Interfacial engineering for the regulation of the charge carrier dynamics in solar cells is a critical factor in the fabrication of high-efficiency devices.Based on the successful preparation of highly dispersible gra...Interfacial engineering for the regulation of the charge carrier dynamics in solar cells is a critical factor in the fabrication of high-efficiency devices.Based on the successful preparation of highly dispersible graphdiyne oxide(GDYO)with a large number of functional groups,we fabricated organic solar cells employing GDYO-modified poly(3,4-ethylenedioxythiophene)/poly(styrene sulfonate)(PEDOT:PSS)as hole transport materials.Results show that theπ±πinteraction between GDYO and PEDOT:PSS is beneficial to the formation of an optimized charge carrier transfer channel and improves the conductivity and charge carrier mobility in the hole transport layer.Moreover,the improved interfacial contact contributes to the suppression of charge carrier recombination and the elevation of charge carrier extraction between the hole transport layer and the active layer.More importantly,the occurrence of charge carrier separation benefits from the optimized morphology of the active layer,which efficiently improves the performance,as proven by the results of transient absorption measurements.Therefore,with the holistic management approach to the multiobjective optimization of the charge carrier dynamics,a photoelectric conversion efficiency of 17.5%(with the certified value of 17.2%)is obtained for binary organic solar cells.All of these results indicate the potential application of the functionalized graphdiyne in the field of organic optoelectronic devices.展开更多
Two new conjugated copolymers, PBDT-T6-TTF and PBDT-T12-TTF, were derived from a novel 4-fluorobenzoyl thienothi- ophene （TTF）. In addition, two types of benzodithiophene （BDT） units with 2,3-dihexylthienyl （T6）...Two new conjugated copolymers, PBDT-T6-TTF and PBDT-T12-TTF, were derived from a novel 4-fluorobenzoyl thienothi- ophene （TTF）. In addition, two types of benzodithiophene （BDT） units with 2,3-dihexylthienyl （T6） and 2,3-didodecylthienyl （T12） substituents, respectively, were successfully synthesized. The effect of the dual two-dimensional （2D） substitutions of the building blocks upon the optoelectronic properties of the polymers was investigated. Generally, the two polymers exhibited good solubility and broad absorption, showing similar optical band gaps of ~1.53 eV. However, PBDT-T6-TTF with its shorter alkyl chain length possessed a larger extinction coefficient in thin solid film. The highest occupied molecular orbital （HOMO） level of PBDT-T6-TTF was located at -5.38 eV while that of PBDT-T12-TTF was at -5.51 eV. In space charge-limited- current （SCLC） measurement, PBDT-T6-TTF and PBDT-T12-TTF displayed respective hole mobilities of 3.0~10-~ and 1.6x10 5 cm2 V-1 s-l. In polymer solar cells, PBDT-T6-TTF and PBDT-T12-TTF showed respective power conversion efficiencies （PCEs） of 2.86% and 1.67%. When 1,8-diiodooctane （DIO） was used as the solvent additive, the PCE of PBDT-T6-TTF was remarkably elevated to 4.85%, but the use of DIO for the PBDT-T12-TTF-blend film resulted in a lower PCE of 0.91%. Atomic force microscopy （AFM） indicated that the superior efficiency of PBDT-T6-TTF with 3% DIO （v/v） should be related to the better continuous phase separation of the blend film. Nevertheless, the morphology of the PBDT-T12-TTF deteriorated when the 3% DIO （v/v） was added. Our results suggest that the alkyl-chain length on the 2D BDT units play an important role in determining the optoelectronic properties of dual 2D BDT-TT-based polymers.展开更多
基金supported by the National Natural Science Foundation of China(21975273,21801014,21773012,and U2032112)Shandong Provincial Natural Science Foundation(ZR2021QE191)+3 种基金the Scientific Research Starting Foundation of Outstanding Young Scholar of Shandong Universitythe Future Young Scholars Program of Shandong Universitythe Fundamental Research Funds of Shandong Universitysupported by the Analysis&Testing Center of Beijing Institute of Technology。
文摘Interfacial engineering for the regulation of the charge carrier dynamics in solar cells is a critical factor in the fabrication of high-efficiency devices.Based on the successful preparation of highly dispersible graphdiyne oxide(GDYO)with a large number of functional groups,we fabricated organic solar cells employing GDYO-modified poly(3,4-ethylenedioxythiophene)/poly(styrene sulfonate)(PEDOT:PSS)as hole transport materials.Results show that theπ±πinteraction between GDYO and PEDOT:PSS is beneficial to the formation of an optimized charge carrier transfer channel and improves the conductivity and charge carrier mobility in the hole transport layer.Moreover,the improved interfacial contact contributes to the suppression of charge carrier recombination and the elevation of charge carrier extraction between the hole transport layer and the active layer.More importantly,the occurrence of charge carrier separation benefits from the optimized morphology of the active layer,which efficiently improves the performance,as proven by the results of transient absorption measurements.Therefore,with the holistic management approach to the multiobjective optimization of the charge carrier dynamics,a photoelectric conversion efficiency of 17.5%(with the certified value of 17.2%)is obtained for binary organic solar cells.All of these results indicate the potential application of the functionalized graphdiyne in the field of organic optoelectronic devices.
基金financially supported by the National Natural Science Foundation of China(21225418 and 51173048)the National Basic Research Program of China(2013CB834705 and 2014CB643505)GDUPS(2013)
文摘Two new conjugated copolymers, PBDT-T6-TTF and PBDT-T12-TTF, were derived from a novel 4-fluorobenzoyl thienothi- ophene （TTF）. In addition, two types of benzodithiophene （BDT） units with 2,3-dihexylthienyl （T6） and 2,3-didodecylthienyl （T12） substituents, respectively, were successfully synthesized. The effect of the dual two-dimensional （2D） substitutions of the building blocks upon the optoelectronic properties of the polymers was investigated. Generally, the two polymers exhibited good solubility and broad absorption, showing similar optical band gaps of ~1.53 eV. However, PBDT-T6-TTF with its shorter alkyl chain length possessed a larger extinction coefficient in thin solid film. The highest occupied molecular orbital （HOMO） level of PBDT-T6-TTF was located at -5.38 eV while that of PBDT-T12-TTF was at -5.51 eV. In space charge-limited- current （SCLC） measurement, PBDT-T6-TTF and PBDT-T12-TTF displayed respective hole mobilities of 3.0~10-~ and 1.6x10 5 cm2 V-1 s-l. In polymer solar cells, PBDT-T6-TTF and PBDT-T12-TTF showed respective power conversion efficiencies （PCEs） of 2.86% and 1.67%. When 1,8-diiodooctane （DIO） was used as the solvent additive, the PCE of PBDT-T6-TTF was remarkably elevated to 4.85%, but the use of DIO for the PBDT-T12-TTF-blend film resulted in a lower PCE of 0.91%. Atomic force microscopy （AFM） indicated that the superior efficiency of PBDT-T6-TTF with 3% DIO （v/v） should be related to the better continuous phase separation of the blend film. Nevertheless, the morphology of the PBDT-T12-TTF deteriorated when the 3% DIO （v/v） was added. Our results suggest that the alkyl-chain length on the 2D BDT units play an important role in determining the optoelectronic properties of dual 2D BDT-TT-based polymers.
