Herein, we investigated a series of fullerene-free organic solar cells (OSCs) based on six different donor:acceptor (D:A) blends with varied highest occupied molecular orbital (HOMO) offsets from −0.05 to 0.21 eV. First, to verify the energetic compatibility of a specific D:A pair, especially for HOMO offsets, we established a simple method to estimate the hole transfer tendencies between D and A by using bilayer hole-only devices. It reveals that the asymmetrical diode effect of the bilayer hole-only devices can correlate with the FF and J sc of the relevant OSCs. Second, to find out whether HOMO offset is the main restriction of hole transfer, we measured transient absorption spectra and examined the hole transfer behavior in the blends, revealing that the occurrence of hole transfer is independent of the HOMO offsets and ultrafast in the time scale of ≤4.6 ps for those blends with ≥0 eV HOMO offsets. In contrast, a negative HOMO offset can significantly slow down the hole transfer with a half-time of ∼400 ps. Furthermore, we compare the device parameters under varied light intensities and discover that the bimolecular recombination should be one of the main restrictions for high device performance. Surprisingly, small HOMO offsets of 0 and 0.06 eV can also enable high PCEs of 10.42% and 11.75% for blend 2 (PTQ10:HC-PCIC) and blend 3 (PBDB-TF:HC-PCIC), respectively. Overall, our work demonstrates not only the validity of high-performance OSCs operating at the near zero HOMO offsets but also the charge dynamic insights of these blends, which will help gain understanding on the further improvement of OSCs.
Charged defects at the surface of the organic–inorganic perovskite active layer are detrimental to solar cells due to exacerbated charge carrier recombination. Here we show that charged surface defects can be benign after passivation and further exploited for reconfiguration of interfacial energy band structure. Based on the electrostatic interaction between oppositely charged ions, Lewis-acid-featured fullerene skeleton after iodide ionization (PCBB-3N-3I) not only efficiently passivates positively charged surface defects but also assembles on top of the perovskite active layer with preferred orientation. Consequently, PCBB-3N-3I with a strong molecular electric dipole forms a dipole interlayer to reconfigure interfacial energy band structure, leading to enhanced built-in potential and charge collection. As a result, inverted structure planar heterojunction perovskite solar cells exhibit the promising power conversion efficiency of 21.1% and robust ambient stability. This work opens up a new window to boost perovskite solar cells via rational exploitation of charged defects beyond passivation.
Recent advances in material design for organic solar cells (OSCs) are primarily focused on developing near-infrared nonfullerene acceptors, typically A-DA′D-A type acceptors (where A abbreviates an electron-withdrawing moiety and D, an electron-donor moiety), to achieve high external quantum efficiency while maintaining low voltage loss. However, the charge transport is still constrained by unfavorable molecular conformations, resulting in high energetic disorder and limiting the device performance. Here, a facile design strategy is reported by introducing the "wing" (alkyl chains) at the terminal of the DA′D central core of the A-DA′D-A type acceptor to achieve a favorable and ordered molecular orientation and therefore facilitate charge carrier transport. Benefitting from the reduced disorder, the electron mobilities could be significantly enhanced for the "wing"-containing molecules. By carefully changing the length of alkyl chains, the mobility of acceptor has been tuned to match with that of donor, leading to a minimized charge imbalance factor and a high fill factor (FF). We further provide useful design strategies for highly efficient OSCs with high FF.
photovoltaic performance, as they not only maintain the simple device configuration and low-cost processing of single-junction polymer solar cells (PSCs), but also inherit the major benefit of incorporating multiple polymers in tandem cells. [1][2][3] In general, the third component mainly plays a role in energy transfer or electron transfer on the condition of proper cascaded energy levels, which lead to an increase in shortcircuit current density (J sc ) by extended absorption and more efficient charge generation. [2,[4][5][6] Besides, the third component with relatively high crystallinity may also act as a template to facilitate supramolecular assembly for achieving ideal morphology of active layer, [2,7,8,4] providing numerous D/A area for exciton dissociation and affording optimized phase separation to facilitate the charge transport. [9][10][11][12][13] Therefore, compared with the corresponding binary systems, TSCs have the potential to achieve higher light-harvesting and/or improved charge transport, leading to increased J sc and/or FF. [14][15][16] However, it should be noted that the emission of the third component and the absorption of the donor or acceptor must overlap in order to get efficient energy transfer. In addition, the morphology tuning highly depends on the crystallinity and miscibility properties of the materials involved. Unfortunately for ternary systems, Aimed at achieving ideal morphology, illuminating morphology-performance relationship, and further improving the power conversion efficiency (PCE) of ternary polymer solar cells (TSCs), a ternary system is designed based on PTB7-Th:PffBT4T-2OD:PC 71 BM in this work. The PffBT4T-2OD owns large absorption cross section, proper energy levels, and good crystallinity, which enhances exciton generation, charge dissociation and transport and suppresses charge recombination, thus remarkably increasing the short-circuit current density (J sc ) and fill factor (FF). Finally, a notable PCE of 10.72% is obtained for the TSCs with 15% weight ratio of PffBT4T-2OD. As for the working mechanism, it confirmed the energy transfer from PffBT4T-2OD to PTB7-Th, which contributes to the improved exciton generation. And morphology characterization indicates that the devices with 15% PffBT4T-2OD possess both appropriate domain size (25 nm) and enhanced domain purity. Under this condition, it affords numerous D/A interface for exciton dissociation and good bicontinuous nanostructure for charge transport simultaneously. As a result, the device with 15% PffBT4T-2OD exhibits improved exciton generation, enhanced charge dissociation possibility, elevated hole mobility and inhibited charge recombination, leading to elevated J sc (19.02 mA cm −2 ) and FF (72.62%) simultaneously. This work indicates that morphology optimization as well as energy transfer plays a significant role in improving TSC performance.
