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Although the layer‐by‐layer (LBL) processing can usually achieve an optimal bulk‐heterojunction morphology for high‐performance Organic photovoltaics (OPVs), the unambiguous working principles governing the morphology evolution are still lacking. To address this issue, here the phase‐separation kinetics of LBL processing are comprehensively studied using in situ spectroscopies, which are very sensitive to the intermolecular interactions, e.g. the molecular packing and D:A phase‐separation. Upon casting the nonfullerene acceptor (i.e., the BTP‐eC9) solution on top of the polymer donor, i.e., PM6, it is found that 1) the solvent will first swell the polymer and induce a polymer gel, 2) following the polymer gelation, the NFAs will immediately permeate into the cavities of polymer gel and form a molecular‐level D:A mixing, and 3) with the evaporation of the solvent, phase‐separation between the donor and acceptor occurs and results in a bulk‐heterojunction morphology as those achieved with blend‐cast processing. With these understandings, more diverse processing conditions have been purposely utilized to dictate the phase evolution process precisely. As a result, a high efficiency of 19.7% is reached, representing one of the best among binary OPVs. Therefore, this work deciphers phase‐separation kinetics of LBL processing and should pave the way toward advanced morphology control for high‐performance OPVs. [ABSTRACT FROM AUTHOR]

In this study, six different donor‐π‐acceptor1‐π‐donor‐acceptor2 type random co‐polymers containing benzodithiophene as a donor, benzooxadiazole (BO), and thieno[3,4‐c]pyrrole‐4,6‐dione (TPD) as acceptor, have been synthesized and characterized. In addition to the acceptor core ratio at different values, the effect of aromatic bridge structures on the optical, electronic, and photovoltaic properties of six different random co‐polymers is investigated by using thiophene and selenophene structures as aromatic bridge units. To investigate how the acceptor unit ratio and replacement of aromatic bridge units impact the structural, electronic, and optical properties of the polymers, density functional theory (DFT) calculations are carried out for the tetramer models. The open‐circuit voltage (VOC), which is strongly correlated with the HOMO levels of the donor material, is enhanced with the increasing ratio of the TPD moiety. On the other hand, the short‐circuit current (JSC), which is associated with the absorption ability of the donor material, is improved by the increasing ratio of BO moiety with the π‐bridges. BO moiety dominant selenophene π‐bridged co‐polymer (P4) showed the best performance with a power conversion efficiency (PCE) of 6.26%, a JSC of 11.44 mA cm2, a VOC of 0.80 V, and a fill factor (FF) of 68.81%. [ABSTRACT FROM AUTHOR]

Top electrodes of organic photovoltaics (OPVs) are usually thermally evaporated in the vacuum, which is non‐continuous and time‐consuming and has been the bottleneck for the OPV fabrication process. Printable top electrodes that are free of vacuum, high temperature, and solvents will make OPVs more attractive. Low‐melting‐point alloys (LMPAs) are promising candidates for printable OPV electrodes thanks to the merits of matching work functions, high electron conductivity, high environment stability, and no need for post‐treatment. Here, LMPA electrodes are directly deposited on OPVs by simply falling a single LMPA droplet onto the substrate. The LMPA droplet spreads to form a thin film with a smooth interface intimately contacting the substrate. The electrode area can be tailored by adjusting the droplet diameter or the Weber number, which is the ratio of inertia to surface tension. The interface morphology is mainly affected by the contact temperature. The degree of oxidation and charges on the droplet can also influence the electrode area and interface morphology. OPVs with droplet‐impacted LMPA electrodes exhibit power conversion efficiencies of up to 16.17%. This work demonstrates the potential of single‐droplet impact deposition as a simple method for printing OPV electrodes for scalable manufacturing. [ABSTRACT FROM AUTHOR]

Organic solar cells (OSCs) have made remarkable progress due to developing novel materials and device architectures. Herein, we designed six new non-fullerene acceptors (QM1–QM6) having a quinoxalineimide (QI) as the central-building-block. We aimed to explore the potential of QI-containing structures for developing high-performance acceptors for OSCs. These designed molecules possess a fusion of the QI unit with a thienylthiophene backbone and are equipped with various efficient end-capping groups. Extensive theoretical calculations were carried out to evaluate the structural and charge distribution characteristics, including the optical, optoelectronics, density of states, transition density matrix, molecular electrostatic potential (ESP), reorganization energies, and photovoltaic properties. The results revealed that the designed series exhibited improved electron–hole pair coherences, efficient charge transportation, and favorable ESP patterns, suggesting their suitability for enhanced optical and electronic characteristics. Furthermore, the hole and electron overlap analyses demonstrated significant overlap in QM1–QM6, indicating efficient charge transfer and higher charge mobilities. Additionally, the analysis of reorganization energies showed low reorganization energy values, indicating favorable charge mobility rates and potential for high-efficiency solar cell devices. This research establishes a strong foundation for utilizing QI-containing fused units as central building blocks for designing high-performance acceptors, opening up new avenues for advancements in OSCs technology. We designed a series of new non-fullerene acceptors and explored their potential for organic photovoltaics. Various efficient theoretical calculations were carried out to evaluate the structural and charge distribution characteristics, including the optical, optoelectronics, density of states, and photovoltaic properties. This research establishes a strong foundation for designing high-performance acceptors, opening up new avenues for advancements in OSC technology. [ABSTRACT FROM AUTHOR]

Nine molecules based on benzo[1,2‐b:4,5‐b′]dithiophene (BDT) and 2D‐BDT derivatives are studied as donor materials in organic photovoltaic (OPV) devices fabricated by thermal evaporation, aiming to understand how different alkyl lateral substituents affect the molecular packing, the charge transport, and, subsequently, the device performance. Synthesis of the molecules is followed by a comprehensive characterization using thermal and differential scanning calorimetry analyses, which confirm their thermal stability and suitability for vacuum‐processed OPV devices. Thermal analysis also demonstrates a strong correlation between the melting point reduction of the molecules and the disorder caused by the alkyl chains. As the synthesized molecules present similar optical properties, the differences in the device performance are caused by the different substituents. BDT derivatives with low melting point temperatures produce reduced current density, hole mobility, and overall device performance, which are attributed to poor molecular packing. Additionally, energy‐dispersive X‐ray spectroscopy analysis suggests phase separation with fullerene, further impacting the efficiency of the devices. The findings indicate that the photovoltaic performance of BDT‐based molecules can be modulated by avoiding aliphatic substituents, providing a strategy for the design of more efficient materials, with thermal evaporation as an ideal method to evaluate and decouple molecular packing from solubility. [ABSTRACT FROM AUTHOR]

