Iodinated Electron Acceptor with Significantly Extended Exciton Diffusion Length for Efficient Organic Photovoltaic Cells.

Iodination has unlocked new potentials in organic photovoltaics (OPVs). A newly designed and synthesized iodinated non-fullerene acceptor, BO-4I, showcases exceptional excitation delocalization property with the exciton diffusion length increased to 80 nm. The enhanced electron delocalization property is attributed to the larger atomic radius and electron orbit of the iodine atom, which facilitates the formation of intra-moiety excitations in the acceptor phase. This effectively circumvents the charge transfer state-related recombination mechanisms, leading to a substantial reduction in non-radiative energy loss (ΔEnr ). As a result, OPV cell based on PBDB-TF : BO-4I achieves an impressive efficiency of 18.9 % with a notable ΔEnr of 0.189 eV, markedly surpassing their fluorinated counterparts. This contribution highlights the pivotal role of iodination in reducing energy loss, thereby affirming its potential as a key strategy in the development of advanced next-generation OPV cells.

Optimizing Molecular Packing via Steric Hindrance for Reducing Non-Radiative Recombination in Organic Solar Cells.

Innovative molecule design strategy holds promise for the development of next-generation acceptor materials for efficient organic solar cells with low non-radiative energy loss (ΔEnr). In this study, we designed and prepared three novel acceptors, namely BTP-Biso, BTP-Bme and BTP-B, with sterically structured triisopropylbenzene, trimethylbenzene and benzene as side chains inserted into the shoulder of the central core. The progressively enlarged steric hindrance from BTP-B to BTP-Bme and BTP-Biso induces suppressed intramolecular rotation and altered the molecule packing mode in their aggregation states, leading to significant changes in absorption spectra and energy levels. By regulating the intermolecular π-π interactions, BTP-Bme possesses relatively reduced non-radiative recombination rate and extended exciton diffusion lengths. The binary device based on PB2 : BTP-Bme exhibits an impressive power conversion efficiency (PCE) of 18.5 % with a low ΔEnr of 0.19 eV. Furthermore, the ternary device comprising PB2 : PBDB-TF : BTP-Bme achieves an outstanding PCE of 19.3 %. The molecule design strategy in this study proposed new perspectives for developing high-performance acceptors with low ΔEnr in OSCs.

Completely Non-Fused Low-Cost Acceptor Enables Organic Photovoltaic Cells with 17 % Efficiency.

To meet the industrial requirements of organic photovoltaic (OPV) cells, it is imperative to accelerate the development of cost-effective materials. Thiophene-benzene-thiophene central unit-based acceptors possess the advantage of low synthetic cost, while their power conversion efficiency (PCE) is relatively low. Here, by incorporating a para-substituted benzene unit and 1st-position branched alkoxy chains with large steric hindrance, a completely non-fused non-fullerene acceptor, TBT-26, was designed and synthesized. The narrow band gap of 1.38 eV ensures the effective utilization of sunlight. The favorable phase separation morphology of TBT-26-based blend film facilitates the efficient exciton dissociation and charge transport in corresponding OPV cell. Therefore, the TBT-26-based small-area cell achieves an impressive PCE of 17.0 %, which is the highest value of completely non-fused OPV cells. Additionally, we successfully demonstrated the scalability of this design by fabricating a 28.8 cm2 module with a high PCE of 14.3 %. Overall, our work provides a practical molecular design strategy for developing high-performance and low-cost acceptors, paving the way for industrial applications of OPV technology.

Pyrrole-Based Fully Non-fused Acceptor for Efficient and Stable Organic Solar Cells.

Organic solar cells (OSCs) are still suffering from the low light utilization and unstable under ultraviolet irradiation. To tackle these challenges, we design and synthesize a non-fused acceptor based on 1-(2-butyloctyl)-1H-pyrrole as π-bridge unit, denoted as GS70, which serves as active layer in the front-cell for constructing tandem OSCs with a parallel configuration. Benefiting from the well-complementary absorption spectra with the rear-cell, GS70-based parallel tandem OSCs exhibit an improved photoelectron response over the range between 600-700 nm, yielding a high short-circuit current density of 28.4 mA cm-2. The improvement in light utilization translates to a power conversion efficiency of 19.4 %, the highest value among all parallel tandem OSCs. Notably, owing to the intrinsic stability of GS70, the manufactured parallel tandem OSCs retain 84.9 % of their initial PCE after continuous illumination for 1000 hours. Overall, this work offers novel insight into the molecular design of low-cost and stability non-fused acceptors, emphasizing the importance of adopting a parallel tandem configuration for achieving efficient light harvesting and improved photostability in OSCs.

