Yingzhi Jin

Research into organic solar cells has gone from pure scientific curiosity to a topic of commercial relevance in the past few years, as a result of rapid development of non-fullerene acceptors. This transition is mainly driven by the development of new materials. Recently in Joule, Zou and co-workers developed a new acceptor material and reached a record efficiency for single-junction organic solar cells.

This research provides a structure-property relation that sheds light on morphological stability of NF-OSCs by using the thermodynamic and the kinetic perspectives. We show that NF-OSCs can suffer from excessive amorphous-amorphous phase separation in the blends and crystallization of NF-SMA. The former instability channel can be eliminated in systems with an optimal miscibility, whereas the excessive phase separation in low miscibility systems and NF-SMA crystallization need to be suppressed through the utilization of polymers or NF-SMAs with low flexibility.

A quantitative correlation between energetic disorder from charge transport and band bending measurements is established for two organic semiconducting polymers providing direct experimental evidence that charge carrier mobility is compromised due to the relaxation of charge carriers into the tail states of the density‐of‐states distribution. Ordered and disordered regions of polymer films were distinguished and quantified at an atomic‐scale.

Abstract

Characterizing the density of states (DOS) width accurately is critical in understanding the charge‐transport properties of organic semiconducting materials as broader DOS distributions lead to an inferior transport. From a morphological standpoint, the relative densities of ordered and disordered regions are known to affect charge‐transport properties in films; however, a comparison between molecular structures showing quantifiable ordered and disordered regions at an atomic level and its impact on DOS widths and charge‐transport properties has yet to be made. In this work, for the first time, the DOS distribution widths of two model conjugated polymer systems are characterized using three different techniques. A quantitative correlation between energetic disorder from band‐bending measurements and charge transport is established, providing direct experimental evidence that charge‐carrier mobility in disordered materials is compromised due to the relaxation of carriers into the tail states of the DOS. Distinction and quantification of ordered and disordered regions of thin films at an atomic level is achieved using solid‐state NMR spectroscopy. An ability to compare solid‐state film morphologies of organic semiconducting polymers to energetic disorder, and in turn charge transport, can provide useful guidelines for applications of organic conjugated polymers in pertinent devices.

A water‐soluble conjugated molecule for solar‐driven hydrogen evolution from seawater is developed. The formation of the supramolecular structure induced by the electrostatic interactions between chloride ions and the rationally designed positively charged small molecule facilitates the loading of Pt nanoparticles and promotes light‐induced charge carrier transport and separation.

Abstract

Photocatalytic hydrogen evolution is an attractive method for the acquisition of clean and sustainable energy with the use of solar power. Most reported studies have been carried out in scarce pure water. Therefore, the development of an artificial photosynthesis system that works perfectly with the earth's abundant seawater would be attractive. Herein, a supramolecular strategy for photocatalytic hydrogen production from the simulated seawater under sunlight irradiation (AM 1.5G, 100 mW cm⁻²) is presented using a water‐soluble, conjugated molecule as the photosensitizer and the photodeposited Pt nanoparticles as the catalyst. Inspired by the natural photosynthesis system, unprecedented advantage of the chloride ions in seawater is taken and the formation of supramolecular structure is promoted by electrostatic interactions between chloride ions and the fine‐designed PorFN, which further facilitates the loading of Pt nanoparticles and multielectron transfer. As a result, a hydrogen evolution rate of 10.8 mmol h⁻¹ g⁻¹ is achieved in the simulated seawater. Moreover, the photocatalytic activity shows relatively low dependence on the light intensity, which is of great importance for practical applications.

Ternary organic heterojunction based photodiodes are achieved with broadband photoresponse covering the whole visible and near‐infrared range. These photodiodes exhibit enhanced figure of merits, including relatively low dark current and noise, decent responsivity, large linear dynamic range, fast response, and superior stability, indicating remarkable potential for next generation photodetection and imaging.