The significant progress of p‐type and n‐type active layer materials in the past several years has pushed the power conversion efficiency (PCE) of organic solar cells (OSCs) toward 19%. Due to the relatively low synthesis cost and simple synthesis method of carboxylate‐containing building blocks, including thiophene, thieno[3,2‐b]thiophene, thieno[3,4‐b]thiophene, furan, pyrazine, benzodithiophene, benzothiazole, quinoxaline, etc., are widely used to construct p‐type photovoltaic polymers. These resulting carboxylate‐bearing polymers present downward energy levels, high absorption coefficient, narrow bandgap, high hole mobility, and strong aggregation behavior, which have dabbled in the fabrication of mechanically stretchable, semitransparent, indoor, and tandem OSCs, etc., and produce excellent photovoltaic performance. The low‐cost carboxylate‐containing copolymers exhibit a satisfying PCE approaching 17%, and the random terpolymer systems achieve a high PCE over 19%. This review focuses on the progress of carboxylate‐containing photovoltaic polymers, summarizes the molecular characteristics, discusses their structure‐performance relationship, and offers a summary and outlook on the challenges for future molecular development. [ABSTRACT FROM AUTHOR]

The development of high‐performance organic photovoltaics (OPVs) with thick film active layers is key to moving this technology from laboratory preparation to industrial production. Design and synthesis of active layer materials to achieve a bi‐continuous interpenetrating morphology with appropriate nanoscale phase separation has been demonstrated as an effective method to realize high‐efficiency thick film devices. Here, two non‐fullerene acceptors are developed to compare the effect of symmetric (diDT‐BO) and asymmetric (DTC11‐BO) substituted alkyl chains on active layer morphology and device performance by introducing asymmetric side chains to the central core pyrrole ring. Based on the solubility and crystallinity differences of DTC11‐BO and diDT‐BO, the power conversion efficiencies (PCEs) of 19.0% and 18.1% are realized with D18 as the donor. Importantly, D18:DTC11‐BO devices with 300 and 500 nm active layers achieve excellent PCEs of 17.7% and 16.1%, which are among the top‐class values for thick film OPVs reported to date. The work demonstrates that tunning the crystallinity by optimizing the asymmetric alkyl chains is an effective material design strategy to achieve high‐efficiency thick film OPVs. [ABSTRACT FROM AUTHOR]

Stretchable organic photovoltaics (OPVs) are pivotal for advancing conformable electronics, yet achieving both efficient and intrinsically stretchable OPVs remains a significant challenge. The main issue is maintaining electronic and mechanical properties under deformation. Here, a ternary blend system, PTzBI‐oF:PYIT:EVA is presented, incorporating ethylene‐vinyl acetate (EVA) to establish a conjugated and elastomeric dual‐network morphology. The elastomer network dissipates applied stress, preserving the crystalline packing of the conjugated network and enabling improved mechanical stability of charge carrier generation and transport. Specifically, with 15% EVA content, the ternary blend achieved a power conversion efficiency (PCE) of 15.28% in rigid devices and exhibited a crack onset strain of 17.23%. Notably, the stretchable OPVs retained over 80% of their initial PCE under 30% strain. These findings underscore the potential of conjugated and elastomeric dual‐network morphology in developing high‐performance stretchable electronics for various applications. [ABSTRACT FROM AUTHOR]

The energetic driving force for electron transfer must be minimized to realize efficient optoelectronic devices including organic light‐emitting diodes (OLEDs) and organic photovoltaics (OPVs). Exploring the dynamics of a charge‐transfer (CT) state at an interface leads to a comprehension of the relationship between energetics, electron‐transfer efficiency, and device performance. Here, we investigate the electron transfer from the CT state to the triplet excited state (T1) in upconversion OLEDs with 45 material combinations. By analyzing the CT emission and the singlet excited‐state emission from triplet–triplet annihilation via the dark T1, their energetics and electron‐transfer efficiencies are extracted. We demonstrate that the CT→T1 electron transfer is enhanced by the stronger CT interaction and a minimal energetic driving force (<0.1 eV), which is explained using the Marcus theory with a small reorganization energy of <0.1 eV. Through our analysis, a novel donor–acceptor combination for the OLED is developed and shows an efficient blue emission with an extremely low turn‐on voltage of 1.57 V. This work provides a solution to control interfacial CT states for efficient optoelectronic devices without energy loss. [ABSTRACT FROM AUTHOR]

The global interest in environmental issues and sustainable energy has propelled extensive research in photovoltaic (PV) technologies. Brazil has emerged as one of the top ten solar energy producers and flexible PV suppliers in the world. In this context, organic photovoltaic cells (OPVs) have garnered attention due to their flexibility and ability to integrate into various surfaces, albeit facing challenges regarding lifespan and efficiency compared to silicon cells. This review examines the current state of research on OPVs and thin-film solar technologies, employing the systematic literature review methodology Proknow-C. The review includes an analysis of raw materials such as conductive polymers, fabrication processes including film deposition and encapsulation, and technological advancements that enhance the efficiency and stability of OPVs. Utilizing the Proknow-C methodology, a bibliographic portfolio was constructed to identify the current state of research in this field. Of 268 papers from major scientific databases, only 30 were deemed relevant to the theme, highlighting a significant research gap. This paper is a valuable resource for researchers, providing an updated overview and a foundation for future investigations in organic photovoltaics. The results emphasize the importance of materials such as conductive polymers and donor–acceptor molecules and the role of nanotechnology in advancing OPVs. Innovations in manufacturing techniques, such as inkjet and blade coating-based printing techniques, are shown to increase efficiency by providing precise control over film thickness and uniformity and reducing costs through lower material waste. Overall, this review highlights the necessity of further exploration and collaboration within the scientific community to address the challenges and propel advancements in organic photovoltaic cells. These advancements are crucial for transitioning to cleaner energy sources, reinforcing the ongoing significance of thin-film technologies in energy innovation. [ABSTRACT FROM AUTHOR]

The electron transport layer (ETL) has gained significant attention recently for its essential role in facilitating charge extraction, transportation, and reducing recombination in photovoltaic cells. Organic photovoltaics (OPVs) with ETLs have achieved remarkable efficiencies exceeding 19%, and indoor OPVs have reached a peak efficiency of 29.4% under 3000 LX illumination. Despite these accomplishments, the difficulties in choosing appropriate ETLs for contact alignment have constrained device performance. This review comprehensively overviews the latest advancements in ETL materials used in conventional and inverted OPVs. Additionally, it investigates the evolution of dopant materials, emphasizing the need for improved electron mobility, energy level alignment, and surface passivation treatment of the buffer layer and absorber layers in OPVs. Continual studies of transport materials and the potential utilization of doping or multilayer ETLs are suggested as inevitable research toward achieving higher power conversion efficiency and stability in OPV technology. Additionally, identifying optimal ETL materials capable of synergistic interactions remains crucial for sustained progress in renewable energy technology. [ABSTRACT FROM AUTHOR]

