The photovoltaic performance of poly(3-hexylthiophene) (P3HT) has been improved greatly by using indene–C60 bisadduct (ICBA) as acceptor instead of phenyl-C61-butyric acid methyl ester (PCBM). However, the solvent of dichlorobenzene (DCB) used in fabricating polymer solar cells (PSCs) limited the application of the PSCs, because of the environmental problem caused by the harmful halogenated solvent. In this work, we fabricated the PSCs based on P3HT/ICBA processed with four low-harmful non-halogenated solvents of toluene, o-xylene, m-xylene, and p-xylene. The PSCs based on P3HT/ICBA (1:1, w/w) with toluene as the solvent exhibit the optimized power conversion efficiency (PCE) of 4.5% with open-circuit voltage (Voc) of 0.84 V, short circuit current density (Jsc) of 7.2 mA/cm2, and fill factor (FF) of 71%, under the illumination of AM 1.5G at 100 mW/cm2. Upon using 1% N-methyl pyrrolidone (NMP) as a solvent additive in the toluene solvent, the PCE of the PSCs was greatly improved to 6.6% with a higher Jsc of 10.3 mA/cm2 and a high FF of 75%, which is even higher than that of the devices fabricated with halogenated DCB solvent. The X-ray diffraction (XRD) measurement shows that the crystallinity of P3HT increased with the NMP additive. The investigations on morphology of the active layers by atomic force microscopy (AFM) and transmission electron microscopy (TEM) indicate that the NMP additive promotes effective phase separation and formation of nanoscaled interpenetrating network structure of the active layer, which is beneficial to the improvement of Jsc and PCE for the PSCs fabricated with toluene as the solvent.Keywords: indene−C60 bisadduct; N-methyl pyrrolidone additive; non-halogenated solvents; polymer solar cells; toluene solvent;

The photovoltaic performance of poly(3-hexylthiophene) (P3HT) has been improved greatly by using indene–C60 bisadduct (ICBA) as acceptor instead of phenyl-C61-butyric acid methyl ester (PCBM). However, the solvent of dichlorobenzene (DCB) used in fabricating polymer solar cells (PSCs) limited the application of the PSCs, because of the environmental problem caused by the harmful halogenated solvent. In this work, we fabricated the PSCs based on P3HT/ICBA processed with four low-harmful non-halogenated solvents of toluene, o-xylene, m-xylene, and p-xylene. The PSCs based on P3HT/ICBA (1:1, w/w) with toluene as the solvent exhibit the optimized power conversion efficiency (PCE) of 4.5% with open-circuit voltage (Voc) of 0.84 V, short circuit current density (Jsc) of 7.2 mA/cm2, and fill factor (FF) of 71%, under the illumination of AM 1.5G at 100 mW/cm2. Upon using 1% N-methyl pyrrolidone (NMP) as a solvent additive in the toluene solvent, the PCE of the PSCs was greatly improved to 6.6% with a higher Jsc of 10.3 mA/cm2 and a high FF of 75%, which is even higher than that of the devices fabricated with halogenated DCB solvent. The X-ray diffraction (XRD) measurement shows that the crystallinity of P3HT increased with the NMP additive. The investigations on morphology of the active layers by atomic force microscopy (AFM) and transmission electron microscopy (TEM) indicate that the NMP additive promotes effective phase separation and formation of nanoscaled interpenetrating network structure of the active layer, which is beneficial to the improvement of Jsc and PCE for the PSCs fabricated with toluene as the solvent.Keywords: indene−C60 bisadduct; N-methyl pyrrolidone additive; non-halogenated solvents; polymer solar cells; toluene solvent;

