Stereoisomeric Non-Fullerene Acceptors-Based Organic Solar Cells.

Chiral alkyl chains are ubiquitously observed in organic semiconductor materials and can regulate solution processability and active layer morphology, but the effect of stereoisomers on photovoltaic performance has rarely been investigated. For the racemic Y-type acceptors widely used in organic solar cells, it remains unknown if the individual chiral molecules separate into the conglomerate phase or if racemic phase prevails. Here, the photovoltaic performance of enantiomerically pure Y6 derivatives, (S,S)/(R,R)-BTP-4F, and their chiral mixtures are compared. It is found that (S,S) and (R,R)-BTP-4F molecule in the racemic mixtures tends to interact with its enantiomer. The racemic mixtures enable efficient light harvesting, fast hole transfer, and long polaron lifetime, which is conducive to charge generation and suppresses the recombination losses. Moreover, abundant charge diffusion pathways provided by the racemate contribute to efficient charge transport. As a result, the racemate system maximizes the power output and minimizes losses, leading to a higher efficiency of 18.16% and a reduced energy loss of 0.549 eV, as compared to the enantiomerically pure molecules. This study demonstrates that the chirality of non-fullerene acceptors should receive more attention and be designed rationally to enhance the efficiency of organic solar cells.

In Situ Formation of Iodide Precursor for Perovskite Quantum Dots with Application in Efficient Solar Cells.

Perovskite quantum dots (PQDs) become a kind of competitive material for fabricating high-performance solar cells due to their solution processability and outstanding optoelectronic properties. However, the current synthesis method of PQDs is mostly based on the binary-precursor method, which results in a large deviation of the I/Pb input ratio in the reaction system from the stoichiometric ratio of PQDs. Herein, a ternary-precursor method with an iodide source self-filling ability is reported for the synthesis of the CsPbI3 PQDs with high optoelectronic properties. Systematically experimental characterizations and theoretical calculations are conducted to fundamentally understand the effects of the I/Pb input molar ratio on the crystallographic and optoelectronic properties of PQDs. The results reveal that increasing the I/Pb input molar ratio can obtain ideal cubic structure PQDs with iodine-rich surfaces, which can significantly reduce the surface defects of PQDs and realize high orientation of PQD solids, facilitating charge carrier transport in the PQD solids with diminished nonradiative recombination. Consequently, the PQD solar cells exhibit an impressive efficiency of 15.16%, which is largely improved compared with that of 12.83% for the control solar cell. This work provides a feasible strategy for synthesizing high-quality PQDs for high-performance optoelectronic devices.

Tri-Step Water-Assisted Strategy for Suppressing Cs4PbBr6 Phase in Printable Carbon-Based CsPbBr3 Solar Cells to Achieve High Stability.

Often deemed the "natural nemesis" of perovskites, water molecules have been largely circumvented by the majority of researchers in the field of perovskite solar cells. This has resulted in significant hurdles in investigating the beneficial impacts of water molecules on perovskite crystallization. Herein, it is found that by utilizing ethanol with minimal water content and subjecting all-inorganic perovskite to three distinct annealing temperatures within the same solvent, the residual CsBr can be effectively removed, and the formation of the Cs4PbBr6 phase can be curtailed. By selecting an optimal water content, substantial improvements are observed in the crystalline quality of CsPbBr3, the perovskite/carbon interface, and the mesoporous filling effect. The Urbach energy (Eu) is reduced from 38.96 to 35.59 meV, and the defect density decreased from 4.16 × 1014 to 3.39 × 1014 cm-3. As a result, the power conversion efficiency (PCE) improved from 7.55% in the control group to 9.37%. Under severe environmental conditions with a temperature (T) of 85 °C and a relative humidity (RH) of 40%, tracking tests over 1200 h retained 89.3% of the initial PCE. This research signifies a breakthrough in the fabrication of highly stable and efficient all-inorganic printable mesoscopic perovskite solar cells.

Molecular Design of Active Layer for High-Performance Stretchable Organic Solar Cells.