Abstract

Organic semiconductors have attracted tremendous attention in the past few years, thanks to their excellent flexibility, solution‐processability, low‐cost, chemical versatility, etc. Particularly, organic solar cells based on ternary heterojunctions have shown remarkable device performance, with the recent development of nonfullerene acceptor materials. These novel materials are also promising for photodetection. However, there are several key limits facing organic photodetectors, such as relatively large bandgaps, poor charge transport, and stability. In this work, a novel nonfullerene acceptor—CO _i 8DFIC—is introduced, blended with a fullerene derivative and a donor to form ternary heterojunctions. After optimization, photodiodes based on such ternary blends exhibit compelling performance metrics, including low dark current, decent responsivity, large linear dynamic range, fast response, and excellent stability. This device performance is actually on a par with the established silicon technology, suggesting great potential for photodetection and imaging.

A high‐efficiency parallel‐like ternary organic photovoltaic device is developed through synergetic effects among a wide‐bandgap donor polymer, a narrow‐bandgap nonfullerene acceptor, and fullerene acceptors. Morphological optimization of the ternary devices via the incorporation of fullerenes yields simultaneous enhancement of the charge generation and extraction. An efficiency of 12.1% at an energy loss of 0.61 eV is realized.

Abstract

Ternary organic photovoltaic (OPV) devices with multiple light‐absorbing active materials have emerged as an efficient strategy for realizing further improvements in the power conversion efficiency (PCE) without building complex multijunction structures. However, the third component often acts as recombination centers and, hence, the optimization of ternary blend morphology poses a major challenge to improving the PCE of these devices. In this work, the performance of OPVs is enhanced through the morphological modification of nonfullerene acceptor (NFA)‐containing binary active layers. This modification is achieved by incorporating fullerenes into the layers. The uniformly dispersed fullerenes are sufficiently continuous and successfully mediate the ordering of NFA without charge or energy transfer. Owing to the simultaneous improvement in the charge generation and extraction, the PCE (12.1%) of these parallel‐linked ternary devices is considerably higher than those of the corresponding binary devices (9.95% and 7.78%). Moreover, the additional energy loss of the ternary device is minimized, compared with that of the NFA‐based binary device, due to the judicious control of the effective donor:acceptor composition of the ternary blends.

Poly[(5,6‐bis(2‐hexyldecyloxy)benzo[c][1,2,5]thiadiazole‐4,7‐diyl)‐alt‐(5,50‐(2,5‐difluoro‐1,4‐phenylene)bis(thiophen‐2‐yl))] (PDTBTBz‐2Fanti)‐based organic photovoltaics (OPVs) show an exceptionally high efficiency of 23.1% under a 1000‐lx light‐emitting diode lamp.

Abstract

The unique electro‐optical features of organic photovoltaics (OPVs) have led to their use in applications that focus on indoor energy harvesters. Various adoptable photoactive materials with distinct spectral absorption windows offer enormous potential for their use under various indoor light sources. An in‐depth study on the performance optimization of indoor OPVs is conducted using various photoactive materials with different spectral absorption ranges. Among the materials, the fluorinated phenylene‐alkoxybenzothiadiazole‐based wide bandgap polymer—poly[(5,6‐bis(2‐hexyldecyloxy)benzo[c][1,2,5]thiadiazole‐4,7‐diyl)‐alt‐(5,50‐(2,5‐difluoro‐1,4‐phenylene)bis(thiophen‐2‐yl))] (PDTBTBz‐2F_anti)‐contained photoactive layer—exhibits a superior spectrum matching with indoor lights, particularly a light‐emitting diode (LED), which results in an excellent power absorption ratio. These optical properties contribute to the state‐of‐the‐art performance of the PDTBTBz‐2F_anti:[6,6]‐phenyl‐C₇₁ butyric acid methyl ester (PC₇₁BM)‐based OPV with an unprecedented high power‐conversion efficiency (PCE) of 23.1% under a 1000 lx LED. Finally, its indoor photovoltaic performance is observed to be better than that of an interdigitated‐back‐contact‐based silicon photovoltaic (PCE of 16.3%).

