Multifold Enhanced Photon Upconversion in a Composite Annihilator System Sensitized by Perovskite Nanocrystals.

Photon upconversion via triplet-triplet annihilation (TTA-UC) provides a pathway to overcoming the thermodynamic efficiency limits in single-junction solar cells by allowing the harvesting of sub-bandgap photons. Here, we use mixed halide perovskite nanocrystals (CsPbX3, X = Br/I) as triplet sensitizers, with excitation transfer to 9,10-diphenylanthracene (DPA) and/or 9,10-bis[(triisopropylsilyl)ethynyl]anthracene (TIPS-An) which act as the triplet annihilators. We observe that the upconversion efficiency is five times higher with the combination of both annihilators in a composite system compared to the sum of the individual single-acceptor systems. Our work illustrates the importance of using a composite system of annihilators to enhance TTA upconversion, demonstrated in a perovskite-sensitized system, with promise for a range of potential applications in light-harvesting, biomedical imaging, biosensing, therapeutics, and photocatalysis.

Regulating Phase Separation Kinetics for High-Efficiency and Mechanically Robust All-Polymer Solar Cells.

All-polymer solar cells (all-PSCs) possess excellent operation stability and mechanical robustness than other types of organic solar cells, thereby attracting considerable attention for wearable flexible electron devices. However, the power conversion efficiencies (PCEs) of all-PSCs are still lagging behind those of small-molecule-acceptor-based systems owing to the limitation of photoactive materials and unsatisfactory blend morphology. In this work, a novel terpolymer, denoted as PBDB-TFCl (poly4,8-bis(5-(2-ethylhexyl)-4-fluorothiophen-2-yl)benzo[1,2-b:4,5-b″]dithiophene-1,3-bis(2-ethylhexyl)-5,7-di(thiophen-2-yl)-4H,8H-benzo[1,2-c:4,5-c″]dithiophene-4,8-dione-4,8-bis(4-chloro-5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene), is used as an electron donor coupled with a ternary strategy to optimize the performance of all-PSCs. The addition of PBDB-TCl unit deepens the highest occupied molecular orbital energy level, reducing voltage losses. Moreover, the introduction of the guest donor (D18-Cl) effectively regulates the phase-transition kinetics of PBDB-TFCl:D18-Cl:PY-IT during the film formation, leading to ideal size of aggregations and enhanced crystallinity. PBDB-TFCl:D18-Cl:PY-IT devices exhibit a PCE of 18.6% (certified as 18.3%), judged as the highest value so far obtained with all-PSCs. Besides, based on the ternary active layer, the manufactured 36 cm2 flexible modules exhibit a PCE of 15.1%. Meanwhile, the ternary PSCs exhibit superior photostability and mechanical stability. In summary, the proposed strategy, based on molecular design and the ternary strategy, allows optimization of the all-polymer blend morphology and improvement of the photovoltaic performance for stable large-scale flexible PSCs.

Low-Cost Fully Non-fused Ring Acceptor Enables Efficient Organic Photovoltaic Modules for Multi-Scene Applications.

Organic photovoltaic (OPV) cells, with highly tunable light-response ranges, offer significant potential for use in driving low-power consumption off-grid electronics in multi-scenarios. However, development of photoactive layer materials that can meet simultaneously the requirements of diverse irradiation conditions is a still challenging task. Herein, a low-cost fully non-fused acceptor (denoted as GS60) featuring well-matched absorption spectra with solar, scattered light and artificial light radiation was designed and synthesized. Systematic characterizations revealed that GS60 possessed outstanding photoelectron properties and ideal morphology, which resulted in reduced voltage loss and suppressed charge recombination. By blending with a non-fused ring polymer PTVT-T, the as-obtained GS60 based OPV cells achieved a good power conversion efficiency (PCE) of 14.1 %, a high value for the cells based on non-fused ring bulk heterojunction. Besides, manufactured large-area OPV modules based on PTVT-T:GS60 yielded PCEs of 11.2 %, 11.8 %, 12.1 %, 23.1 %, and 20.3 % under irradiation of AM 1.5G, natural light of cloudy weather, natural light in shadow, laser and indoor, respectively. The PTVT-T:GS60 devices exhibited considerable potential in terms of improving photostability and reducing material cost. Overall, this work provides novel insight into the molecular design of low-cost non-fused ring acceptors, and extended potential of medium band gap acceptors based OPV cells used in various application scenarios.