Stretchable organic solar cells (SOSCs) have advanced rapidly in the last few years as power sources required to realize portable and wearable electronics become available. Through rational material and device engineering, SOSCs are now able to retain their photovoltaic performance even when subjected to repeated mechanical deformations. However, reconciling a high efficiency and an excellent stretchability is still a huge challenge, and the development of SOSCs has lagged far behind that of flexible OSCs. In this perspective article, recent strategies for imparting mechanical robustness to SOSCs while maintaining high power conversion efficiency are reviewed, with emphasis on the molecular design of active layers. Initially, an overview of molecular design approaches and recent research advances is provided in improving the stretchability of active layers, including donors, acceptors, and single-component materials. Subsequently, another common strategy for regulating photovoltaic and mechanical properties of SOSCs, namely multi-component system, is summarized and analyzed. Lastly, considering that SOSCs research is in its infancy, the current challenges and future directions are pointed out.

Fabrication of Erbium-Doped Upconversion Nanoparticles and Carbon Quantum Dots for Efficient Perovskite Solar Cells.

Upconversion nanoparticles (UCNPs) and carbon quantum dots (CQDs) have emerged as promising candidates for enhancing both the stability and efficiency of perovskite solar cells (PSCs). Their rising prominence is attributed to their dual capabilities: they effectively passivate the surfaces of perovskite-sensitive materials while simultaneously serving as efficient spectrum converters for sunlight. In this work, we synthesized UCNPs doped with erbium ions as down/upconverting ions for ultraviolet (UV) and near-infrared (NIR) light harvesting. Various percentages of the synthesized UCNPs were integrated into the mesoporous layers of PSCs. The best photovoltaic performance was achieved by a PSC device with 30% UCNPs doped in the mesoporous layer, with PCE = 16.22% and a fill factor (FF) of 74%. In addition, the champion PSCs doped with 30% UCNPs were then passivated with carbon quantum dots at different spin coating speeds to improve their photovoltaic performance. When compared to the pristine PSCs, a fabricated PSC device with 30% UCNPs passivated with CQDs at a spin coating speed of 3000 rpm showed improved power conversion efficiency (PCE), from 16.65% to 18.15%; a higher photocurrent, from 20.44 mA/cm2 to 22.25 mA/cm2; and a superior fill factor (FF) of 76%. Furthermore, the PSCs integrated with UCNPs and CQDs showed better stability than the pristine devices. These findings clear the way for the development of effective PSCs for use in renewable energy applications.

Dipolar Chemical Bridge Induced CsPbI3 Perovskite Solar Cells with 21.86 % Efficiency.

CsPbI3 perovskite receives tremendous attention for photovoltaic applications due to its ideal band gap and good thermal stability. However, CsPbI3 perovskite solar cells (PSCs) significantly suffer from photovoltage deficits because of serious interfacial energy losses within the PSCs, which to a large extent affects the photovoltaic performance of PSCs. Herein, a dipolar chemical bridge (DCB) is constructed between the perovskite and TiO2 layers to lower interfacial energy losses and thus improve the charge extraction of PSCs. The results reveal that the DCB could form a beneficial interfacial dipole between the perovskite and TiO2 layers, which could optimize the interfacial energetics of perovskite/TiO2 layers and thus improve the energy level alignment within the PSCs. Meanwhile, the constructed DCB could also simultaneously passivate the surface defects of perovskite and TiO2 layers, greatly lowering interfacial recombination. Consequently, the photovoltage deficit of CsPbI3 PSCs is largely reduced, leading to a record efficiency of 21.86 % being realized. Meanwhile, the operation stability of PSCs is also largely improved due to the high-quality perovskite films with released interfacial tensile strain being obtained after forming the DCB within the PSCs.

Physical Fields Manipulation for High-Performance Perovskite Photovoltaics.

With the efforts of researchers from all over the world, metal halide perovskite solar cells (PSCs) have been booming rapidly in recent years. Generally, perovskite films are sensitive to surrounding conditions and will be changed under the action of physical fields, resulting in lattice distortion, degradation, ion migration, and so on. In this review, the progress of physical fields manipulation in PSCs, including the electric field, magnetic field, light field, stress field, and thermal field are reviewed. On this basis, the influences of these fields on PSCs are summarized and prospected. Finally, challenges and prospective research directions on how to make better use of external-fields while minimizing the unnecessary and disruptive impacts on commercial PSCs with high-efficiency and steady output are proposed.