Quaternary blend organic photovoltaics (Q‐OPVs) exhibit efficient operation under diverse irradiation conditions and improved thermal durability with suppressed morphological evolution during operation. The unique properties of the Q‐OPVs such as semitransparency, high film thickness tolerance, and color codability expand their applicability to emerging energy systems, which operate autonomously by any incident light all day, even when there is no sunlight.

Abstract

The unique properties of organic photovoltaics (OPVs) offer great promise in emerging applications such as wearable electronics or the Internet of Things. For their successful utilization, OPV operation should be designed for versatile irradiation circumstances in addition to solar light since they should be capable of providing electric power when there is no sunlight or when they operate indoors. Here, a quaternary OPV (Q‐OPV) as a semitransparent, colorful energy platform that operates efficiently under both solar and artificial light irradiation is demonstrated. The experimentally optimized Q‐OPV shows a broadened spectral response and improved charge transport process with suppressed recombination, thereby providing high output powers that are sufficient to autonomously operate low‐power electronic devices. In addition, the Q‐OPV benefits from improved morphological stability with a reduced driving force for grain growth by the increased entropy in the quaternary blend system. The important features of the Q‐OPV platform such as semitransparency, high tolerance to film thickness, and color codability, while pursuing the improved performance and thermal durability, further open new opportunities as an all‐day (24/7/365) power generator in broad practical applications.

A small molecule donor with appropriate energy levels and good compatibility is designed and synthesized as the third component for the construction of two types (fullerene/non‐fullerene) of all‐small‐molecule ternary solar cells with higher PCEs of over 10%. The results demo‐nstrate that introducing a homologous donor for the host donor is a promising way toward developing highly efficient all‐small‐molecule solar cells.

Abstract

Two types of all‐small‐molecule ternary solar cells consisting of two small‐molecule donors and one acceptor (fullerene/non‐fullerene) are developed. Interestingly, both these devices have a common component: a carefully designed medium bandgap small molecule, which possesses appropriate energy levels and displays good compatibility with the host donor. In the fullerene system, the charge‐relaying role of the additive donor is confirmed by the improved charge transportation and suppressed charge recombination. While in the non‐fullerene system, the mixed face‐on and edge‐on orientation of the ternary film induced by the additive donor dominates the promotion of charge transportation. Accordingly, both ternary devices deliver higher short‐circuit current density, fill factor, and power conversion efficiencies of over 10% compared to binary ones. This work offers a promising guideline on the construction of high‐performance all‐small‐molecule ternary solar cells by incorporating a miscible small‐molecule donor.

By using the new electron‐rich heptacyclic anthracene(cyclopentadithiophene) (AT) core, together with energy level modulations by end‐group optimizations enabling the match with polymer donors, two new nonfullerene small molecule acceptors AT‐NC and AT‐4Cl are synthesized. With both halogenated donor and acceptor, the organic photovoltaics device based on AT‐4Cl achieves a high power conversion efficiency of 13.27% with simultaneously improved J _sc and fill factor.

Abstract

Two new nonfullerene small molecule acceptors (NF‐SMAs) AT‐NC and AT‐4Cl based on heptacyclic anthracene(cyclopentadithiophene) (AT) core and different electron‐withdrawing end groups are designed and synthesized. Although the two new acceptor molecules use two different end groups, naphthyl‐fused indanone (NINCN) and chlorinated INCN (INCN‐2Cl) demonstrate similar light absorption. AT‐4Cl with chlorinated INCN as end groups are shifted significantly due to the strong electron‐withdrawing ability of chlorine atoms. Thus, desirable V _oc and photovoltaic performance are expected to be achieved when polymer PBDB‐T is used as the electron donor with AT‐NC as the acceptor, and fluorinated analog PBDB‐TF with down‐shifted energy levels is selected to blend with AT‐4Cl. Consequently, the device based on PBDB‐TF:AT‐4Cl yields a high power conversion efficiency of 13.27% with a slightly lower V _oc of 0.901 V, significantly enhanced J _sc of 19.52 mA cm⁻² and fill factor of 75.5% relative to the values based on PBDB‐T:AT‐NC. These results demonstrate that the use of a new electron‐rich AT core, together with energy levels modulations by end‐group optimizations enabling the match with polymer donors, is a successful strategy to construct high‐performance NF‐SMAs.