Small molecules with narrow bandgap of <1.6 eV can harvest the visible and near-infrared solar photons. In this Article, we report a new method to achieve narrow bandgap small molecule donors by using electron-deficient quinoidal methyl-dioxocyano-pyridine (MDP) to induce possible quinoidal resonance structure along the conjugated A−π–D−π–A backbone. Practically, two MDP moieties are covalently linked onto an electron-rich benzodithiophene (BDT) through the oligothiophene (0T–5T) π-bridge. The affording small molecules, namely, nTBM, exhibit broad and strong absorption bands covering the visible and near-infrared region from 400 to 870 nm. The estimated optical bandgap is down to 1.4 eV. The narrow bandgap is associated with the low-lying lowest unoccupied molecular orbital (LUMO) energy level (about −3.7 eV) and the high-lying highest occupied molecular orbital (HOMO) energy level (around −5.1 eV). Density-functional theory calculations reveal that the HOMO and LUMO energy levels, with the increase of the size of the oligothiophene bridge, become localizations in different moieties, i.e., the central electron-donating and the terminal electron-withdrawing units, respectively, which provides necessary driving force for the delocalization of the excited electrons and formation of the quinoidal resonance structure. The quinoidal structure enhances the photoinduced intramolecular charge-transfer, leading to the absorbance enhancement of the low-energy absorption band. With the increase of the size of the oligothiophene from 0 to 5 thienyl units and the change of the direction of the alkyl chains on the bridged thiophene from “outward” to “inward”, the crystalline nature, fibril length, and phase size of the blend films as well as the cell performance are all fine-tuned, also. With the “inward” alkyl chains, the terthiophene bridged molecule is amorphous, while the pentathiophene bridged one is relatively crystalline. Both molecules form nanoscale interpenetrating networks with a phase size of 15–20 nm when blended with PC71BM, showing the higher hole mobility and promising electric performance.

Small molecules with narrow bandgap of <1.6 eV can harvest the visible and near-infrared solar photons. In this Article, we report a new method to achieve narrow bandgap small molecule donors by using electron-deficient quinoidal methyl-dioxocyano-pyridine (MDP) to induce possible quinoidal resonance structure along the conjugated A−π–D−π–A backbone. Practically, two MDP moieties are covalently linked onto an electron-rich benzodithiophene (BDT) through the oligothiophene (0T–5T) π-bridge. The affording small molecules, namely, nTBM, exhibit broad and strong absorption bands covering the visible and near-infrared region from 400 to 870 nm. The estimated optical bandgap is down to 1.4 eV. The narrow bandgap is associated with the low-lying lowest unoccupied molecular orbital (LUMO) energy level (about −3.7 eV) and the high-lying highest occupied molecular orbital (HOMO) energy level (around −5.1 eV). Density-functional theory calculations reveal that the HOMO and LUMO energy levels, with the increase of the size of the oligothiophene bridge, become localizations in different moieties, i.e., the central electron-donating and the terminal electron-withdrawing units, respectively, which provides necessary driving force for the delocalization of the excited electrons and formation of the quinoidal resonance structure. The quinoidal structure enhances the photoinduced intramolecular charge-transfer, leading to the absorbance enhancement of the low-energy absorption band. With the increase of the size of the oligothiophene from 0 to 5 thienyl units and the change of the direction of the alkyl chains on the bridged thiophene from “outward” to “inward”, the crystalline nature, fibril length, and phase size of the blend films as well as the cell performance are all fine-tuned, also. With the “inward” alkyl chains, the terthiophene bridged molecule is amorphous, while the pentathiophene bridged one is relatively crystalline. Both molecules form nanoscale interpenetrating networks with a phase size of 15–20 nm when blended with PC71BM, showing the higher hole mobility and promising electric performance.

Carrier mobility is a vital factor determining the electrical performance of organic solar cells. In this paper we report that a high-efficiency nonfullerene organic solar cell (NF-OSC) with a power conversion efficiency of 6.94 ± 0.27% was obtained by optimizing the hole and electron transportations via following judicious selection of polymer donor and engineering of film-morphology and cathode interlayers: (1) a combination of solvent annealing and solvent vapor annealing optimizes the film morphology and hence both hole and electron mobilities, leading to a trade-off of fill factor and short-circuit current density (Jsc); (2) the judicious selection of polymer donor affords a higher hole and electron mobility, giving a higher Jsc; and (3) engineering the cathode interlayer affords a higher electron mobility, which leads to a significant increase in electrical current generation and ultimately the power conversion efficiency (PCE).