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.

Tandem organic solar cells with 20.6% efficiency enabled by reduced voltage losses.

Large voltage losses are the main obstacle for achieving high efficiency in organic solar cells (OSCs). Here we construct ternary OSCs by introducing an asymmetric small molecule acceptor AITC into PBDB-TCl : BTP-eC9 system and demonstrate the effectiveness in simultaneously decreasing energy disorder and non-radiative voltage losses. It is found that the introduction of AITC can modify domain size and increase the degree of crystallinity, which enhances open-circuit voltage and power conversion efficiency (19.1%, certified as 18.9%). Inspiringly, an output efficiency of 20.6% of the constructed tandem OSCs based on PBDB-TCl : AITC : BTP-eC9 ternary active layer output a recorded efficiency of 20.6% (certified as 20.3%), which is the highest value in OSCs field to date. This work demonstrates that decreasing the voltage losses by ternary strategy and constructing of tandem architecture are effective approaches towards improving photovoltaic performance.

Binary Organic Solar Cells with 19.2% Efficiency Enabled by Solid Additive.

Morphology optimization is critical for achieving high efficiency and stable bulk-heterojunction (BHJ) organic solar cells (OSCs). Herein, the use of 3,5-dichlorobromobenzene (DCBB) with high volatility and low cost to manipulate evolution of the BHJ morphology and improve the operability and photostability of OSCs is proposed. Systematic simulations reveal the charge distribution of DCBB and its non-covalent interaction with the active layer materials. The addition of DCBB can effectively tune the aggregation of PBQx-TF:eC9-2Cl during film formation, resulting in a favorable phase separation and a reinforced molecular packing. As a result, a power conversion efficiency of 19.2% (certified as 19.0% by the National Institute of Metrology) for DCBB-processed PBQx-TF:eC9-2Cl-based OSCs, which is the highest reported value for binary OSCs, is obtained. Importantly, the DCBB-processed devices exhibit superior photostability and have thus considerable application potential in the printing of large-area devices, demonstrating outstanding universality in various BHJ systems. The study provides a facile approach to control the BHJ morphology and enhances the photovoltaic performance of OSCs.

Enhancing Photon Utilization Efficiency for High-Performance Organic Photovoltaic Cells via Regulating Phase-Transition Kinetics.

Efficient photon utilization is key to achieving high-performance organic photovoltaic (OPV) cells. In this study, a multiscale fibril network morphology in a PBQx-TCl:PBDB-TF:eC9-2Cl-based system is constructed by regulating donor and acceptor phase-transition kinetics. The distinctive phase-transition process and crystal size are systematically investigated. PBQx-TCl and eC9-2Cl form fibril structures with diameters of ≈25 nm in ternary films. Additionally, fine fibrils assembled by PBDB-TF are uniformly distributed over the fibril networks of PBQx-TCl and eC9-2Cl. The ideal multiscale fibril network morphology enables the ternary system to achieve superior charge transfer and transport processes compared to binary systems; these improvements promote enhanced photon utilization efficiency. Finally, a high power conversion efficiency of 19.51% in a single-junction OPV cell is achieved. The external quantum efficiency of the optimized ternary cell exceeds 85% over a wide range of 500-800 nm. A tandem OPV cell is also fabricated to increase solar photon absorption. The tandem cell has an excellent PCE of more than 20%. This study provides guidance for constructing an ideal multiscale fibril network morphology and improving the photon utilization efficiency of OPV cells.

A Medium-Bandgap Nonfullerene Acceptor Enabling Organic Photovoltaic Cells with 30% Efficiency under Indoor Artificial Light.