Retaining a stable and high built‐in potential across bulk heterojunction through interfacial modification and device engineering is a prerequisite for efficient and stable operation of nonfullerene organic solar cells.

Abstract

Remarkable progress has been made in the development of high‐efficiency solution‐processable nonfullerene organic solar cells (OSCs). However, the effect of the vertical stratification of bulk heterojunction (BHJ) on the efficiency and stability of nonfullerene OSCs is not fully understood yet. In this work, we report our effort to understand the stability of nonfullerene OSCs, made with the binary blend poly[(2,6‐(4, 8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene))‐alt‐(5,5‐(1′,3′‐di‐2‐thienyl‐5′,7′‐bis(2‐ethylhexyl)benzo[1′,2′‐c:4′,5′‐c′] dithiophene‐4,8‐dione)] (PBDB‐T):3,9‐ bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)‐indanone))‐5,5,11,11‐tetrakis(4‐hexylphenyl)‐ dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′] dithiophene (ITIC) system. It shows that a continuous vertical phase separation process occurs, forming a PBDB‐T‐rich top surface and an ITIC‐rich bottom surface in PBDB‐T:ITIC BHJ during the aging period. A gradual decrease in the built‐in potential (V ₀) in the regular configuration PBDB‐T:ITIC OSCs, due to the interfacial reaction between the poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) hole transporting layer and ITIC acceptor, is one of the reasons responsible for the performance deterioration. The reduction in V ₀, caused by an inevitable reaction at the ITIC/PEDOT:PSS interface in the OSCs, can be suppressed by introducing a MoO₃ interfacial passivation layer. Retaining a stable and high V ₀ across the BHJ through interfacial modification and device engineering, e.g., as seen in the inverted PBDB‐T:ITIC OSCs, is a prerequisite for efficient and stable operation of nonfullerene OSCs.

Schematic of the influence of light and thermal fluctuations on the PCBM:dimer population dynamics of a polymer:fullerene active layer. It is shown that a minimal rate model, parameterized by data from a facile UV–vis assay, can be employed to forecast the evolution and asymptotic behavior of this population, impacting the morphological and performance stability of solar cells.

Abstract

Photoinduced dimerization of phenyl‐C61‐butyric acid methyl ester (PCBM) has a significant impact on the stability of polymer:PCBM organic solar cells (OSCs). This reaction is reversible, as dimers can be thermally decomposed at sufficiently elevated temperatures and both photodimerization and decomposition are temperature dependent. In operando conditions of OSCs evidently involve exposure to both light and heat, following periodic diurnal and seasonal profiles. In this work, the kinetics of dimer formation and decomposition are examined and quantified as a function of temperature, light intensity, blend composition, and time. The activation energy for photodimerization is estimated to be 0.021(3) eV, considerably smaller than that for decomposition (0.96 eV). The findings are benchmarked with a variety of conjugated polymer matrices to propose a descriptive dynamic model of PCBM:dimer population in OSCs, and a framework is proposed to rationalize its interplay with morphology evolution and charge quenching. The model and parameters enable the prediction of the dynamic and long‐term PCBM:dimer populations, under variable temperature and light conditions, which impact the morphological stability of OSCs.

In this work, organic ternary solar cells based on a model system comprising the polymers PDCBT and PTB7‐Th and PC₇₀BM are presented as electron accepting units. The photophysics of this blend is governed by a fast energy transfer process from PDCBT to PTB7‐Th allowed by a favorable molecular affinity between PDCBT and PTB7‐Th.