Understanding the Photovoltaic Performance of Perovskite-Spirobifluorene Solar Cells.

Lead halide perovskite solar cells with remarkable power conversion efficiency have attracted much attention in recent years. However, there still exist many problems with their use that are not completely understood, and further studies are needed. Herein, the hole-transport layer dependence of the photovoltaic performance of perovskite solar cells is investigated in detail. It is found that devices freshly prepared using pristine 2,2',7,7'-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD) and Li-doped spiro-OMeTAD as hole-transport layers exhibit S-shaped current density-voltage curves with poor fill factors. The devices show progressively improved fill factors and efficiencies upon exposure to air, which is attributed to air-induced conductivity improvement in the spiro-OMeTAD layer. After introducing a cobalt salt dopant (FK209) into the spiro-OMeTAD layer, the corresponding devices show remarkable performance without the need of air exposure. These results confirm that the dopant not only increases the conductivity of spiro-OMeTAD layer, but also tunes the surface potential, which helps to improve charge transport and reduce the recombination loss.

Effect of Isomeric Structures on Photovoltaic Performance of D-A Copolymers.

Two donor-acceptor copolymers based on isomeric acceptor units, [7,7'-bithieno[2',3':4,5]thieno[2,3-d]thieno[3,2-b]pyridine]-5,5'(4H,4'H)-dione (BTTP) and [2,2'-bithieno[2',3':4,5]thieno[2,3-d]thieno[3,2-b]pyridine]-5,5'(4H,4'H)-dione (iBTTP), are developed to study the effect of isomeric structures on photovoltaic performance. Compared with PBDTBTTP, PBDTiBTTP possesses a smaller bandgap for good light harvesting and a better π-π stacking for higher hole mobility. PBDTiBTTP solar cells present balanced mobilities and good nanoscale phase separation, giving a power conversion efficiency (PCE) of 6.51%, with higher short-circuit current (Jsc ) and fill factor (FF).

Hexylammonium Acetate-Regulated Buried Interface for Efficient and Stable Perovskite Solar Cells.

Due to current issues of energy-level mismatch and low transport efficiency in commonly used electron transport layers (ETLs), such as TiO2 and SnO2, finding a more effective method to passivate the ETL and perovskite interface has become an urgent matter. In this work, we integrated a new material, the ionic liquid (IL) hexylammonium acetate (HAAc), into the SnO2/perovskite interface to improve performance via the improvement of perovskite quality formed by the two-step method. The IL anions fill oxygen vacancy defects in SnO2, while the IL cations interact chemically with Pb2+ within the perovskite structure, reducing defects and optimizing the morphology of the perovskite film such that the energy levels of the ETL and perovskite become better matched. Consequently, the decrease in non-radiative recombination promotes enhanced electron transport efficiency. Utilizing HAAc, we successfully regulated the morphology and defect states of the perovskite layer, resulting in devices surpassing 24% efficiency. This research breakthrough not only introduces a novel material but also propels the utilization of ILs in enhancing the performance of perovskite photovoltaic systems using two-step synthesis.

Rejuvenating Aged Perovskite Quantum Dots for Efficient Solar Cells.

Perovskite quantum dots (PQDs) have emerged as one of the most promising candidates for next-generation solar cells owing to its remarkable optoelectronic properties and solution processability. However, the optoelectronic properties of PQDs suffer from severe degradation in storage due to the dynamically binding ligands, predominantly affecting photovoltaic applications. Herein, an in situ defect healing treatment (DHT) is reported to effectively rejuvenate aged PQDs. Systematically, experimental studies and theoretical calculations are performed to fundamentally understand the causes leading to the recovered optoelectronic properties of aged PQDs. The results reveal that the I3 - anions produced from tetra-n-octylammonium iodide and iodine could strongly anchor on the surface matrix defects of aged PQDs, substantially diminishing the nonradiative recombination of photogenerated charge carriers. Meanwhile, an DHT could also renovate the morphology of aged PQDs and thus improve the stacking orientation of PQD solids, substantially ameliorating charge carrier transport within PQD solids. Consequently, by using a DHT, the PQD solar cell (PQDSC) yields a high efficiency of up to 15.88%, which is comparable with the PQDSCs fabricated using fresh PQDs. Meanwhile, the stability of PQDSCs fabricated using the rejuvenated PQDs is also largely improved.