Design of a Fully Non-Fused Bulk Heterojunction toward Efficient and Low-Cost Organic Photovoltaics.

To modulate the miscibility between donor and acceptor materials both possessing fully non-fused ring structures, a series of electron acceptors (A4T-16, A4T-31 and A4T-32) with different polar functional substituents were synthesized and investigated. The three acceptors show good planarity, high conformational stability, complementary absorption and energy levels with the non-fused polymer donor (PTVT-BT). Among them, A4T-32 possesses the strongest polar functional group and shows the highest surface energy, which facilitates morphological modulation in the bulk heterojunction (BHJ) blend. Benefiting from the proper morphology control method, an impressive power conversion efficiency (PCE) of approaching 16.0 % and a superior fill factor over 0.795 are achieved in the PTVT-BT : A4T-32-based organic photovoltaic cells with superior photoactive materials price advantage, which represent the highest value for the cells based on the non-fused blend films. Notably, this cell maintains ≈84 % of its initial PCE after nearly 2000 h under the continuous simulated 1-sun-illumination. In addition, the flexible PTVT-BT : A4T-32-based cells were fabricated and delivered a decent PCE of 14.6 %. This work provides an effective molecular design strategy for the non-fused non-fullerene acceptors (NFAs) from the aspect of bulk morphology control in fully non-fused BHJ layers, which is crucial for their practical applications.

Molecular Design for Vertical Phase Distribution Modulation in High-Performance Organic Solar Cells.

Component distribution within the photoactive layer dictates the morphology and electronic structure and substantially influences the performance of organic solar cells (OSCs). In this study, a molecular design strategy is introduced to manipulate component and energetics distribution by adjusting side-chain polarity. Two non-fullerene acceptors (NFAs), ITIC-16F and ITIC-E, are synthesized by introducing different polar functional substituents onto the side chains of ITIC. The alterations result in different distribution tendencies in the bulk heterojunction film: ITIC-16F with intensified hydrophobicity aligns predominantly with the top surface, while ITIC-E with strong hydrophilicity gravitates toward the bottom. This divergence directly impacts the vertical distribution of the excitation energy levels, thereby influencing the excitation kinetics over extended time periods and larger spatial ranges including enhanced diffusion-mediated exciton dissociation and stimulated charge carrier transport. Benefitting from the favorable energy distribution, the device incorporating ITIC-E into the PBQx-TF:eC9-2Cl blend showcases an impressive power conversion efficiency of 19.4%. This work highlights side-chain polarity manipulation as a promising strategy for designing efficient NFA molecules and underscores the pivotal role of spatial energetics distribution in OSC performance.

Design of Chlorinated Indaceno[1,2-b:5,6-b']dithiophene Acceptors toward Efficient Organic Photovoltaics.

Chlorinated modifications have been extensively employed to modulate the optoelectronic properties of π-conjugated materials. Herein, the Cl substitution in designing nonfullerene acceptors (NFAs) with various bandgaps is studied. Four narrow-bandgap electron acceptors (GS-40, GS-41, GS-42, and GS-43) were synthesized by tuning the electrostatic potential distributions of the molecular conjugated backbones. The optical absorption onset of these NFAs ranges from 900 to 1030 nm. Compared to the nonchlorinated analogue, the introduction of Cl atoms on the core of indaceno[1,2-b:5,6-b'] dithiophene (IDT) and π spacer results in an upward shift of the lowest unoccupied molecular orbital levels and induces a blue shift in the absorption spectra of the NFAs. This alteration facilitates achieving appropriate energy-level alignment and favorable bulk heterojunction morphology when blended with the widely used donor PBDB-TF. The PBDB-TF:GS-43-based solar cells show an optimal power conversion efficiency of 13.3%. This work suggests the potential of employing chlorine-modified IDT and thiophene units as fundamental building blocks for developing high-performance photoactive materials.