Abstract

Ternary blends with broad spectral absorption have the potential to increase charge generation in organic solar cells but feature additional complexity due to limited intermixing and electronic mismatch. Here, a model system comprising the polymers poly[5,5‐bis(2‐butyloctyl)‐(2,2‐bithiophene)‐4,4‐dicarboxylate‐alt‐5,5‐2,2‐bithiophene] (PDCBT) and PTB7‐Th and PC₇₀BM as an electron accepting unit is presented. The power conversion efficiency (PCE) of the ternary system clearly surpasses the performance of either of the binary systems. The photophysics is governed by a fast energy transfer process from PDCBT to PTB7‐Th, followed by electron transfer at the PTB7‐Th:fullerene interface. The morphological motif in the ternary blend is characterized by polymer fibers. Based on a combination of photophysical analysis, GIWAXS measurements and calculation of the intermolecular parameter, the latter indicating a very favorable molecular affinity between PDCBT and PTB7‐Th, it is proposed that an efficient charge generation mechanism is possible because PTB7‐Th predominantly orients around PDCBT filaments, allowing energy to be effectively relayed from PDCBT to PTB7‐Th. Fullerene can be replaced by a nonfullerene acceptor without sacrifices in charge generation, achieving a PCE above 11%. These results support the idea that thermodynamic mixing and energetics of the polymer–polymer interface are critical design parameter for realizing highly efficient ternary solar cells with variable electron acceptors.

A 1D ultrabroadband (>450 nm) optical cavity is designed following an inverse electromagnetic computational approach to optimally trap light in a thin film absorber layer. When this novel cavity concept is applied to a low bandgap organic solar cell, a broadband absorption enhancement is demonstrated beyond the conventional limit resulting from light trapping in an ergodic optical geometry.

Abstract

In the subwavelength regime, several nanophotonic configurations have been proposed to overcome the conventional light trapping or light absorption enhancement limit in solar cells also known as the Yablonovitch limit. It has been recently suggested that establishing such limit should rely on computational inverse electromagnetic design instead of the traditional approach combining intuition and a priori known physical effect. In the present work, by applying an inverse full wave vector electromagnetic computational approach, a 1D nanostructured optical cavity with a new resonance configuration is designed that provides an ultrabroadband (≈450 nm) light absorption enhancement when applied to a 107 nm thick active layer organic solar cell based on a low‐bandgap (1.32 eV) nonfullerene acceptor. It is demonstrated computationally and experimentally that the absorption enhancement provided by such a cavity surpasses the conventional limit resulting from an ergodic optical geometry by a 7% average over a 450 nm band and by more than 20% in the NIR. In such a cavity configuration the solar cells exhibit a maximum power conversion efficiency above 14%, corresponding to the highest ever measured for devices based on the specific nonfullerene acceptor used.

The high‐performance PTB7‐Th:IEICO‐4F system exhibits an inherent performance degradation resulting from demixing and crystallization failure. Incorporation of a third component which has a miscibility in the donor polymer at or above the percolation threshold, yet is also partly miscible with the crystallizable acceptor can remedy the performance degradation.

Abstract

Long device lifetime is still a missing key requirement in the commercialization of nonfullerene acceptor (NFA) organic solar cell technology. Understanding thermodynamic factors driving morphology degradation or stabilization is correspondingly lacking. In this report, thermodynamics is combined with morphology to elucidate the instability of highly efficient PTB7‐Th:IEICO‐4F binary solar cells and to rationally use PC₇₁BM in ternary solar cells to reduce the loss in the power conversion efficiency from ≈35% to <10% after storage for 90 days and at the same time improve performance. The hypomiscibility observed for IEICO‐4F in PTB7‐Th (below the percolation threshold) leads to overpurification of the mixed domains. By contrast, the hypermiscibility of PC₇₁BM in PTB7‐Th of 48 vol% is well above the percolation threshold. At the same time, PC₇₁BM is partly miscible in IEICO‐4F suppressing crystallization of IEICO‐4F. This work systematically illustrates the origin of the intrinsic degradation of PTB7‐Th:IEICO‐4F binary solar cells, demonstrates the structure–function relations among thermodynamics, morphology, and photovoltaic performance, and finally carries out a rational strategy to suppress the degradation: the third component needs to have a miscibility in the donor polymer at or above the percolation threshold, yet also needs to be partly miscible with the crystallizable acceptor.

