Abstract
All-polymer solar cells (all-PSCs) based on polymerized small molecular acceptors (PSMAs) have made significant progress recently. Here, we synthesize two A-DA’D-A small molecule acceptor ...based PSMAs of PS-Se with benzoc1,2,5thiadiazole A’-core and PN-Se with benzotriazole A’-core, for the studies of the effect of molecular structure on the photovoltaic performance of the PSMAs. The two PSMAs possess broad absorption with PN-Se showing more red-shifted absorption than PS-Se and suitable electronic energy levels for the application as polymer acceptors in the all-PSCs with PBDB-T as polymer donor. Cryogenic transmission electron microscopy visualizes the aggregation behavior of the PBDB-T donor and the PSMA in their solutions. In addition, a bicontinuous-interpenetrating network in the PBDB-T:PN-Se blend film with aggregation size of 10~20 nm is clearly observed by the photoinduced force microscopy. The desirable morphology of the PBDB-T:PN-Se active layer leads its all-PSC showing higher power conversion efficiency of 16.16%.
Tandem organic solar cells are based on the device structure monolithically connecting two solar cells to broaden overall absorption spectrum and utilize the photon energy more efficiently. Herein, ...we demonstrate a simple strategy of inserting a double bond between the central core and end groups of the small molecule acceptor Y6 to extend its conjugation length and absorption range. As a result, a new narrow bandgap acceptor BTPV-4F was synthesized with an optical bandgap of 1.21 eV. The single-junction devices based on BTPV-4F as acceptor achieved a power conversion efficiency of over 13.4% with a high short-circuit current density of 28.9 mA cm
. With adopting BTPV-4F as the rear cell acceptor material, the resulting tandem devices reached a high power conversion efficiency of over 16.4% with good photostability. The results indicate that BTPV-4F is an efficient infrared-absorbing narrow bandgap acceptor and has great potential to be applied into tandem organic solar cells.
Demonstrated in this work is a simple random ternary copolymerization strategy to synthesize a series of polymer acceptors, PTPBT‐ETx, by polymerizing a small‐molecule acceptor unit modified from Y6 ...with a thiophene connecting unit and a controlled amount of an 3‐ethylesterthiophene (ET) unit. Compared to PTPBT of only Y6‐like units and thiophene units, PTPBT‐ETx (where x represents the molar ratio of the ET unit) with an incorporated ET unit in the ternary copolymers show up‐shifted LUMO energy levels, increased electron mobilities, and improved blend morphologies in the blend film with the polymer donor PBDB‐T. And the all‐polymer solar cell (all‐PSC) based on PBDB‐T:PTPBT‐ET0.3 achieved a high power conversion efficiency over 12.5 %. In addition, the PTPBT‐ET0.3‐based all‐PSC also exhibits long‐term photostability over 300 hours.
All‐polymer solar cells (all‐PSCs) are composed of polymer donors and acceptors, which hold potentially superior morphological stability and mechanical flexibility. In this work, a new random ternary copolymerization strategy was adopted to synthesize new polymer acceptors with high performance. The all‐PSCs based on the new polymer acceptor shows high power conversion efficiency of over 12.5 % and high photostability capable of withstanding long‐term illumination stress.
Reducing the energy loss of sub-cells is critical for high performance tandem organic solar cells, while it is limited by the severe non-radiative voltage loss via the formation of non-emissive ...triplet excitons. Herein, we develop an ultra-narrow bandgap acceptor BTPSeV-4F through replacement of terminal thiophene by selenophene in the central fused ring of BTPSV-4F, for constructing efficient tandem organic solar cells. The selenophene substitution further decrease the optical bandgap of BTPSV-4F to 1.17 eV and suppress the formation of triplet exciton in the BTPSV-4F-based devices. The organic solar cells with BTPSeV-4F as acceptor demonstrate a higher power conversion efficiency of 14.2% with a record high short-circuit current density of 30.1 mA cm
and low energy loss of 0.55 eV benefitted from the low non-radiative energy loss due to the suppression of triplet exciton formation. We also develop a high-performance medium bandgap acceptor O1-Br for front cells. By integrating the PM6:O1-Br based front cells with the PTB7-Th:BTPSeV-4F based rear cells, the tandem organic solar cell demonstrates a power conversion efficiency of 19%. The results indicate that the suppression of triplet excitons formation in the near-infrared-absorbing acceptor by molecular design is an effective way to improve the photovoltaic performance of the tandem organic solar cells.