3D organic–inorganic hybrid halide perovskite solar cells (pero‐SCs) inherently face severe instability issue due to ion migration under operational conditions. This ion migration inevitably results from the decomposition of ionic bonds under lattice strain and is accelerated by the existence of excess charge carriers. In this study, a 1D–3D mixed‐dimensional perovskite material is explored by adding an organic salt with a bulk benzimidazole cation (Bn+). The Bn+ can induce 3D perovskite crystalline growth with the preferred orientation and form a 1D BnPbI3 perovskite spatially distributed in the 3D perovskite film. For the first time, the electro‐strictive response, which has a significant influence on the lattice strain under an electric field, is observed in polycrystalline perovskite. The 1D–3D perovskite can effectively suppress electro‐strictive responses and unbalanced charge carrier extraction, providing an intrinsically stable lattice with enhanced ionic bonds and fewer excess charge carriers. As a result, the ion migration behavior of the p‐i‐n 1D–3D based pero‐SC is dramatically suppressed under operational conditions, showing ultra‐long‐term stability that retains 95.3% of its initial power conversion efficiency (PCE) under operation for 3072 h, and simultaneously achieving an excellent PCE with a hysteresis‐free photovoltaic behavior.
Despite rapid advances in the field of nonfullerene polymer solar cells (NF‐PSCs), successful examples of random polymer‐based NF‐PSCs are limited. In this study, it is demonstrated that random donor polymers based on thieno[2′,3′:5′,6′]pyrido[3,4‐g]thieno[3,2‐c]isoquinoline‐5,11(4H,10H)‐dione (TPTI) containing two simple thiophene (T) and bithiophene (2T) electron‐rich moieties (PTTI‐Tx) can be promising materials for the fabrication of highly efficient NF‐PSCs. With negligible influence on optical bandgaps and energy levels, the crystalline behavior of PTTI‐Tx polymers was modulated by varying the T:2T ratio in the polymer backbone; this resulted in the formation of different microstructures upon blending with a nonfullerene m‐ITIC acceptor in NF‐PSCs. In particular, a PTPTI‐T70:m‐ITIC system enabled favorable small‐scale phase separation with an increased population of face‐on oriented crystallites, thereby boosting the processes of effective exciton dissociation and charge transport in the device. Consequently, the highest power conversion efficiency of 11.02% with an enhanced short‐circuit current density of 17.12 mA cm−2 is achieved for the random polymer‐based NF‐PSCs thus far. These results indicate that random terpolymerization is a simple and practical approach for the optimization of a donor polymer toward highly efficient NF‐PSCs.
Three small molecules with different substituents on bithienyl‐benzo[1,2‐b:4,5‐b′]dithiophene (BDTT) units, BDTT‐TR (meta‐alkyl side chain), BDTT‐O‐TR (meta‐alkoxy), and BDTT‐S‐TR (meta‐alkylthio), are designed and synthesized for systematically elucidating their structure–property relationship in solution‐processed bulk heterojunction organic solar cells. Although all three molecules show similar molecular structures, thermal properties and optical band gaps, the introduction of meta‐alkylthio‐BDTT as the central unit in the molecular backbone substantially results in a higher absorption coefficient, slightly lower highest occupied molecular orbital level and significantly more efficient and balanced charge transport property. The bridging atom in the meta‐position to the side chain is found to impact the microstructure formation which is a subtle but decisive way: carrier recombination is suppressed due to a more balanced carrier mobility and BDTT based devices with the meta‐alkylthio side chain (BDTT‐S‐TR) show a higher power conversion efficiency (PCE of 9.20%) as compared to the meta‐alkoxy (PCE of 7.44% for BDTT‐TR) and meta‐alkyl spacer (PCE of 6.50% for BDTT‐O‐TR). Density functional density calculations suggest only small variations in the torsion angle of the side chains, but the nature of the side chain linkage is further found to impact the thermal as well as the photostability of corresponding devices. The aim is to provide comprehensive insight into fine‐tuning the structure–property interrelationship of the BDTT material class as a function of side chain engineering.
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