This paper investigates TiN for its potential to enhance light-harvesting efficiency as an alternative material to Au for nanoscale plasmonic light trapping in thin-film solar cells. Using nanosphere lithography (NSL), plasmonic arrays of both Au and TiN are fabricated and characterized. Later, the fabricated TiN and Au arrays are integrated into a thin-film organic photovoltaic (OPV) device with a PBDB-T:ITIC-M bulk heterojunction (BHJ) active layer. A comparative study between these Au and TiN nanostructured arrays evaluates their fabrication process and plasmonic response, highlighting the advantages and disadvantages of TiN compared to a conventional plasmonic material such as Au. The effect of the fabricated arrays when integrated into an OPV is presented and compared to understand the viability of TiN. As one of the first experimental studies utilizing TiN arrays for the plasmonic enhancement of photovoltaics, the results offer valuable insight that can guide future applications and decisions in design. [ABSTRACT FROM AUTHOR]

A self-doped conducting polyaniline was used as a hole transport layer (HTL) in organic photovoltaics (OPVs) [indium tin oxide/HTL/zinc-phthalocyanine/C70/bathocuproine/Al]. This polyaniline was characterized by phosphonic acid neutralized with pyridine (PMAP:Py). The current–voltage characteristics were evaluated and were comparable to those of the devices using a conventional hole transport material, poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate) (PEDOT:PSS). PMAP:Py-based OPVs stored in both nitrogen and ambient atmosphere had a longer lifetime than PEDOT:PSS-based ones. [ABSTRACT FROM AUTHOR]

In the advancement of organic photovoltaics (OPV) toward scale‐up production, how to mitigate the batch instability of electron‐donating polymers originated from varied molecular weights remains a great challenge. By taking into consideration the relationship between the molecular weight of electron‐donating polymers and the relevant critical concentration (c*) of the solution, herein it is demonstrated that the aggregation behavior of the electron‐donating polymers can be tailored through manipulating c* of the polymer solution. It is interesting to note that the excessive aggregation in low‐molecular‐weight fractions can be circumvented while the favorable mixing ratio can be identified. By preparing the binary bulk heterojunction film under c*‐defined conditions for mixed‐molecular‐weight polymers, a notable power conversion efficiency of 19.1% for binary devices is achieved. Of particular importance is that a linear interrelation can be established between the c* for the maximum PCE and c* for the low‐molecular‐weight fraction aggregation, validating those straightforward spectra measurements can accurately and rationally guide the molecular weight mixing of photovoltaic donor polymers, thereby fully harnessing the potent driving force and affinity inherent to the low‐molecular‐weight fractions. These findings offer a straightforward and logical framework for addressing batch variability in the large‐scale production of high‐performance OPV devices. [ABSTRACT FROM AUTHOR]

In this work, layer-by-layer organic photovoltaics (LbL OPVs) were prepared by sequentially spin-coating PM1 and L8-BO solutions. The solvent additive 1,8-diiodooctane (DIO), which has a high boiling point, and solid additive l,3,5-trichlorobenzene (TCB), which has a high volatile, were deliberately selected to incorporate with the L8-BO solutions. The power conversion efficiency (PCE) of LbL OPVs was considerably enhanced from 17.43% to 18.50% by employing TCB as the additive, profiting by the concurrently increased short-circuit current density (JSC) of 26.74 mA cm−2 and a fill factor (FF) of 76.88%. The increased JSCs of LbL OPVs with TCB as additive were ascribed to the tilted-up absorption edge in the long wavelength range and the external quantum-efficiency spectral difference between LbL OPVs with and without TCB as an additive. The molecular arrangement of L8-BO and the PM1 domain was enhanced with TCB as an additive, which was most likely responsible for the increased charge mobilities in the layered films processed with additives. It was indicated that the dynamic film-forming process of the acceptor layers plays a vital role in achieving efficient LbL OPVs by employing additive strategy. Over 6% PCE improvement of the LbL OPVs with PM1/L8-BO as the active layers can be achieved by employing TCB as additive. [ABSTRACT FROM AUTHOR]

Organic dyes that absorb light in the visible to near‐infrared region have garnered significant interest, owing to their extensive utility in organic photovoltaics and various biomedical applications. Aza‐boron‐dipyrromethene (Aza‐BODIPY) dyes are a class of chromophores with impressive photophysical properties such as tunable absorption from the visible region towards near infrared (NIR) region, high molar absorptivity, and fluorescence quantum yield. In this review, we discuss the developments in the aza‐BODIPYs, related to their synthetic routes, photophysical properties and their applications. Their design strategies, modifications in chemical structures, mode/position of attachment, and their impact on photo‐physical properties are reviewed. The potential applications of aza‐BODIPY derivatives such as organic solar cells, photodynamic therapy, boron‐neutron capture therapy, fluorescence sensors, photo‐redox catalysis, photoacoustic probes and optoelectronic devices are explained. [ABSTRACT FROM AUTHOR]

Organic photovoltaics (OPVs) represent one of the most promising photovoltaic technologies owing to their high capacity to convert solar energy to electricity. With the continuous structure upgradation of photovoltaic materials, especially that of non‐fullerene acceptors (NFAs), the OPV field has witnessed rapid progress with power conversion efficiency (PCE) exceeding 19%. However, it remains challenging to overcome the intrinsic trade‐off between the photocurrent and photovoltage, restricting the further promotion of the OPV efficiency. In this regard, it is urgent to further tailor the structure of NFAs to broaden their absorption spectra while mitigating the energy loss of relevant devices concomitantly. Heteroatom substitution on the fused‐ring π‐core of NFAs is an efficient way to achieve this goal. In addition to improve the near‐infrared light harvest by strengthening the intramolecular charge transfer, it can also enhance the molecular stacking via forming multiple noncovalent interactions, which is favorable for reducing the energetic disorder. Therefore, in this review we focus on the design rules of NFAs, including the polymerized NFAs, of which the core moiety is substituted by various kinds of heteroatoms. We also afford a comprehensive understanding on the structure–property−performance relationships of these NFAs. Finally, we anticipate the challenges restricting the efficiency promotion and industrial utilization of OPV, and provide potential solutions based on the further heteroatom optimization on NFA core‐moiety. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: The morphology of the active layer plays a crucial role in the performance of organic photovoltaics. Although volatile additives are commonly used to manipulate the morphology, their mechanism of action remains poorly understood. In this study, we conducted a systematic exploration of the mechanism of the traditional volatile additive 1‐CN in film formation kinetics of typical PM6:Y6 system. We found that 1‐CN induces a secondary aggregation effect, improving film morphology and promoting face‐on crystalline orientation. Through elucidating its impact on exciton dynamics, we established a link between morphology optimization and increased exciton diffusion length and accelerated charge separation. Our findings unveil the unique mechanism of action of volatile additive, providing a new perspective for improving the morphology and enhancing the performance of organic photovoltaic devices. [ABSTRACT FROM AUTHOR]