To achieve semiconducting materials with high electron mobility in organic field‐effect transistors (OFETs), low‐lying energy levels (the highest occupied molecular orbital (HOMO) and the lowest ...unoccupied molecular orbital (LUMO)) and favorable molecular packing and ordering are two crucial factors. Here, it is reported that the incorporation of pyridine and selenophene into the backbone of a diketopyrrolopyrrole (DPP)‐based copolymer produces a high‐electron‐mobility semiconductor, PDPPy‐Se. Compared with analogous polymers based on other DPP derivatives and selenophene, PDPPy‐Se features a lower LUMO that can decrease the electron transfer barrier for more effective electron injection, and simultaneously a lower HOMO that, however, can increase the hole transfer barrier to suppress the hole injection. Combined with thermal annealing at 240 °C for thin film morphology optimization to achieve large‐scale crystallite domains with tight molecular packing for effective charge transport along the conducting channel, OFET devices fabricated with PDPPy‐Se exhibit an n‐type‐dominant performance with an electron mobility (μe) as high as 2.22 cm2 V−1 s−1 and a hole/electron mobility ratio (μh/μe) of 0.26. Overall, this study demonstrates a simple yet effective approach to boost the electron mobility in organic transistors by synergistic use of pyridine and selenophene in the backbone of a DPP‐based copolymer.
The synergistic use of pyridine and selenophene in a diketopyrrolopyrrole‐based copolymer helps obtain low frontier orbital energy levels, resulting in increased hole injection barrier and decreased electron injection barrier. Combined with favorable charge carrier transport in the polymer film, an n‐type‐dominant property in organic field‐effect transistors with a high electron mobility of 2.22 cm2 V−1 s−1 is achieved.
Recently, a random ternary copolymerization strategy has become a promising and efficient approach to develop high‐performance polymer donors for polymer solar cells (PSCs). In this study, a low‐cost ...electron‐withdrawing unit, 2,5‐bis(4‐(2‐ethylhexyl)thiophen‐2‐yl)pyrazine (PZ‐T), is incorporated into the polymer backbone of PM6 as the third component, and three D‐A1‐D‐A2 type terpolymers PMZ‐10, PMZ‐20, and PMZ‐30 are synthesized by the random copolymerization strategy, with the PZ‐T proportion of 10%, 20%, and 30%, respectively. The terpolymers exhibit downshifted highest occupied molecular orbital energy levels than PM6, which is beneficial for obtaining higher open‐circuit voltage (Voc) of the PSCs with the polymer as a donor. Importantly, the PSCs based on PMZ‐10:Y6 demonstrate efficient exciton dissociation, higher and balanced electron/hole mobilities, desirable aggregation, and high power conversion efficiency of 18.23%, which is the highest efficiency among the terpolymer‐based PSCs so far. The results indicate that the ternary copolymerization strategy with PZ‐T as the second A‐unit is an efficient approach to further improve the photovoltaic performance and reduce the synthetic cost of the D‐A copolymer donors.
An electron‐withdrawing PZ‐T unit is employed to incorporate into the PM6 polymer backbone as the third component, and a series of high‐performance D‐A1‐D‐A2 type terpolymers are synthesized by random copolymerization strategy. Among them, the PMZ‐10:Y6‐based polymer solar cells (PSCs) achieved an outstanding power conversion efficiency of 18.23%, which is the highest reported performance among the terpolymer‐based PSCs so far.
Demonstrated in this work is a simple random ternary copolymerization strategy to synthesize a series of polymer acceptors, PTPBT‐ETx, by polymerizing a small‐molecule acceptor unit modified from Y6 ...with a thiophene connecting unit and a controlled amount of an 3‐ethylesterthiophene (ET) unit. Compared to PTPBT of only Y6‐like units and thiophene units, PTPBT‐ETx (where x represents the molar ratio of the ET unit) with an incorporated ET unit in the ternary copolymers show up‐shifted LUMO energy levels, increased electron mobilities, and improved blend morphologies in the blend film with the polymer donor PBDB‐T. And the all‐polymer solar cell (all‐PSC) based on PBDB‐T:PTPBT‐ET0.3 achieved a high power conversion efficiency over 12.5 %. In addition, the PTPBT‐ET0.3‐based all‐PSC also exhibits long‐term photostability over 300 hours.
All‐polymer solar cells (all‐PSCs) are composed of polymer donors and acceptors, which hold potentially superior morphological stability and mechanical flexibility. In this work, a new random ternary copolymerization strategy was adopted to synthesize new polymer acceptors with high performance. The all‐PSCs based on the new polymer acceptor shows high power conversion efficiency of over 12.5 % and high photostability capable of withstanding long‐term illumination stress.
As the power conversion efficiency of organic photovoltaic has been dramatically improved to over 18%, achieving long-term stability is now crucial for applications of this promising photovoltaic ...technology. Among the high-efficiency systems, most are using BTP-4F and its analogs as acceptors. Herein, we determine the thermal transition temperatures (Tg) of seven BTP analogs to develop a structure-Tg framework. Our results point out an unresolved molecular design conundrum on how to simultaneously achieve high performance and intrinsic stability with BTP-based acceptors. We also show that PC71BM has miscibility above the percolation threshold in PM6 and can maintain local charge percolation and improved stability in ternary devices. However, PC71BM is not miscible with BTP-C3-4F and unfavorable vertical gradients that develop during aging still degrade performance. This points to a second thermodynamic conundrum. A compound with differential miscibility in the donor polymer can only impact percolation, and a compound with differential miscibility with the BTP only impacts diffusion.