New Method for Preparing ZnO Layer for Efficient and Stable Organic Solar Cells.

Owing to outstanding optoelectronic properties and simple preparation, zinc oxide (ZnO) has widely been used in organic solar cells (OSCs). Although versatile cathode interface materials have been designed in past, ZnO remains indispensable owing to its excellent overall performance. Therefore, solving the persistent problem of residual amine reacting with non-fullerene acceptors will make ZnO superior over other materials, and thus improve the performance and energy budget of OSCs. Herein, a simple, effective, and economical method for removing residual amine in ZnO without distorting ZnO is reported. By accurately comparing the alkalinities of ZnO and residual amine, boric acid (BA) is selected as the amine-removing agent because of its suitable acidic dissociation constant. Moreover, the high water solubility of BA ensures that the post-cleaning process can be easily performed. The work function, electron extraction, and stability of cathode interface layer are optimized through rinsing them with BA. Consequently, the power conversion efficiency (PCE) and stability of OSCs under long-term illumination are significantly improved. The optimal 0.04 and 1.00 cm2  single-junction OSCs are based on PBDB-TF:HDO-4Cl:BTP-eC9 bulk heterojunction output 18.40% and 17.42% efficiencies, respectively. Furthermore, tandem OSCs based on the BA-treated ZnO exhibit a 19.56% PCE, demonstrating the reliability of this method.

Rational control of meniscus-guided coating for organic photovoltaics.

Meniscus-guided coating exhibiting outstanding depositing accuracy, functional diversity, and operating convenience is widely used in printing process of photovoltaic electronics. However, current studies about hydrodynamic behaviors of bulk heterojunction ink are still superficial, and the key dynamic parameter dominating film formation is still not found. Here, we establish the principle of accurately evaluate the Hamaker constant and reveal the critical effect of precursor film length in determining flow evolution, the polymer aggregation, and final morphology. A shorter precursor film is beneficial to restraining chain relaxation, enhancing molecular orientation and mobility. On the basis of our precursor film-length prediction method proposed in this work, the optimal coating speed can be accurately traced. Last, a 18.39% power conversion efficiency has been achieved in 3-cm2 cell based on bulk heterojunction fabricated by blade coating, which shows few reduce from 19.40% in a 0.04-cm2 cell based on spin coating.

Organic laser power converter for efficient wireless micro power transfer.

Wireless power transfer with collimated power transmission and efficient conversion provides an alternative charging mode for off-grid and portable micro-power electronics. However, charging micro-power electronics with low photon flux can be challenging for current laser power converters. Here we show laser power converters with organic photovoltaic cells with good performance for application in laser wireless power transfer. The laser selection strategy is established and the upper limit of efficiency is proposed. The organic laser power converters exhibit a 36.2% efficiency at a 660 nm laser with a photon flux of 9.5 mW cm-2 and achieve wireless micro power transfer with an output of 0.5 W on a 2 meter scale. This work shows the good performance of organic photovoltaic cells in constructing organic laser power converters and provides a potential solution for the wireless power transfer of micro-power electronics.

Large Steric Hindrance Enhanced Molecular Planarity for Low-Cost Non-Fused Electron Acceptors.

Designing efficient non-fused ring electron acceptors is of great importance in decreasing the material cost of organic photovoltaic cells (OPVs). It is a challenge to construct a planar molecular skeleton in non-fused molecules as there are many torsions between adjacent units. Here, we design two non-fused electron acceptors based on bithieno[3,2-b]thiophene units as core structures and study the impact of steric hindrance of substituents on molecular planarity. We use 2,4,6-triisopropylphenyl and 4-hexylphenyl groups to prepare ATTP-1 and ATTP-2, respectively. Our results suggest that the enhanced steric hindrance is beneficial for obtaining a more planar molecular configuration, which significantly increases the optical absorption and charge transport properties. The power conversion efficiency (PCE) of PBDB-TF:ATTP-1 combination (11.3%) is superior to that of PBDB-TF:ATTP-2 combination (3.7%). In addition, an impressive PCE of 10.7% is recorded in ATTP-1-based devices when a low-cost polythiophene donor PDCBT is used, which is an outstanding value in OPVs fabricated by non-fused donor/acceptor combinations. Our work demonstrates that modulation of the steric hindrance effect is of great significance to control the molecular planarity and thus obtain excellent photovoltaic performance of low-cost non-fused electron acceptors.