High-Quality Hybrid Perovskite Thin Films by Post-Treatment Technologies in Photovoltaic Applications.

Incredible progress in photovoltaic devices based on hybrid perovskite materials has been made in the past few decades, and a record-certified power conversion efficiency (PCE) of over 26% has been achieved in single-junction perovskite solar cells (PSCs). In the fabrication of high-efficiency PSCs, the postprocessing procedures toward perovskites are essential for designing high-quality perovskite thin films; developing efficient and reliable post-treatment techniques is very important to promote the progress of PSCs. Here, recent post-treatment technological reforms toward perovskite thin films are summarized, and the principal functions of the post-treatment strategies on the design of high-quality perovskite films have been thoroughly analyzed by dividing into two categories in this review: thermal annealing (TA)-related technique and TA-free technique. The latest research progress of the above two types of post-treatment techniques is summarized and discussed, focusing on the optimization of postprocessing conditions, the regulation of perovskite qualities, and the enhancement of device performance. Finally, an outlook of the prospect trends and future challenges for the fabrication of the perovskite layer and the production of highly efficient PSCs is given.

Band Engineering of Perovskite Quantum Dot Solids for High-Performance Solar Cells.

CsPbI3 perovskite quantum dot (PQD) shows high potential for next-generation photovoltaics due to their tunable surface chemistry, good solution-processability and unique photophysical properties. However, the remained long-chain ligand attached to the PQD surface significantly impedes the charge carrier transport within the PQD solids, thereby predominantly influencing the charge extraction of PQD solar cells (PQDSCs). Herein, a ligand-induced energy level modulation is reported for band engineering of PQD solids to improve the charge extraction of PQDSCs. Detailed theoretical calculations and systemic experimental studies are performed to comprehensively understand the photophysical properties of the PQD solids dominated by the surface ligands of PQDs. The results reveal that 4-nitrobenzenethiol and 4-methoxybenzenethiol molecules with different dipole moments can firmly anchor to the PQD surface through the thiol group to modulate the energy levels of PQDs, and a gradient band structure within the PQD solid is subsequently realized. Consequently, the band-engineered PQDSC delivers an efficiency of up to 16.44%, which is one of the highest efficiencies of CsPbI3 PQDSCs. This work provides a feasible avenue for the band engineering of PQD solids by tuning the surface chemistry of PQDs for high-performing solar cells or other optoelectronic devices.

Providing a Photovoltaic Performance Enhancement Relationship from Binary to Ternary Polymer Solar Cells via Machine Learning.

Ternary polymer solar cells (PSCs) are currently the simplest and most efficient way to further improve the device performance in PSCs. To find high-performance organic photovoltaic materials, the established connection between the material structure and device performance before fabrication is of great significance. Herein, firstly, a database of the photovoltaic performance in 874 experimental PSCs reported in the literature is established, and three different fingerprint expressions of a molecular structure are explored as input features; the results show that long fingerprints of 2D atom pairs can contain more effective information and improve the accuracy of the models. Through supervised learning, five machine learning (ML) models were trained to build a mapping of the photovoltaic performance improvement relationship from binary to ternary PSCs. The GBDT model had the best predictive ability and generalization. Eighteen key structural features from a non-fullerene acceptor and the third components that affect the device's PCE were screened based on this model, including a nitrile group with lone-pair electron, a halogen atom, an oxygen atom, etc. Interestingly, the structural features for the enhanced device's PCE were essentially increased by the Jsc or FF. More importantly, the reliability of the ML model was further verified by preparing the highly efficient PSCs. Taking the PM6:BTP-eC9:PY-IT ternary PSC as an example, the PCE prediction (18.03%) by the model was in good agreement with the experimental results (17.78%), the relative prediction error was 1.41%, and the relative error between all experimental results and predicted results was less than 5%. These results indicate that ML is a useful tool for exploring the photovoltaic performance improvement of PSCs and accelerating the design and application with highly efficient non-fullerene materials.

Smart Photovoltaic Windows for Next-Generation Energy-Saving Buildings.

