To make organic solar cells (OSCs) more competitive in the diverse photovoltaic cell technologies, it is very important to demonstrate that OSCs can achieve very good efficiencies and that their cost can be reduced. Here, a pair of nonfullerene small-molecule acceptors, IT-2Cl and IT-4Cl, is designed and synthesized by introducing easy-synthesis chlorine substituents onto the indacenodithieno[3,2-b]thiophene units. The unique feature of the large dipole moment of the CCl bond enhances the intermolecular charge-transfer effect between the donor-acceptor structures, and thus expands the absorption and down shifts the molecular energy levels. Meanwhile, the introduction of CCl also causes more pronounced molecular stacking, which also helps to expand the absorption spectrum. Both of the designed OSCs devices based on two acceptors can deliver a power conversion efficiency (PCE) greater than 13% when blended with a polymer donor with a low-lying highest occupied molecular orbital level. In addition, since IT-2Cl and IT-4Cl have very good compatibility, a ternary OSC device integrating these two acceptors is also fabricated and obtains a PCE greater than 14%. Chlorination demonstrates effective ability in enhancing the device performance and facile synthesis route, which both deserve further exploitation in the modification of photovoltaic materials.
To simultaneously achieve low photon energy loss ( E) and broad spectral response, the molecular design of the wide band gap (WBG) donor polymer with a deep HOMO level is of critical importance in fullerene-free polymer solar cells (PSCs). Herein, we developed a new benzodithiophene unit, i.e., DTBDT-EF, and conducted systematic investigations on a WBG DTBDT-EF-based donor polymer, namely, PDTB-EF-T. Due to the synergistic electron-withdrawing effect of the fluorine atom and ester group, PDTB-EF-T exhibits a higher oxidation potential, i.e., a deeper HOMO level (ca. -5.5 eV) than most well-known donor polymers. Hence, a high open-circuit voltage of 0.90 V was obtained when paired with a fluorinated small molecule acceptor (IT-4F), corresponding to a low E of 0.62 eV. Furthermore, side-chain engineering demonstrated that subtle side-chain modulation of the ester greatly influences the aggregation effects and molecular packing of polymer PDTB-EF-T. With the benefits of the stronger interchain π-π interaction, the improved ordering structure, and thus the highest hole mobility, the most symmetric charge transport and reduced recombination are achieved for the linear decyl-substituted PDTB-EF-T (P2)-based PSCs, leading to the highest short-circuit current density and fill factor (FF). Due to the high Flory-Huggins interaction parameter (χ), surface-directed phase separation occurs in the P2:IT-4F blend, which is supported by X-ray photoemission spectroscopy results and cross-sectional transmission electron microscope images. By taking advantage of the vertical phase distribution of the P2:IT-4F blend, a high power conversion efficiency (PCE) of 14.2% with an outstanding FF of 0.76 was recorded for inverted devices. These results demonstrate the great potential of the DTBDT-EF unit for future organic photovoltaic applications.
Besides broadening of the absorption spectrum, modulating molecular energy levels, and other well-studied properties, a stronger intramolecular electron push-pull effect also affords other advantages in nonfullerene acceptors. A strong push-pull effect improves the dipole moment of the wings in IT-4F over IT-M and results in a lower miscibility than IT-M when blended with PBDB-TF. This feature leads to higher domain purity in the PBDB-TF:IT-4F blend and makes a contribution to the better photovoltaic performance. Moreover, the strong push-pull effect also decreases the vibrational relaxation, which makes IT-4F more promising than IT-M in reducing the energetic loss of organic solar cells. Above all, a power conversion efficiency of 13.7% is recorded in PBDB-TF:IT-4F-based devices.
With rapid development for tens of years, organic solar cells (OSCs) have attracted much attention for their potential in practical applications. As an important photovoltaic parameter, the fill factor (FF) of OSCs stands for the effectiveness of charge generation and collection, which significantly depends on the properties of the interlayer and active layer. Here, a facile and effective strategy to improve the FF through hole-transporting layer (HTL) modification is demonstrated. By mixing WO nanoparticles with a poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) emulsion, the surface free energy of the HTL is improved and the morphology of the active layer is optimized. Benefiting from increased carrier lifetime, a device based on WO :PEDOT:PSS HTL exhibits a boosted performance with an FF of 80.79% and power conversion efficiency of 14.57% PCE. The results are certified by the National Institute of Metrology (NIM), which, to date, are the highest values in this field with certification. This work offers a simple and viable option of HTL modification to realize highly efficient OSCs.
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