Influence of Large Steric Hinderance Substituent Position on Conformation and Charge Transfer Process for Non-Fused Ring Acceptors.

To obtain stable and planar molecular geometry in non-fused electron acceptors, A4T-25 and A4T-26 are designed and synthesized by introducing the bulk 2,4,6-triisopropylphenyl side groups onto different positions of the central two thiophene units. A4T-25 and A4T-26 both show a narrow-bandgap of 1.39 and 1.46 eV, with highest occupied molecular orbital/lowest unoccupied molecular orbital levels of -5.56/-3.81 and -5.65/-3.83 eV, respectively, and the electrostatic potential distributions imply that they have strong electron-accepting capability. The single crystal structure analysis and the transfer integral calculation demonstrate that the much more compact π-π stacking in A4T-26 can promote efficient charge transportation compared to that in A4T-25. Therefore, the electron mobility of A4T-26 is obviously higher and more balanced than that of A4T-25. When blending the two acceptors with the same polymer donor PBDB-TF, the photovoltaic cell based on PBDB-TF:A4T-25 has an inadequate power conversion efficiency (PCE) of 7.83%, while the PBDB-TF:A4T-26-based one yields an enhanced PCE of 12.1%. Overall, this study offers an insight into the relationship between the fine-tuning of the molecular structure of non-fused ring acceptors and the corresponding charge transfer process in organic solar cells.

A High-Performance Nonfused Wide-Bandgap Acceptor for Versatile Photovoltaic Applications.

Wide-bandgap (WBG) nonfullerene acceptors (NFAs) with nonfused conjugated structures play a critical role in organic photovoltaic (OPV) cells. Here, NFAs named GS-OEH, GS-OC6, and GS-ISO, with optical bandgaps larger than 1.70 eV, are synthesized without using the fused ring structures. Compared with GS-OEH and GS-OC6, GS-ISO exhibits much stronger crystallinity, leading to a smaller energetic disorder and a larger exciton diffusion coefficient. GS-ISO also possesses a higher electroluminescence external quantum efficiency of 1.0 × 10-2 . The OPV cell based on PBDB-TF:GS-ISO demonstrates a power conversion efficiency (PCE) of 11.62% under the standard one sun illumination. Besides, the PBDB-TF:GS-ISO-based cell with effective area of 1.0 cm2  exhibits a PCE of 28.37% under 2700 K illumination of 500 lux. A tandem OPV cell using PBDB-TF:GS-ISO as the front subcell shows an outstanding efficiency of 19.10%. Importantly, the GS-ISO-based OPV cell exhibits promising stability under the continuous illumination of simulated sunlight. This study indicates that the molecular design strategy demonstrated in this work has great superiority in developing nonfused NFAs and also that GS-ISO is a promising WBG acceptor for versatile photovoltaic applications.

Completely non-fused electron acceptor with 3D-interpenetrated crystalline structure enables efficient and stable organic solar cell.

Non-fullerene acceptors (NFAs) based on non-fused conjugated structures have more potential to realize low-cost organic photovoltaic (OPV) cells. However, their power conversion efficiencies (PCEs) are much lower than those of the fused-ring NFAs. Herein, a new bithiophene-based non-fused core (TT-Pi) featuring good planarity as well as large steric hindrance was designed, based on which a completely non-fused NFA, A4T-16, was developed. The single-crystal result of A4T-16 reveals that a three-dimensional interpenetrating network can be formed due to the compact π-π stacking between the adjacent end-capping groups. A high PCE of 15.2% is achieved based on PBDB-TF:A4T-16, which is the highest value for the cells based on the non-fused NFAs. Notably, the device retains ~84% of its initial PCE after 1300 h under the simulated AM 1.5 G illumination (100 mW cm-2). Overall, this work provides insight into molecule design of the non-fused NFAs from the aspect of molecular geometry control.

Suppressing Energetic Disorder Enables Efficient Indoor Organic Photovoltaic Cells With a PTV Derivative.