Development of single‐component organic solar cells employing a conjugated double‐cable polymer is an elegant strategy to overcome the microstructure instability of typical bulk‐heterojunction organic solar cells. This communication demonstrates that single‐component solar cells can exhibit excellent thermal‐ and photostability under harsh conditions, such as 90 °C & 1 sun illumination, and retain 100% performance at 160 °C for over 400 h.

Abstract

Solution‐processed organic solar cells (OSCs) are promising low‐cost, flexible, portable renewable sources for future energy supply. The state‐of‐the‐art OSCs are typically fabricated from a bulk‐heterojunction (BHJ) active layer containing well‐mixed donor and acceptor molecules in the nanometer regime. However, BHJ solar cells suffer from stability problems caused by the severe morphological changes upon thermal or illumination stress. In comparison, single‐component organic solar cells (SCOSCs) based on a double‐cable conjugated polymer with a covalently stabilized microstructure is suggested to be a key strategy for superior long‐term stability. Here, the thermal‐ and photostability of SCOSCs based on a model double‐cable polymer is systematically investigated. It is encouraging to find that under 90 °C & 1 sun illumination, the performance of SCOSCs remains substantially stable. Transport measurements show that charge generation and recombination (lifetime and recombination order) hardly change during the aging process. Particularly, the SCOSCs exhibit ultrahigh long‐term thermal stability with 100% PCE remaining after heating at temperature up to 160 °C for over 400 h, indicating an excellent candidate for extremely rugged applications.

In organic solar cells, energetic disorder has a major impact on the charge‐recombination rates and thus on open‐circuit voltage losses. In poly‐3‐hexyl‐thiophene (P3HT):[6,6]‐phenyl‐C61‐butyric‐acid methyl ester amorphous heterojunctions, the torsional flexibility of the P3HT backbones is seen as the main origin of the large dynamic and static disorders impacting both charge‐transfer and transport states.

Abstract

Molecular dynamics simulations are combined with density functional theory calculations to evaluate the impact of static and dynamic disorders on the energy distribution of charge‐transfer (CT) states at donor–acceptor heterojunctions, such as those found in the active layers of organic solar cells. It is shown that each of these two disorder components can be partitioned into contributions related to the energetic disorder of the transport states and to the disorder associated with the hole–electron electrostatic interaction energies. The methodology is applied to evaluate the energy distributions of the CT states in representative bulk heterojunctions based on poly‐3‐hexyl‐thiophene and phenyl‐C₆₁‐butyric‐acid methyl ester. The results indicate that the torsional fluctuations of the polymer backbones are the main source of both static and dynamic disorders for the CT states as well as for the transport levels. The impact of static and dynamic disorders on radiative and nonradiative geminate recombination processes is also discussed.

A series of room‐temperature and ecofriendly solvent processable polymers are designed and synthesized by backbone modification of the high temperature processable PNTz4T polymer. The resulting random terpolymer (PNTz4T‐5MTC)‐based solar cells show 9.66% power conversion efficiency (PCE) on a small area (0.12 cm²) and an outstanding 6.61% PCE on large‐area module (54.45 cm²) at room temperature processing conditions in air.