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•BTP-based OSCs (including BTP-4F) are intrinsically unstable or have low performance•Molecular designs that yield materials with high Tg are needed to get long-term stability•Additives in ink formulations that reduce the mobility of BTP-based NFAs are required
Organic solar cells (OSCs) have attracted considerable attention for their promise of large-scale processing. Particularly, OSCs based on non-fullerene acceptors have enjoyed significant attention due to dramatically improving efficiency, however, long-term stability is crucial and, therefore, becomes an imperative research goal in the field. Here, we determine the Tg of seven BTP-based non-fullerene acceptors. Using the Gordon-Tayler relations, we have developed a structure-Tg framework that can disentangle the contribution to Tg of the outer and inner sidechains, as well as the two different cores. We also show that PC71BM has miscibility above the percolation threshold in PM6 and can, thus, maintain local charge percolation. However, PC71BM is not miscible with BTP-C3-4F and unfavorable vertical gradients that still degrades performance. A high Tg component with suitable electronic structures that prevents BTP diffusion would be required to achieve commercial viability.
We determine the thermal transition temperatures (Tg) of seven BTP-based non-fullerene acceptors and have developed a structure-Tg framework. We also show that PC71BM has a miscibility above the percolation threshold in PM6 and thus can maintain local charge percolation. However, PC71BM is not miscible with BTP-C3-4F and can, thus, not prevent BTP-C3-4F diffusion, and the unfavorable vertical gradients that still degrades performance, a high Tg component with suitable electronic structures that prevent BTP diffusion would be required to achieve commercial viability.
All‐polymer solar cells (all‐PSCs) have drawn growing attention and achieved tremendous progress recently, but their power conversion efficiency (PCE) still lags behind small‐molecule‐acceptor ...(SMA)‐based PSCs due to the relative difficulty on morphology control of polymer photoactive blends. Here, low‐cost PTQ10 is introduced as a second polymer donor (a third component) into the PM6:PY‐IT blend to finely tune the energy‐level matching and microscopic morphology of the polymer blend photoactive layer. The addition of PTQ10 decreases the π–π stacking distance, and increases the π–π stacking coherence length and the ordered face‐on molecular packing orientation, which improves the charge separation and transport in the photoactive layer. Moreover, the deeper highest occupied molecular orbital energy level of the PTQ10 polymer donor than PM6 leads to higher open‐circuit voltage of the ternary all‐PSCs. As a result, a PCE of 16.52% is achieved for ternary all‐PSCs, which is one of the highest PCEs for all‐PSCs. In addition, the ternary devices exhibit a high tolerance of the photoactive layer thickness with high PCEs of 15.27% and 13.91% at photoactive layer thickness of ≈205 and ≈306 nm, respectively, which are the highest PCEs so far for all‐PSCs with a thick photoactive layer.
A 16.52% efficiency all‐polymer solar cell is achieved by morphology control of the photoactive layer through adding a low‐cost polymer donor, PTQ10, into the PM6:PY‐IT blend. Meanwhile, ternary devices exhibit a high tolerance of the photoactive layer thickness, with high power conversion efficiencies of 15.27% and 13.91% at photoactive layer thicknesses of ≈205 and ≈306 nm, respectively.
Two medium‐bandgap p‐type organic small molecules H21 and H22 with an alkylsily‐thienyl conjugated side chain on benzo1,2‐b:4,5‐b′dithiophene central units are synthesized and used as donors in ...all‐small‐molecule organic solar cells (SM‐OSCs) with a narrow‐bandgap n‐type small molecule 2,2′‐((2Z,2′Z)‐((4,4,9,9‐tetrahexyl‐4,9‐dihydro‐s‐indaceno1,2‐b:5,6‐b′dithiophene‐2,7‐diyl)bis(methanylylidene))bis(3‐oxo‐2,3‐dihydro‐1H‐indene‐2,1‐diylidene))dimalononitrile (IDIC) as the acceptor. In comparison to H21 with 3‐ethyl rhodanine as the terminal group, H22 with cyanoacetic acid esters as the terminal group shows blueshifted absorption, higher charge‐carrier mobility and better 3D charge pathway in blend films. The power conversion efficiency (PCE) of the SM‐OSCs based on H22:IDIC reaches 10.29% with a higher open‐circuit voltage of 0.942 V and a higher fill factor of 71.15%. The PCE of 10.29% is among the top efficiencies of nonfullerene SM‐OSCs reported in the literature to date.
High‐efficiency (10.29%) all‐small‐molecule organic solar cells are demonstrated based on an acceptor–donor–acceptor‐structured 2D conjugated organic molecule with an alkylsilyl‐thienyl conjugated side chain and cyanoacetic acid ester terminal groups as the donor and a narrow‐bandgap n‐type organic semiconductor, IDIC, as the acceptor.