Indoor organic photovoltaics (IOPVs) cells have attracted considerable attention in the past few years. Herein, two PTV-derivatives, PTVT-V and PTVT-T, were used as donor materials to fabricate IOPV cells with ITCC as the acceptor. The preferred orientation of the crystals changed from edge-on to face-on after replacing the ethylene in the backbones of PTVT-V by the thiophene in that of PTVT-T. Besides, it was found that, the energetic disorder of the PTVT-T:ITCC based system is 58 meV, which is much lower than that of PTVT-V:ITCC-based system (70 meV). The lower energetic disorder in PTVT-T:ITCC leads to an efficient charge transfer, charge transport, and thus the weak charge recombination. As a result, a PCE of 9.60% under AM 1.5 G and a PCE of 24.27% under 1,000 lux (LED 2,700 K) with a low non-radiative energy loss of 0.210 eV were obtained based on PTVT-T:ITCC blend. The results indicate that to improve the PTV-derivatives photovoltaic properties by suppressing the energetic disorder is a promising way to realize low-cost IOPV cells.

Molecular design revitalizes the low-cost PTV-polymer for highly efficient organic solar cells.

Developing photovoltaic materials with simple chemical structures and easy synthesis still remains a major challenge in the industrialization process of organic solar cells (OSCs). Herein, an ester substituted poly(thiophene vinylene) derivative, PTVT-T, was designed and synthesized in very few steps by adopting commercially available raw materials. The ester groups on the thiophene units enable PTVT-T to have a planar and stable conformation. Moreover, PTVT-T presents a wide absorption band and strong aggregation effect in solution, which are the key characteristics needed to realize high performance in non-fullerene-acceptor (NFA)-based OSCs. We then prepared OSCs by blending PTVT-T with three representative fullerene- and NF-based acceptors, PC71BM, IT-4F and BTP-eC9. It was found that PTVT-T can work well with all the acceptors, showing great potential to match new emerging NFAs. Particularly, a remarkable power conversion efficiency of 16.20% is achieved in a PTVT-T:BTP-eC9-based device, which is the highest value among the counterparts based on PTV derivatives. This work demonstrates that PTVT-T shows great potential for the future commercialization of OSCs.

Single-Junction Organic Photovoltaic Cell with 19% Efficiency.

Improving power conversion efficiency (PCE) is important for broadening the applications of organic photovoltaic (OPV) cells. Here, a maximum PCE of 19.0% (certified value of 18.7%) is achieved in single-junction OPV cells by combining material design with a ternary blending strategy. An active layer comprising a new wide-bandgap polymer donor named PBQx-TF and a new low-bandgap non-fullerene acceptor (NFA) named eC9-2Cl is rationally designed. With optimized light utilization, the resulting binary cell exhibits a good PCE of 17.7%. An NFA F-BTA3 is then added to the active layer as a third component to simultaneously improve the photovoltaic parameters. The improved light unitization, cascaded energy level alignment, and enhanced intermolecular packing result in open-circuit voltage of 0.879 V, short-circuit current density of 26.7 mA cm-2 , and fill factor of 0.809. This study demonstrates that further improvement of PCEs of high-performance OPV cells requires fine tuning of the electronic structures and morphologies of the active layers.

Intra- and Intermolecular Steric Hindrance Effects Induced Higher Open-Circuit Voltage and Power Conversion Efficiency.

A pair of donor-acceptor polymers PBDThDTBT and PBDTchDTBT are synthesized, which share the same conjugated backbone, but are designed with hexyl and cyclohexyl side chains, respectively. The stronger steric hindrance of cyclohexyl endows PBDTchDTBT a deeper lying HOMO energy level of -5.39 eV compared to -5.22 eV for PBDThDTBT. However, PBDThDTBT and PBDTchDTBT exhibit a similar optical bandgap around 1.72 eV and a hole mobility around 10-5 cm2 V-1 s-1. Interestingly, the PBDTchDTBT/PC71BM blends exhibited higher hole mobility than PBDThDTBT/PC71BM after DIO was added. The higher hole mobility and fibrillar network in the active layer endows PBDTchDTBT higher power conversion efficiency of 7.9%, together with simultaneously improved open-circuit voltage of 0.80 V, short-circuit current density of 13.50 mA cm-2, and fill factor of 72.74% after a systemic study of their solar cell devices.