Evaporable indano[60]fullerene ketone (FIDO) was converted to indano[60]fullerene thioketone (FIDS) in high yield by using Lawesson's reagent. Three compounds with different substituents in para position were successfully converted to the corresponding thioketones, showing that the reaction tolerates compounds with electron-donating and electron-withdrawing substituents. Computational studies with density functional theory revealed the unique vibrations of the thioketone group in FIDS. The molecular structure of FIDS was confirmed by single-crystal X-ray analysis. Bulk heterojunction organic solar cells using three evaporable fullerene derivatives (FIDO, FIDS, C60) as electron-acceptors were compared, and the open-circuit voltage with FIDS was 0.16 V higher than that with C60.

Intrinsically stretchable organic photovoltaic cells (OPVs) have garnered significant attention as crucial devices for powering next‐generation wearable electronics. Despite the rapid power conversion efficiency gains in champion OPVs, their brittle stretchability has failed to meet the demands of the Internet of Things era, severely hindering further development and practical applications. In this regard, a new dual‐donor polymer blending strategy is demonstrated for constructing intrinsically stretchable OPVs by designing a novel high‐molecular–weight conjugated polymer PM6‐HD. This PM6 derivative featuring long alkyl chains can reach a sufficiently high molecular weight and thus exhibits a high fracture strain exceeding 90%, which is ≈12 times higher than the benchmark PM6. Synergistic optimization of mechanical properties and photovoltaic performance in polymer:small molecule and all‐polymer systems constructed from the physical blends of PM6 and PM6‐HD is achieved. Crucially, the resulting intrinsically stretchable OPV demonstrates excellent stretchability and stability, with a record PCE80% strain of 50.3% and the efficiency retention of above 80% even after 1000 cycles of cyclic stretching at high strains. This work contributes to the advancement of intrinsically stretchable OPV technology and opens up new possibilities for its integration into wearable electronic devices. [ABSTRACT FROM AUTHOR]

Organic photovoltaics (OPV) has attracted tremendous attention as a promising alternative to silicon wafer‐based technologies for building integration. While significant progress has been achieved on the power conversion efficiency of OPV technologies, their field stability is rarely studied. This work investigates the field performance and reliability of a large‐area OPV module designed for building integration in tropical Singapore for 4.5 years. The device suffered more than 14% degradation in power at the standard testing conditions from the initial performance, largely due to losses in fill factor (−12% relative). During the monitoring period, it exhibited comparable performance to more conventional silicon PV technologies, with an average specific energy yield of about 4 kWh/kWp/day and an average performance ratio of 0.96. Excellent performance at low light conditions was also observed. However, its field performance was heavily impacted by soiling, which typically led to a 5 to 10% loss in the current output after several months. Further, the device's outdoor performance also showed a three‐stage degradation process, including (1) an initial slow degradation in the first 2 years (about −1%/year), (2) a stable period with negligible performance loss from Years 2 to 3.5, and (3) a rapid degradation in the last year (about −5%/year). [ABSTRACT FROM AUTHOR]

Organic photovoltaics (OPVs) show great promise for both outdoor and indoor applications. However, there remains a lack of understanding around the stability of OPVs, particularly for indoor applications. In this work, the photostability of the poly[(thiophene)‐alt‐(6,7‐difluoro‐2‐(2‐hexyldecyloxy)quinoxaline)]:2,2′‐((2Z,2′Z)‐((4,4,9,9‐tetrahexyl‐4,9‐dihydro‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene‐2,7‐diyl)bis(methanylylidene))bis(3‐oxo‐2,3‐dihydro‐1H‐indene‐2,1‐diylidene))dimalononitrile blend is investigated for both outdoor and indoor applications. Photostability is found to vary drastically with illumination intensity. Devices under high‐intensity white light‐emitting diode (LED) illumination, with their short‐circuit current density (JSC) matching JSC–EQE for AM1.5 G illumination, lose 42% of their initial performance after 30 days of illumination. Contrastingly, after almost 47 days of illumination devices under 1000 lux white LED illumination show no loss in performance. The poor photostability under 1 sun illumination is linked to the poor photostability of IDIC. Through Raman spectroscopy and mass spectrometry, IDIC is found to suffer from photoisomerization, which detrimentally impacts light absorption and carrier extraction. In this work, it is highlighted that under low light levels, the requirement of intrinsic material photostability may be less stringent. [ABSTRACT FROM AUTHOR]

Optimizing light utilization is crucial in organic photovoltaics. Understanding the intricate connection between the optical properties and the chemical structure of organic materials is pivotal yet challenging in this regard. Herein, over 2800 published reports with a database of ≈300 organic non‐fullerene acceptors (NFAs) are surveyed and a mathematical model suitable for predicting and analyzing the optical properties of organic photovoltaic materials is established. The model is used to predict the optical properties of representative NFAs within experimental error, including four newly synthesized organic materials to validate the model. In addition, the reliability and applicability of the model through data transformation are demonstrated and it is found that the addition of double bonds and asymmetry in the chemical structure does not necessarily reduce the optical bandgap of organic materials. Based on the model, the strong noncovalent interaction is more significant than the weak noncovalent interaction and asymmetry on the reduction of the bandgap, which provides new insights into the design and development of organic photovoltaic materials with tunable optical properties. [ABSTRACT FROM AUTHOR]