The global energy system transforming from fossil fuels to renewable green energy through the adaption of innovative and dynamic green technologies. Energy-saving buildings (ESBs) are attracting extensive attention as intelligent architectures capable of significantly reducing the energy consumption for heating, air-conditioning, and lighting. They provide comfortable working and living environment by regulating and harnessing solar energy. Smart photovoltaic windows (SPWs) offer a promising platform for designing ESBs due to their unique feature. They can modulate solar energy based on dynamic color switching behavior under external stimuli and generate electrical power by harvesting solar energy. In this review, the-state-of-art of strategies and technologies are summarized putting SPWs toward high-efficiency ESBs. The SPWs are systematically categorized according to the working principle and functional component. For each type of SPWs, material and architecture engineering are focused on to optimize operation mode, optical modulation capability, photovoltaic performance and durability for giving ESBs flexible manipulation, extraordinary energy-saving effect, and high electricity power. In addition, the challenges and opportunities in this cutting-edge research area are discussed, with the aim of promoting the development of advanced multifunctional SPWs and their application in high efficiency ESBs.

Compositionally Graded MoS2xTe2(1-x)/MoS2 van der Waals Heterostructures for Ultrathin Photovoltaic Applications.

van der Waals heterojunctions utilizing two-dimensional (2D) transition-metal dichalcogenide (TMD) materials have emerged as focal points in the field of optoelectronic devices, encompassing applications in light-emitting devices, photodetectors, solar cells, and beyond. In this study, we transferred few-atomic-layer films of compositionally graded ternary MoS2xTe2(1-x) alloys onto metal-organic chemical vapor deposition-grown molybdenum disulfide (MoS2) as p- and n-type structures, leading to the creation of a van der Waals vertical heterostructure. The characteristics of the fabricated MoS2xTe2(1-x)/MoS2 vertical-stacked heterojunction were investigated considering the influence of tellurium (Te) incorporation. The systematic variation of parameter x (i.e., 0.8, 0.6, 0.5, 0.3, and 0) allowed for an exploration of the impact of Te incorporation on the photovoltaic performance of these heterojunctions. As a result, the power conversion efficiency was enhanced by approximately 6 orders of magnitude with increasing Te concentration; notably, photoresponsivities as high as ∼6.4 A/W were achieved. These findings emphasize the potential for enhancing ultrathin solar energy conversion in heterojunctions based on 2D TMDs.

Harnessing synergistic effects in GQD@Pt(II) nanocomposites for enhanced photovoltaic performance: a computational study.

CONTEXT: The development of efficient solar energy conversion technologies is crucial for addressing global energy challenges and reducing reliance on fossil fuels. Platinum(II) complexes are promising materials for photovoltaic applications due to their strong light absorption and long-lived excited states. However, their narrow absorption in the visible spectrum and stability issues limit their performance. Combining platinum(II) complexes with graphene quantum dots (GQDs) can enhance photovoltaic performance by leveraging the complementary light harvesting and charge transfer characteristics of the two components. This study utilizes density functional theory (DFT) calculations to explore their electronic structures, charge transfer dynamics, and photoelectric performance. Specifically, it investigates the effects of incorporating different substituents, either electron-donating or electron-withdrawing, onto the fluorene motif of the Pt(II) complex. The findings reveal that combining GQDs with Pt(II) complexes extends light absorption into the UV range, enabling comprehensive solar utilization. Upon photoexcitation, electrons migrate between the GQD conduction band and the Pt(II) complex, stabilizing charges and enhancing extraction. Substituents significantly influence charge transfer dynamics: electron-withdrawing groups promote transfer to the GQD, while electron-donating groups encourage charge separation and delocalization. Nanocomposites featuring electron-donating substituents achieve the highest energy conversion efficiencies, with GQD@Pt(II)-NPh2 reaching 24.6%. This is attributed to improved light harvesting, efficient charge injection, and reduced recombination. These insights guide the rational design of GQD-Pt(II) nanocomposites, optimizing charge separation and transfer processes for enhanced photovoltaic performance. The computational approach employed here provides a robust tool for developing advanced materials in renewable energy technologies. METHODS: The computational studies reported in this work were performed using the DFT approach, specifically employing the hybrid functional PBE0. The PBE0 functional's accuracy in describing electronic structures and excited-state properties is essential for understanding charge transfer processes, photoabsorption, and emission characteristics in metal-organic complexes. Geometry optimizations and time-dependent DFT (TD-DFT) calculations were carried out to investigate the properties of the nanocomposites. The effects of solvents were replicated using the conductor-like polarizable continuum model (CPCM). The charge transfer length (ΔL) and interfragment charge transfer (ΔQ) were calculated using the Multiwfn software package, and all calculations were performed using the BDF software package.