Abstract

The room temperature (RT) processability of the photoactive layers in polymer solar cells (PSCs) from halogen‐free solvent along with their highly reproducible power conversion efficiencies (PCEs) and intrinsic thickness tolerance are extremely desirable for the large‐area roll‐to‐roll (R2R) production. However, most of the photoactive materials in PSCs require elevated processing temperatures due to their strong aggregation, which are unfavorable for the industrial R2R manufacturing of PSCs. These limiting factors for the commercialization of PSCs are alleviated by synthesizing random terpolymers with components of (2‐decyltetradecyl)thiophen‐2‐yl)naphtho[1,2‐c:5,6‐c′]bis[1,2,5]thiadiazole and bithiophene substituted with methyl thiophene‐3‐carboxylate (MTC). In contrast to the temperature‐dependent PNTz4T polymer, the resulting random terpolymers (PNTz4T‐MTC) show better solubility, slightly reduced crystallinity and aggregation, and weaker intermolecular interaction, thus enabling PNTz4T‐MTC to be processed at RT from a halogen‐free solvent. Particularly, the PNTz4T‐5MTC‐based photoactive layer exhibits an excellent PCE of 9.66%, which is among the highest reported PCEs for RT and ecofriendly halogen‐free solvent processed fullerene‐based PSCs, and a thickness tolerance with a PCE exceeding 8% from 100 to 520 nm. Finally, large‐area modules fabricated with the PNTz4T and PNTz4T‐5MTC polymer have shown 4.29% and 6.61% PCE respectively, with an area as high as 54.45 cm² in air.

Operation stability of ultraflexible organic solar cells (OSCs) is demonstrated by a 1.3 µm‐thick transparent polyimide substrate, which can block ultraviolet (UV) rays. In UV irradiation and maximum‐power‐point tracking tests, the stability of the device performance is improved dramatically by installing ultrathin transparent polyimide in OSCs. With the aforementioned feature, the OSCs can function stably and correctly under sunlight.

Abstract

Ultralightweight and flexible power sources are essential for driving textile or wearable electronic devices and soft robots because they do not induce discomfort or limit movement when they are attached to human skin, textiles, or soft actuators. Organic solar cells (OSCs) are good candidates for developing such power sources because they have the advantages of being lightweight and flexible. However, achieving operational stability and ultrathin shape simultaneously remains difficult because the ultrathin substrate cannot prevent the penetration of ultraviolet (UV) light, which is major a cause for the degradation of OSCs. Here, ultrathin OSCs that show great operational stability and high performance are reported. The 1.3 µm thick transparent polyimide utilized as a substrate can block light of 350 nm wavelength in the UV range by 90%. The ultrathin OSCs with the transparent polyimide substrate produce a power conversion efficiency (PCE) of 9.0% and realize both photostability and operational stability. The PCE was maintained at 90% after 3 h in a maximum power point tracking test, indicating much better operational stability than the reference rigid OSCs.

Two solid additives are proven to improve the molecular packing of acceptors, while devices processed with different additives exhibit different photovoltaic performances due to the different volatilities. The working mechanism and basic design rules of solid additives are revealed, and a feasible method for achieving high‐efficiency polymer solar cells is established.

Abstract

Fine‐tuning of the nanoscale morphologies of the active layers in polymer solar cells (PSCs) through various techniques plays a vital role in improving the photovoltaic performance. However, for emerging nonfullerene (NF) PSCs, the morphology optimization of the active‐layer films empirically follows the methods originally developed in fullerene‐based blends and lacks systematic studies. In this work, two solid additives with different volatilities, SA‐4 and SA‐7, are applied to investigate their influence on the morphologies and photovoltaic performances of NF‐PSCs. Although both solid additives effectively promote the molecular packing of the NF acceptors, due to the higher volatility of SA‐4, the devices processed with SA‐4 exhibit a power conversion efficiency of 13.5%, higher than that of the control devices, and the devices processed with SA‐7 exhibit poor performances. Through a series of detailed morphological analyses, it is found that the volatilization of SA‐4 after thermal annealing is beneficial for the self‐assembly packing of acceptors, while the residuals due to the incomplete volatilization of SA‐7 have a negative effect on the film morphology. The results delineate the feasibility of applying volatilizable solid additives and provide deeper insights into the working mechanism, establishing guidelines for further material design of solid additives.

Organic solar cells achieve over 15% efficiency through the use of a copolymer donor, and simultaneously enhanced open‐circuit voltage and short‐circuit current density are obtained. High‐performance solar cells are adaptable for environment‐friendly solvents using a blade‐coating method, while showing better photostability than the corresponding ternary solar cells.