In this work, pseudo-bilayer planar heterojunction (PPHJ) all-polymer solar cells (APSCs) were constructed on the basis of the commonly used PY-IT and PM6 as the acceptor and donor, respectively. A nonfullerene small molecular acceptor (NF-SMA) BTP-eC9 was incorporated into the PY-IT layer as the solid additive in consideration of its similar building block to PY-IT. BTP-eC9 can serve as a photon capture reinforcer and morphology-regulating agent to realize more adequate photon capture, as well as a more orderly molecular arrangement for effective carrier transport. By incorporating 2 wt% BTP-eC9, the efficiency of PM6/PY-IT-based PPHJ-APSCs was boosted from 15.11% to 16.47%, accompanied by a synergistically enhanced short circuit current density (JSC, 23.36 vs. 24.08 mA cm−2) and fill factor (FF, 68.83% vs. 72.76%). In another all-polymer system, based on PBQx-TCl/PY-DT as the active layers, the efficiency could be boosted from 17.51% to 18.07%, enabled by the addition of 2 wt% L8-BO, which further verified the effectiveness of using an NF-SMA as a solid additive. This work demonstrates that incorporating an NF-SMA as a solid additive holds great potential for driving the development of PPHJ-APSCs. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Charge generation, a critical process in the operation of organic solar cell (OSC), requires thorough investigation in an ultrafast perspective. This work demonstrates that the utilization of alloy model for the non‐fullerene acceptor (NFA) component can regulate the crystallization properties of active layer films, which in turn affects exciton diffusion and hole transfer (HT), ultimately influencing the charge generation process. By incorporating BTP‐eC7 as a third component, without expanding absorption range or changing molecular energy levels but regulating the ultrafast exciton diffusion and HT processes, the power conversion efficiency (PCE) of the optimized PM6:BTP‐eC9:BTP‐eC7 based ternary OSC is improved from 17.30% to 17.83%, primarily due to the enhancement of short‐circuit current density (JSC). Additionally, the introduction of BTP‐eC7 also reduces the trap state density in the photoactive layer which helps to reduce the loss of JSC. This study introduces a novel approach for employing ternary alloy models by incorporating dual acceptors with similar structures, and elucidates the underlying mechanism of charge generation and JSC in ternary OSCs. [ABSTRACT FROM AUTHOR]

Within recent years, there has been an increased interest towards organic photovoltaics (OPVs), especially with their significant device performance reaching beyond 19% since 2022. With these advances in the device performance of laboratory-scaled OPVs, there has also been more attention directed towards using printing and coating methods that are compatible with large-scale fabrication. Though large-area (>100 cm2) OPVs have reached an efficiency of 15%, this is still behind that of laboratory-scale OPVs. There also needs to be more focus on determining strategies for improving the lifetime of OPVs that are suitable for scalable manufacturing, as well as methods for reducing material and manufacturing costs. In this paper, we compare several printing and coating methods that are employed to fabricate OPVs, with the main focus towards the deposition of the active layer. This includes a comparison of performances at laboratory (<1 cm2), small (1–10 cm2), medium (10–100 cm2), and large (>100 cm2) active area fabrications, encompassing devices that use scalable printing and coating methods for only the active layer, as well as "fully printed/coated" devices. The article also compares the research focus of each of the printing and coating techniques and predicts the general direction that scalable and large-scale OPVs will head towards. [ABSTRACT FROM AUTHOR]

The short exciton diffusion length in organic semiconductors results in a strong dependence of the conversion efficiency of organic photovoltaic (OPV) cells on the morphology of the donor-acceptor bulk-heterojunction blend. Strong light–matter coupling provides a way to circumvent this dependence by combining the favorable properties of light and matter via the formation of hybrid exciton–polaritons. By strongly coupling excitons in P3HT-C60 OPV cells to Fabry–Perot optical cavity modes, exciton-polaritons are formed with increased propagation lengths. We exploit these exciton–polaritons to enhance the internal quantum efficiency of the cells, determined from the external quantum efficiency and the absorptance. Additionally, we find a consistent decrease in the Urbach energy for the strongly coupled cells, which indicates the reduction of energetic disorder due to the delocalization of exciton–polaritons in the optical cavity. [ABSTRACT FROM AUTHOR]

Efficient and stable hole transport layer (HTL) is an important component of organic photovoltaics (OPV). Herein, a novel self‐assembled monolayer material of 4PADCB (short for (4‐(7H‐dibenzo[c,g]carbazol‐7‐yl)butyl)phosphonic acid) as HTL for non‐fullerene (NF) OPV is reported. Compared to the widely used PEDOT:PSS HTL, the usage of 4PADCB not only enhances photon incident and charge generation but also effectively improves the morphology of the upper active layer, promotes molecular packing, and balances the carrier transport within active layer. As a result, the single‐junction binary D18:L8BO OPV, employing 4PADCB as HTL, achieves a high‐power conversion efficiency (PCE) of 19.02% with excellent storage stability. Furthermore, a 19.3 cm2 OPV module comprising seven sub‐cells demonstrates a maximum PCE of 15.44%, which is the highest value of reported efficiency for large‐area binary OPV modules. Meanwhile, the module is the first demonstration of an OPV module based on self‐assembled monolayer material. This work underscores the substantial potential for the application of 4PADCB in efficient NF OPV devices and high‐throughput large‐area modules. [ABSTRACT FROM AUTHOR]

Organic‐inorganic heterostructures play a pivotal role in modern electronic and optoelectronic applications including photodetectors and field effect transistors, as well as in solar energy conversion such as photoelectrodes of dye‐sensitized solar cells, photoelectrochemical cells, and in organic photovoltaics. To a large extent, performance of such devices is controlled by charge transfer dynamics at and across (inner) interfaces, e.g. between a wide band gap semiconductor and molecular sensitizers and/or catalysts. Hence, a detailed understanding of the structure‐dynamics‐function relationship of such functional interfaces is necessary to rationalize possible performance limitations of these materials and devices on a molecular level. Vibrational sum‐frequency generation (VSFG) spectroscopy, as an interface‐sensitive spectroscopic technique, allows to obtain chemically specific information from interfaces and combines such chemical insights with ultrafast time resolution, when integrated as a spectroscopic probe into a pump‐probe scheme. Thus, this minireview discusses the advantages and potential of VSFG spectroscopy for investigating interfacial charge transfer dynamics and structural changes at inner interfaces. A critical perspective of the unique spectroscopic view of otherwise inaccessible interfaces is presented, which we hope opens new opportunities for an improved understanding of function‐determining processes in complex materials, and brings together communities who are devoted to designing materials and devices with spectroscopists. [ABSTRACT FROM AUTHOR]

The performance of organic solar cells is sensitive to the film thickness and the uniformity of the donor and acceptor distribution in the photoactive layer. Especially, in the quasi‐planar heterojunction fabricated by layer‐by‐layer process, the donor and acceptor materials may be non‐homogeneously distributed across the entire photoactive layer. Visualization of the spatial distributions of donor and acceptor components sheds light on the relationship between nanostructures and device performances. Based on the distinct infrared absorption characteristics of the organic donor and acceptor, a quasi‐monochromatic light transmittance (QMLT) technique is proposed to quantify the donor and/or acceptor thickness in the photoactive layer blend across the entire device area with nanometer precision. The variation in thickness of donor and acceptor can be clearly and separately revealed. Accordingly, the impacts of spin coating techniques (such as dynamic or static dispensing, and on‐center or off‐center spin coating), as well as solvent choices, on film morphology and device performance can be correlated by the noncontact, nondestructive, and convenient QMLT method. [ABSTRACT FROM AUTHOR]