Effect of Number and Position of Chlorine Atoms on the Photovoltaic Performance of Asymmetric Nonfullerene Acceptors.

It has been well proved that the introduction of halogen can effectively modify the optoelectronic properties of classic symmetric nonfullerene acceptors (NFAs). However, the relevant studies for asymmetric NFAs are limited, especially the effect of halogen substitution number and position on the photovoltaic performance is not clear. In this work, four asymmetric NFAs with A-D-A1-A2 structure are developed by tuning the number and position of chlorine atoms on the 1,1-dicyanomethylene-3-indanone end groups, namely, A303, A304, A305, and A306. The related NFAs show progressively deeper energy levels and red-shifted absorption spectra as the degree of chlorination increases. The PM6:A306-constructed organic solar cells (OSCs) give a champion power conversion efficiency (PCE) of 13.03%. This is mainly ascribed to the most efficient exciton dissociation and collection, suppressed charge recombination, and optimal morphology. Moreover, by alternating the substitution position, the PM6:A305-based device yielded a higher PCE of 12.53% than that of PM6:A304 (12.05%). This work offers fresh insights into establishing excellent asymmetric NFAs for OSCs.

Building a Charge Transfer Bridge between g-C3N4 and Perovskite with Molecular Engineering to Achieve Efficient Perovskite Solar Cells.

Effective defect passivation and efficient charge transfer within polycrystalline perovskite grains and corresponding boundaries are necessary to achieve highly efficient perovskite solar cells (PSCs). Herein, focusing on the boundary location of g-C3N4 during the crystallization modulation on perovskite, molecular engineering of 4-carboxyl-3-fluorophenylboronic acid (BF) on g-C3N4 was designed to obtain a novel additive named BFCN. With the help of the strong bonding ability of BF with both g-C3N4 and perovskite and favorable intramolecular charge transfer within BFCN, not only has the crystal quality of perovskite films been improved due to the effective defects passivation, but the charge transfer has also been greatly accelerated due to the formation of additional charge transfer channels on the grain boundaries. As a result, the champion BFCN-based PSCs achieve the highest photoelectric conversion efficiency (PCE) of 23.71% with good stability.

Spiro-Bifluorene-Cored Dopant-Free Conjugated Polymeric Hole-Transporting Materials Containing Passivation Parts for Inverted Perovskite Solar Cells.

Two spiro-bifluorene-based dopant-free HTMs (X22 and X23) have been synthesized by facilely condensing spiro-bifluorene diamine with 3,4-ethylenedioxythiophene (EDOT)-5,7-dicarbonyl dichloride and 2,3,5,6-tetrafluoro-terephthaloyl dichloride, respectively. In the X22 molecule, lone pairs of electrons on the sulfur (S) and oxygen (O) functional groups interact with the perovskite materials. The hole mobility (µh) of X22 (3.9 × 10-4 cm2 V-1 S1-) is more than twice that of X23 (1.4 × 10-4 cm2 V-1 S1-). The conductivity (σ0) of X22 is 2.73 × 10-4 S cm-1, which is also higher than that of X23 (2.39 × 10-4 S cm-1). The EDOT moiety benefits the contact angle of CH3NH3PbI3 precursor solutions on HTMs as low as 24°. The X22-based device with an indium-doped tin oxide/hole transport material (HTM)/CH3NH3PbI3/phenyl-C61-butyric acid methyl ester (PC61BM)/bathocuproine/Ag structure achieves a power conversion efficiency (PCE) of 19.18%. The PCE of the device based on X23 containing fluorine is 18.70%, and the contact angle between HTM and the perovskite precursor solution is 32°. The X22- and X23-based devices at ambient temperature (≈25 °C) in N2 retain 86% and 79% of the initial PCE after 150 days. The effect of S, O, and F heteroatoms plays an important role in the side chain modification of HTMs, improving defect passivation in HTM/CH3NH3PbI3 interfaces by multiple functional groups.