The correlation between molecular structure and photovoltaic performance is lagging for constructing high-performance indoor organic photovoltaic (OPV) cells. Herein, this relationship is investigated in depth by employing two medium-bandgap nonfullerene acceptors (NFAs). The newly synthesized NFA of FTCCBr exhibits a similar bandgap and molecular energy level, but a much stronger dipole moment and larger average electrostatic potential (ESP) compared with ITCC. After blending with the polymer donor PB2, the PB2:ITCC and PB2:FTCCBr blends exhibit favorable bulk-heterojunction morphologies and the same driving force, but the PB2:FTCCBr blend exhibits a large ESP difference. In OPV cells, the PB2:ITCC-based device produces a power conversion efficiency (PCE) of 11.0%, whereas the PB2:FTCCBr-based device gives an excellent PCE of 14.8% with an open-circuit voltage (VOC ) of 1.05 V, which is the highest value among OPV cells with VOC values above 1.0 V. When both acceptor-based devices work under a 1000 lux of 3000 K light-emitting diode, the PB2:ITCC-based 1 cm2 device yields a good PCE of 25.4%; in contrast, the PB2:FTCCBr-based 1 cm2 device outputs a record PCE of 30.2%. These results suggest that a large ESP offset in photovoltaic materials is important for achieving high-performance OPV cells.

A New Polymer Donor Enables Binary All-Polymer Organic Photovoltaic Cells with 18% Efficiency and Excellent Mechanical Robustness.

The development of polymerized small-molecule acceptors has boosted the power conversion efficiencies (PCEs) of all-polymer organic photovoltaic (OPV) cells to 17%. However, the polymer donors suitable for all-polymer OPV cells are still lacking, restricting the further improvement of their PCEs. Herein, a new polymer donor named PQM-Cl is designed and its photovoltaic performance is explored. The negative electrostatic potential and low average local ionization energy distribution of the PQM-Cl surface enable efficient charge generation and transfer process. When blending with a well-used polymer acceptor, PY-IT, the PQM-Cl-based devices deliver an impressive PCE of 18.0% with a superior fill factor of 80.7%, both of which are the highest values for all-polymer OPV cells. The relevant measurements demonstrate that PQM-Cl-based films possess excellent mechanical and flexible properties. As such, PQM-Cl-based flexible photovoltaic cells are fabricated and an excellent PCE of 16.5% with high mechanical stability is displayed. These results demonstrate that PQM-Cl is a potential candidate for all-polymer OPV cells and provide insights into the design of polymer donors for high-efficient all-polymer OPV cells.

A Universal Nonhalogenated Polymer Donor for High-Performance Organic Photovoltaic Cells.

Nonhalogenated polymers have great potential in the commercialization of organic photovoltaic (OPV) cells due to their advantage in low-cost preparation. However, non-halogenated polymers usually have high highest occupied molecular orbital (HOMO) energy levels and inferior self-aggregation properties in solution, thus resulting in low power conversion efficiencies (PCEs). Herein, two nonhalogenated polymers, PB1 and PB2, are prepared. When the polymers are used to fabricate OPV cells with BTP-eC9, the PB1-based device only gives a PCE of 5.3%, while the PB2-based device shows an outstanding PCE of 17.7%. After the introduction of PBDB-TF as the third component, the PB2:PBDB-TF:BTP-eC9-based device with an optimal weight ratio of 0.5:0.5:1 achieves a PCE up to 18.4%. More importantly, PB2 exhibits good compatibility with various nonfullerene acceptors to achieve better PCEs than those of classical polymer (PBDB-T and PBDB-TF)-based devices. When PB2 is combined with a wide-bandgap electron acceptor (F-BTA3), this device shows excellent PCE of 27.1% and 24.6% for 1 and 10 cm2 devices, respectively, under light intensity of 1000 lux light-emitting diode illumination. These results provide new insight in the rational design of novel nonhalogenated polymer donors for further development of low-cost materials and broadening the application of OPV 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.

18.5% Efficiency Organic Solar Cells with a Hybrid Planar/Bulk Heterojunction.

The donor:acceptor heterojunction has proved as the most successful approach to split strongly bound excitons in organic solar cells (OSCs). Establishing an ideal architecture with selective carrier transport and suppressed recombination is of great importance to improve the photovoltaic efficiency while remains a challenge. Herein, via tailoring a hybrid planar/bulk structure, highly efficient OSCs with reduced energy losses (Eloss s) are fabricated. A p-type benzodithiophene-thiophene alternating polymer and an n-type naphthalene imide are inserted on both sides of a mixed donor:acceptor active layer to construct the hybrid heterojunction, respectively. The tailored structure with the donor near the anode and the acceptor near the cathode is beneficial for obtaining enhanced charge transport, extraction, and suppressed charge recombination. As a result, the photovoltaic characterizations suggest a reduced nonradiative Eloss by 25 meV, and the best OSC records a high efficiency of 18.5% (certified as 18.2%). This study highlights that precisely regulating the structure of donor:acceptor heterojunction has the potential to further improve the efficiencies 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.