Organic photovoltaics (OPV) present a promising thin-film solar cell technology with particular benefits in terms of weight, aesthetics, transparency, and cost. However, despite being studied intensively since the mid 90's, OPV has not entered the mass consumer market yet. Although the efficiency gap with other thin-film photovoltaics has largely been overcome, active layer stability and performance reproducibility issues have not been fully resolved. State-of-the-art OPV devices employ a physical mixture of electron donor and acceptor molecules in a bulk heterojunction active layer. These blends are prone to morphological changes, leading to performance losses over time. On the other hand, in "single-component" organic solar cells, the donor and acceptor constituents are chemically connected within a single material, preventing demixing and thereby enhancing device stability. Novel single-component materials affording reasonably high solar cell efficiencies and improved lifetimes have recently emerged. In particular, the combination of donor and acceptor structures in conjugated block copolymers (CBCs) presents an exciting approach. Nevertheless, the current CBCs are poorly defined from a structural point of view, while synthetic protocols remain unoptimized. More controlled synthesis followed by proper structural analysis of CBCs is, however, essential to develop rational structure-property-device relations and to drive the field forward. In this perspective, we provide a short overview of the state-of-the-art in single- component organic solar cells prepared from CBCs, reflect on their troublesome characterization and the importance of chemical precision in these structures, give some recommendations, and discuss the potential impact of these aspects on the field. [ABSTRACT FROM AUTHOR]

The selection of electron donors and nonfullerene acceptors (NFAs) in organic solar cells (OSCs) is crucial for improving photovoltaic performance. Machine learning (ML) has brought a breakthrough solution. Herein, 292 donor‐NFA pairs with experimental OSC parameters from the reported articles are collected. The ML descriptors include device processing parameters, molecular properties, and molecular structure. The five ML regression models, random forest (RF), extra tree regression, gradient boosting regression tree, adaptive boosting, and artificial neural network (ANN) are trained. GridSearchCV is used for hyperparameter optimization of ML regression models. The SHapley Additive exPlanation approach is employed to analyze descriptor importance. Among the trained five ML models, the RF model shows superior performance, achieving Pearson's correlation coefficient (r) of 0.81 on the test set. Based on the donors and NFAs in constructed dataset, the 9779 donor–NFA pairs for OSCs are generated by randomly combining donor and acceptor molecules. The trained RF model is utilized to predict the power conversion efficiency (PCE) of new donor–acceptor pairs for OSCs. The results indicate that the OSC composed of PBDB‐TF as donor and L8‐BO as acceptor can achieve the remarkable PCE of 17.9%. [ABSTRACT FROM AUTHOR]

Photoinduced intermolecular charge transfer (PICT) determines the voltage loss in bulk heterojunction (BHJ) organic photovoltaics (OPVs), and this voltage loss can be minimized by inducing efficient PICT, which requires energy‐state matching between the donor and acceptor at the BHJ interfaces. Thus, both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT. In this study, an effective method for quantifying the hot state matching of OPVs was developed. The degree of energy‐state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor (MF) calculated from the modified optical density of the BHJ. Furthermore, the correlation between the open‐circuit voltage (Voc) of the OPV device and energy‐state matching at the BHJ interface was investigated using the calculated MF. The OPVs with small absolute MF values exhibited high Voc values. This result clearly indicates that the energy‐state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs. Because the MF indicates the degree of energy‐state matching, which is a critical factor for suppressing energy loss, it can be used to estimate the Voc loss in OPVs. [ABSTRACT FROM AUTHOR]

Abstract Organic photovoltaics (OPVs) represent one of the most promising photovoltaic technologies owing to their high capacity to convert solar energy to electricity. With the continuous structure upgradation of photovoltaic materials, especially that of non‐fullerene acceptors (NFAs), the OPV field has witnessed rapid progress with power conversion efficiency (PCE) exceeding 19%. However, it remains challenging to overcome the intrinsic trade‐off between the photocurrent and photovoltage, restricting the further promotion of the OPV efficiency. In this regard, it is urgent to further tailor the structure of NFAs to broaden their absorption spectra while mitigating the energy loss of relevant devices concomitantly. Heteroatom substitution on the fused‐ring π‐core of NFAs is an efficient way to achieve this goal. In addition to improve the near‐infrared light harvest by strengthening the intramolecular charge transfer, it can also enhance the molecular stacking via forming multiple noncovalent interactions, which is favorable for reducing the energetic disorder. Therefore, in this review we focus on the design rules of NFAs, including the polymerized NFAs, of which the core moiety is substituted by various kinds of heteroatoms. We also afford a comprehensive understanding on the structure–property−performance relationships of these NFAs. Finally, we anticipate the challenges restricting the efficiency promotion and industrial utilization of OPV, and provide potential solutions based on the further heteroatom optimization on NFA core‐moiety.

In situ online observation of surface morphology during degradation processes is of paramount importance for exploring the stability of organic photovoltaic materials. In this study, we designed an in situ online characterization system based on hyperspectral and neural network technologies, and observed the degradation processes of P3HT:PCBM thin film materials. The system is capable of collecting hyperspectral image data from 101 channels within the 400–700 nm wavelength range for characterizing detailed surface features of materials. Additionally, to automate the processing of hyperspectral image data, we designed a spectral image segmentation algorithm based on neural networks and proposed a foreground attention mechanism to improve the segmentation accuracy of the algorithm. The experimental results indicate that the system can achieve high spectral characterization of P3HT:PCBM thin film materials and automate image data processing through artificial intelligence algorithms, with an image segmentation accuracy of 99.62 %. Furthermore, owing to the higher spectral resolution of this system and its computer-assisted analysis capabilities for material image data, not only are the in-situ variations in size, density, and formation rate of aggregates formed during the thermal degradation process of P3HT:PCBM thin film materials experimentally analyzed, but also the fluorescence changes at the edges of aggregates during the photodegradation process are revealed. The reliable code can be found at the following link: https://github.com/HyperSystemAndImageProc/IONFMDP-UHHNN.