Abstract

Ternary blending and copolymerization strategies have proven advantageous in boosting the photovoltaic performance of organic solar cells. Here, 15% efficiency solar cells using copolymerization donors are demonstrated, where the electron‐withdrawing unit, ester‐substituted thiophene, is incorporated into a PBDB‐TF polymer to downshift the molecular energy and broaden the absorption. Copolymer‐based solar cells suitable for large‐area devices can be fabricated by a blade‐coating method from a nonhalogen and nonaromatic solvent mixture. Although ternary solar cells can achieve comparable efficiencies, they are not suitable for environment‐friendly processing conditions and show relatively low photostability compared to copolymer‐based devices. These results not only demonstrate high‐efficiency organic photovoltaic cells via copolymerization strategies but also provide important insights into their applications in practical production.

To harvest a large photocurrent in bulk‐heterojunction organic photovoltaic cells (OPVs), materials with long‐lifetime triplet excitons are expected to be potential candidates for providing sufficient time for diffusion of excitons to donor/acceptor interfaces. Recent progress of various triplet‐material‐based OPVs (T‐OPVs) is briefly summarized, and performance limitations and strategies to further enhance the performance of T‐OPVs are discussed.

Abstract

Organic photovoltaic cells (OPVs) have attracted broad attention and become a very energetic field after the emergence of nonfullerene acceptors. Long‐lifetime triplet excitons are expected to be good candidates for efficiently harvesting a photocurrent. Parallel with the development of OPVs based on singlet materials (S‐OPVs), the potential of triplet materials as photoactive layers has been explored. However, so far, OPVs employing triplet materials in a bulk heterojunction have not exhibited better performance than S‐OPVs. Here, the recent progress of representative OPVs based on triplet materials (T‐OPVs) is briefly summarized. Based on that, the performance limitations of T‐OPVs are analyzed. The shortage of desired triplet materials with favorable optoelectronic properties for OPVs, the tradeoff between long lifetime and high binding energy of triplet excitons, as well as the low charge mobility in most triplet materials are crucial issues restraining the efficiencies of T‐OPVs. To overcome these limitations, first, novel materials with desired optoelectronic properties are urgently demanded; second, systematic investigation on the contribution and dynamics of triplet excitons in T‐OPVs is necessary; third, close multidisciplinary collaboration is required, as proved by the development of S‐OPVs.

Ring fusion and backbone fluorination yield a novel ladder‐type building block f‐FBTI2, a desirable “stronger acceptor” for enabling n‐type electron‐acceptor polymers. The resulting polymer semiconductor f‐FBTI2‐T shows an excellent power conversion efficiency of 8.1% with a very small energy loss of 0.53 eV in all‐polymer solar cell devices.

Abstract

A novel imide‐functionalized arene, di(fluorothienyl)thienothiophene diimide (f‐FBTI2), featuring a fused backbone functionalized with electron‐withdrawing F atoms, is designed, and the synthetic challenges associated with highly electron‐deficient fluorinated imide are overcome. The incorporation of f‐FBTI2 into polymer affords a high‐performance n‐type semiconductor f‐FBTI2‐T, which shows a reduced bandgap and lower‐lying lowest unoccupied molecular orbital (LUMO) energy level than the polymer analog without F or with F‐functionalization on the donor moiety. These optoelectronic properties reflect the distinctive advantages of fluorination of electron‐deficient acceptors, yielding “stronger acceptors,” which are desirable for n‐type polymers. When used as a polymer acceptor in all‐polymer solar cells, an excellent power conversion efficiency of 8.1% is achieved without any solvent additive or thermal treatment, which is the highest value reported for all‐polymer solar cells except well‐studied naphthalene diimide and perylene diimide‐based n‐type polymers. In addition, the solar cells show an energy loss of 0.53 eV, the smallest value reported to date for all‐polymer solar cells with efficiency > 8%. These results demonstrate that fluorination of imide‐functionalized arenes offers an effective approach for developing new electron‐deficient building blocks with improved optoelectronic properties, and the emergence of f‐FBTI2 will change the scenario in terms of developing n‐type polymers for high‐performance all‐polymer solar cells.