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.

Effect of the Energy Offset on the Charge Dynamics in Nonfullerene Organic Solar Cells.

The energy offset, considered as the driving force for charge transfer between organic molecules, has significant effects on both charge separation and charge recombination in organic solar cells. Herein, we designed material systems with gradually shifting energy offsets, including both positive and negative values. Time-resolved spectroscopy was used to monitor the charge dynamics within the bulk heterojunction. It is striking to find that there is still charge transfer and charge generation when the energy offset reached -0.10 eV (ultraviolet photoelectron spectroscopy data). This work not only indicates the feasibility of the free carrier generation and the following charge separation under the condition of a negative offset but also elucidates the relationship between the charge transfer and the energy offset in the case of polymer chlorination.

Organic photovoltaic cell with 17% efficiency and superior processability.

The development of organic photoactive materials, especially the newly emerging non-fullerene electron acceptors (NFAs), has enabled rapid progress in organic photovoltaic (OPV) cells in recent years. Although the power conversion efficiencies (PCEs) of the top-performance OPV cells have surpassed 16%, the devices are usually fabricated via a spin-coating method and are not suitable for large-area production. Here, we demonstrate that the fine-modification of the flexible side chains of NFAs can yield 17% PCE for OPV cells. More crucially, as the optimal NFA has a suitable solubility and thus a desirable morphology, the high efficiencies of spin-coated devices can be maintained when using scalable blade-coating processing technology. Our results suggest that optimization of the chemical structures of the OPV materials can improve device performance. This has great significance in larger-area production technologies that provide important scientific insights for the commercialization of OPV cells.

Hole Transfer Originating from Weakly Bound Exciton Dissociation in Acceptor-Donor-Acceptor Nonfullerene Organic Solar Cells.

The underlying hole-transfer mechanism in high-efficiency OSC bulk heterojunctions based on acceptor-donor-acceptor (A-D-A) nonfullerene acceptors (NFAs) remains unclear. Herein, we study the hole-transfer process between copolymer donor J91 and five A-D-A NFAs with different highest occupied molecular orbital energy offsets (ΔEH) (0.05-0.42 eV) via ultrafast optical spectroscopies. Transient absorption spectra reveal a rapid hole-transfer rate with small ΔEH, suggesting that a large energy offset is not required to overcome the exciton binding energy. Capacitance-frequency spectra and time-resolved photoluminescence spectra confirm the delocalization of an A-D-A-structured acceptor exciton with weak binding energy. Relative to the hole-transfer rate, hole-transfer efficiency is the key factor affecting device performance. We propose that holes primarily stem from weakly bound acceptor exciton dissociation, revealing a new insight into the hole-transfer process in A-D-A NFA-based OSCs.

Morphology Control Enables Efficient Ternary Organic Solar Cells.

Ternary organic solar cells are promising alternatives to the binary counterpart due to their potential in achieving high performance. Although a growing number of ternary organic solar cells are recently reported, less effort is devoted to morphology control. Here, ternary organic solar cells are fabricated using a wide-bandgap polymer PBT1-C as the donor, a crystalline fused-ring electron acceptor ITIC-2Cl, and an amorphous fullerene derivative indene-C60 bisadduct (ICBA) as the acceptor. It is found that ICBA can disturb π-π interactions of the crystalline ITIC-2Cl molecules in ternary blends and then help to form more uniform morphology. As a result, incorporation of 20% ICBA in the PBT1-C:ITIC-2Cl blend enables efficient charge dissociation, negligible bimolecular recombination, and balanced charge carrier mobilities. An impressive power conversion efficiency (PCE) of 13.4%, with a high fill factor (FF) of 76.8%, is eventually achieved, which represents one of the highest PCEs reported so far for organic solar cells. The results manifest that the adoption of amorphous fullerene acceptor is an effective approach to optimizing the ternary blend morphology and thereby increases the solar cell performance.