In the field of organic photovoltaics (OPVs), significant progress has been made in tailoring molecular structures to enhance the open‐circuit voltage and the short‐circuit current density. However, there remains a crucial gap in the development of coordinated material design strategies focused on improving the fill factor (FF). Here, we introduce a molecular design strategy that incorporates electrostatic potential fluctuation to design organic photovoltaic materials. By reducing the fluctuation amplitude of IT‐4F, we synthesized a new acceptor named ITOC6‐4F. When using PBQx‐TF as a donor, the ITOC6‐4F‐based cell shows a markedly low recombination rate constant of 0.66×10−14 cm3 s−1 and demonstrates an outstanding FF of 0.816, both of which are new records for binary OPV cells. Also, we find that a small fluctuation amplitude could decrease the energetic disorder of OPV cells, reducing energy loss. Finally, the ITOC6‐4F‐based cell creates the highest efficiency of 16.0 % among medium‐gap OPV cells. Our work holds a vital implication for guiding the design of high‐performance OPV materials. [ABSTRACT FROM AUTHOR]

The layer‐by‐layer (LbL) organic photovoltaics (OPVs) are constructed with wide‐bandgap donor PM1 and narrow‐bandgap acceptor L8‐BO. The exciton utilization near cathode is still challenging considering restricted diffusion distance of excitons and inability for transferring energy from L8‐BO to PM1. Herein, donor incorporation into acceptor layer (DIA) strategy is employed to improve exciton utilization near cathode. The efficiency of LbL OPVs can be improved from 18.02% to 18.81% by incorporating 10 wt% PM1 into L8‐BO layer, which is closely associated with efficient exciton separation into L8‐BO layer originated from more adequate donor/acceptor interface for faster charge transfer, as evidenced by magneto‐photocurrent and transient absorption results. The in situ test and morphological characterization clarify that molecular packing property can be improved benefited from prolonged aggregation and nucleation time of acceptor layer assisted by DIA strategy, contributing to more efficient charge transport and inhibited charge recombination in active layers. The thickness insensitive property of LbL OPVs can be also improved induced by DIA strategy, indicated by PCE retention value (82.2% vs. 74.0%) for PM1/L8‐BO:PM1 and PM1/L8‐BO OPVs when acceptor layer thickness increased to ≈180 nm. This work demonstrates the effectiveness of DIA strategy in improving efficiency and thickness tolerance of LbL OPVs. [ABSTRACT FROM AUTHOR]

Future industrialization of organic photovoltaics (OPVs) requires OPVs' processing to be more energy‐efficient and streamlined. Currently, only MoO3 and PEDOT:PSS are commonly used as the anode interface layer (AIL). The processing of MoO3 typically involves vacuum thermal evaporation with stringent thickness requirements. PEDOT:PSS necessitates separate processing and thermal annealing at temperatures exceeding 100 °C to eliminate moisture. This work utilized 3,4,5‐trichlorobenzoic acid (3CBA) as the AIL material. The distinct advantage of 3CBA over PEDOT:PSS and MoO3 is the in situ self‐assembly of 3CBA eliminates the need for separate solution processing, thermal evaporation, or thermal annealing. Remarkably, OPV devices incorporating PM6, BTP‐eC9, and the 3CBA AIL exhibited a superior efficiency of 18.2% compared to those with PEDOT:PSS (17.7%). By using nonhalogenated solvent, o‐xylene, to meet industrialization requirements, the devices achieved an exceptional efficiency of 18.8%, the highest reported value among devices with in situ self‐assembled interface layers. Furthermore, semi‐transparent devices with 3CBA displayed higher PCE and AVT values (13.1% and 25.7%) than their PEDOT: PSS counterparts, due to the weak absorption of the 3CBA AIL. This work contributes significantly to the high‐throughput production of OPVs by streamlining the AIL processing. [ABSTRACT FROM AUTHOR]

The global energy landscape is in the midst of a transformative shift, compelled by the urgent need to reduce our reliance on fossil fuels and embrace eco-friendly alternatives. Organic photovoltaics (OPVs) have emerged as a promising alternative, offering the distinct advantage of performing well in low-light conditions, including indoor environments. Extensive research and development efforts are dedicated to realizing the full potential of OPVs as adaptable, cost-effective, and environmentally friendly solar energy solutions. This paper conducts a thorough examination of the intricate characterization of organic solar cells, with a specific emphasis on crucial parameters like power conversion efficiency, opencircuit voltage, and fill factor. The study utilizes a single diode model to simulate these cells' behavior, employing a meticulous process for parameter extraction. This method leverages Origin software and Python programming, incorporating open-source packages to ensure robust validation. This systematic and rigorous approach significantly enhances our comprehension of OPVs and plays a substantial role in optimizing their performance. In essence, this research represents a significant step forward in advancing sustainable energy technologies, laying a foundation for a greener and more environmentally conscious future. [ABSTRACT FROM AUTHOR]

The power conversion efficiency of organic photovoltaics (OPVs) has witnessed continuous breakthroughs in the past few years, mostly benefiting from the extensive use of a facile ternary blending strategy by blending the host polymer donor:small molecule acceptor mixture with a second small molecule acceptor. Nevertheless, this rather general strategy used in the well‐known PM6 systems fails in constructing high‐performance P3HT‐based ternary OPVs. As a result, the efficiencies of all resulting ternary blends based on a benchmark host P3HT:ZY‐4Cl and a second acceptor are no more than 8%. Employing the mutual miscibility of the binary blends as a guide to screen the second acceptor, here we were able to break the longstanding 10%‐efficiency barrier of ternary OPVs based on P3HT and dual nonfullerene acceptors. With this rational approach, we identified a multifunctional small molecule acceptor BTP‐2Br to simultaneously improve the photovoltaic performance in both P3HT and PM6‐based ternary OPVs. Attractively, the P3HT:ZY‐4Cl:BTP‐2Br ternary blend exhibited a record‐breaking efficiency of 11.41% for P3HT‐based OPVs. This is the first‐ever report that over 11% efficiency is achieved for P3HT‐based ternary OPVs. Importantly, the study helps the community to rely less on trial‐and‐error methods for constructing ternary solar cells. [ABSTRACT FROM AUTHOR]

Although fullerene derivatives such as [6,6]‐phenyl‐C61/C71‐butyric acid methyl ester (PC61BM/PC71BM) have dominated the the photoactive acceptor materials in bulk heterojunction organic solar cells (OSCs) for decades, they have several drawbacks such as weak absorption, limited structural tunability, prone to aggregation, and high costs of production. Constructing non‐fullerene small molecules with three‐dimensional (3D) molecular geometry is one of the strategies to replace fullerenes in OSCs. In this study, a 3D molecule, contorted hexa‐cata‐hexabenzocoronene tetra perylenediimide (HBC‐4‐PDI), was designed and synthesized. HBC‐4‐PDI shows a wide and strong light absorption in the whole UV‐vis region as well as suitable energy levels as an acceptor for OSCs. More importantly, the 3D construction effectively reduced the self‐aggregation of c‐HBC, leading to an appropriate scale phase separation of the blend film morphology in OSCs. A preliminary power conversion efficiency of 2.70 % with a champion open‐circuit voltage of 1.06 V was obtained in OSCs with HBC‐4‐PDI as the acceptor, which was the highest among the previously reported OSCs based on c‐HBC derivatives. The results indicated that HBC‐4‐PDI may serve as a good non‐fullerene acceptor for OSCs. [ABSTRACT FROM AUTHOR]

