduced steric hindrance, stronger molecular packing, and tunable energy levels. In previous research, the performance of BDF-based devices lagged behind those of BDT-based devices. In this study, a high efficiency (18.4%) is achieved using a BDF-based polymer donor, which is the highest efficiency reported for BDF donor materials to date. The high efficiency is enabled by a donor polymer (D18-Fu) and the aid of a solid additive (2-chloronaphthalene), which is the isomer of the commonly used additive 1-chloronaphthalene. These results revealed the significant effect of 2-chloronaphthalene in optimizing the morphology and enhancing the device parameters. This work not only provides a new building block that can achieve an efficiency comparable to dominant BDT units but also proposes a new solid additive that can replace the widely used 1-chloronaphthalene additive.