In the past five years, significant advancements in the development of novel conjugated polymer donors (D) and non‐fullerene acceptors (A), such as small molecules, have substantially boosted the power conversion efficiency of bulk heterojunction (BHJ) organic photovoltaics (OPVs) devices to over 19%. Recently, in the pursuit of broader impact and heightened efficiency for OPVs, an alternative processing approach has emerged; this approach involves a sequential deposition (SD) technique or a layer‐by‐layer method, creating active layers with p–i–n structures (p and n stand for D and A region, respectively; i stands for BHJ region). Notably, this SD method is particularly effective in semitransparent organic photovoltaics (ST‐OPVs), despite the material requirements it entails. SD‐processing methods enable the creation of vertical multiple junctions and controllable D/A interfaces, facilitating exciton dissociation and charge transport through a well‐designed pseudo p–i–n structure. Furthermore, ST‐OPVs can be integrated into building‐incorporated photovoltaic modules, offering potential applications in greenhouses and agricultural modernization. This integration allows for the comprehensive utilization of solar spectrum energy. In this review, current literature is consolidated on new materials, such as conjugated polymers and non‐fullerene small molecules as electron‐donating and electron‐withdrawing materials, aimed at high‐efficiency OPVs and ST‐OPVs with BHJ‐ and p–i–n structured active layers, and perspectives are offered for future developments. [ABSTRACT FROM AUTHOR]

Transient absorption spectroscopy (TAS) is a time‐resolved spectroscopic technique that can quantitatively observe temporal changes in the absorption spectrum associated with transient species, such as excitons and charges. Therefore, it is extensively used in photophysics, photochemistry, and photobiology. TAS plays a crucial role in unveiling charge generation and recombination dynamics in organic solar cells (OSCs). However, the interpretation of TA data is sometimes difficult for those who are not familiar with TAS. In this Perspective, therefore, the utility of TAS is briefly explained in studying OSCs and highlight key considerations for interpreting TA data. Measuring TA data at appropriate excitation fluence and appropriate spectral assignment are essential to correctly interpret photophysics of OSCs. With this Perspective, it aims to offer readers sufficient advice to enable them to perform TA measurements appropriately and interpret the TA data correctly. [ABSTRACT FROM AUTHOR]

Thanks to the development of novel electron acceptor materials, the power conversion efficiencies (PCE) of organic photovoltaic (OPV) devices are now approaching 20%. Further improvement of PCE is complicated by the need for a driving force to split strongly bound excitons into free charges, causing voltage losses. This review discusses recent approaches to finding efficient OPV systems with minimal driving force, combining near unity quantum efficiency (maximum short circuit currents) with optimal energy efficiency (maximum open circuit voltages). The authors discuss apparently contradicting results on the amount of exciton binding in recent literature, and approaches to harmonize the findings. A comprehensive view is then presented on motifs providing a driving force for charge separation, namely hybridization at the donor:acceptor interface and polarization effects in the bulk, of which quadrupole moments (electrostatics) play a leading role. Apart from controlling the energies of the involved states, these motifs also control the dynamics of recombination processes, which are essential to avoid voltage and fill factor losses. Importantly, all motifs are shown to depend on both molecular structure and process conditions. The resulting high dimensional search space advocates for high throughput (HT) workflows. The final part of the review presents recent HT studies finding consolidated structure–property relationships in OPV films and devices from various deposition methods, from research to industrial upscaling. [ABSTRACT FROM AUTHOR]

The global climate change negatively affects the photovoltaic performance of traditional solar cell technologies. This article investigates the potential of organic photovoltaics (OPV) for high‐temperature environments, ranging from urban hot summers (30—40 °C) and desert regions (65 °C) up to (aero) space conditions (130 °C), the thermal window in which OPV can operate. The approach is based on a combination of experiments and simulations up to 180 °C, moving significantly beyond the conventional temperature ranges reported in the literature. New 2H‐benzo[d][1,2,3]triazole‐5,6‐dicarboxylic imide‐based copolymers with decomposition onset temperatures above 340 °C are used for this study, in combination with non‐fullerene acceptors. Contrary to their inorganic counterparts, OPV devices show a positive temperature coefficient up to ≈90 °C. At temperatures of 150 °C, they are still operational, retaining their room temperature efficiency. Complementary simulations are performed using an in‐house developed software package that numerically solves the drift‐diffusion equations to understand the general trends in the obtained current–voltage characteristics and the materials' intrinsic behavior as a function of temperature. The presented methodology of combined high‐temperature experiments and simulations can be further applied to investigate the thermal window of operation for other OPV material systems, opening novel high‐temperature application routes. [ABSTRACT FROM AUTHOR]

Organic photovoltaics (OPVs) show great promise for both outdoor and indoor applications. However, there remains a lack of understanding around the stability of OPVs, particularly for indoor applications. In this work, the photostability of the poly[(thiophene)‐alt‐(6,7‐difluoro‐2‐(2‐hexyldecyloxy)quinoxaline)]:2,2′‐((2Z,2′Z)‐((4,4,9,9‐tetrahexyl‐4,9‐dihydro‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene‐2,7‐diyl)bis(methanylylidene))bis(3‐oxo‐2,3‐dihydro‐1H‐indene‐2,1‐diylidene))dimalononitrile blend is investigated for both outdoor and indoor applications. Photostability is found to vary drastically with illumination intensity. Devices under high‐intensity white light‐emitting diode (LED) illumination, with their short‐circuit current density (JSC) matching JSC–EQE for AM1.5 G illumination, lose 42% of their initial performance after 30 days of illumination. Contrastingly, after almost 47 days of illumination devices under 1000 lux white LED illumination show no loss in performance. The poor photostability under 1 sun illumination is linked to the poor photostability of IDIC. Through Raman spectroscopy and mass spectrometry, IDIC is found to suffer from photoisomerization, which detrimentally impacts light absorption and carrier extraction. In this work, it is highlighted that under low light levels, the requirement of intrinsic material photostability may be less stringent.