In this contribution, a facile and universal method is successfully reported to fabricate perovskite solar cells (PSCs) with enhanced efficiency and stability. Through dissolving functional conjugated polymers in antisolvent chlorobenzene to treat the spinning CH 3 NH 3 PbI 3 perovskite film, the resultant devices exhibit significantly enhanced efficiency and longevity simultaneously. In-depth characterizations demonstrate that thin polymer layer well covers the top surface of perovskite film, resulting in certain surface passivation and morphology modification. More importantly, it is shown that through rational chemical modification, namely molecular fluorination, the air stability and photostability of the perovskite solar cells are remarkably enhanced. Considering the vast selection of conjugated polymer materials and easy functional design, promising new results are expected in further enhancement of device performance. It is believed that the findings provide exciting insights into the role of conjugated polymer in improving the current perovskite-based solar cells.
Molecular design enabled reduction of interface trap density affords Molecular design enabled reduction of interface trap density affords highly efficient and stable perovskite solar cells with over 83% fill highly efficient and stable perovskite solar cells with over 83% fill factor factor
Tuning the donor–acceptor (D–A) weight ratio is an essential step to optimize the performance of a bulk heterojunction (BHJ) solar cell. The unoptimized regime with a low acceptor concentration is generally unexplored despite it may reveal the early stage electronic D–A interactions. In this study, PTB7:PC71BM is used to examine factors that limit the device performance in unoptimized regime. The key limiting factor is the creation of traps and localized states originated from fullerene molecules. Photothermal deflection spectroscopy is used to quantify the trap density. Starting with pristine PTB7, addition of small concentration of fullerene increases the electron trap density and lowers the electron mobility. When the D–A weight ratio reaches 1:0.1, fullerene percolation occurs. There is an abrupt drop in trap density and simultaneously a six orders of magnitude increase in the electron mobility. Furthermore, the fill factors of the corresponding photovoltaic devices are found to anticorrelate with the trap density. This study reveals that electron trapping is the key limiting factor for unoptimized BHJ solar cells in low fullerene regime.
The light soaking effect (LSE) is widely known in perovskite solar cells (PVSCs), but its origin is still elusive. In this study, we show that in common with hysteresis, the LSE is owed to the ion migration in PVSCs. Driven by the photovoltage, the mobile ions in the perovskite materials (MA/I) migrate to the selective contacts, forming a boosted P-i-N junction resulting in enhanced charge separation. Besides, the mobile ions (MA) can soften and suture the PCBM/perovskite interface and thus reduce the trap density, in keeping with a higher open-circuit voltage. Finally, almost LSE-free PVSCs can be prepared by using 0.1 wt % MAI-doped PCBM as the electron transport material, whereas overdoping (1 wt % MAI doping) makes the LSE even more pronounced due to excess mobile ions that need time to migrate to reach a new quasi-static state.
Despite the rapid development of nonfullerene acceptors (NFAs), the fundamental understanding on the relationship between NFA molecular architecture, morphology, and device performance is still lacking. Herein, poly[[4,8-bis[5-(2-ethylhexyl)thiophene-2-yl]benzo[1,2-b:4,5-b0]dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]-thieno[3,4-b]thiophenediyl]](PTB7-Th) is used as the donor polymer to compare an NFA with a 3D architecture (SF-PDI4) to a well-studied NFA with a linear acceptor-donoracceptor (A-D-A) architecture (ITIC). The data suggest that the NFA ITIC with a linear molecular structure shows a better device performance due to an increase in short-circuit current ( J sc ) and fill factor (FF) compared to the 3D SF-PDI4. The charge generation dynamics measured by femtosecond transient absorption spectroscopy (TAS) reveals that the exciton dissociation process in the PTB7-Th:ITIC films is highly efficient. In addition, the PTB7-Th:ITIC blend shows a higher electron mobility and lower energetic disorder compared to the PTB7-Th:SF-PDI4 blend, leading to higher values of J sc and FF. The compositional sensitive resonant soft X-ray scattering (R-SoXS) results indicate that ITIC molecules form more pure domains with reduced domain spacing, resulting in more efficient charge transport compared with the SF-PDI4 blend. It is proposed that both the molecular structure and the corresponding morphology of ITIC play a vital role for the good solar cell device performance.
To better understand the correlation of the dielectric properties with the photovoltaic response in conjugated polymer:fullerene bulk heterojunction materials, the concept of introducing minimal structural change is employed to increase the polymer dielectric constant via polar cyano groups added to the end of butyl or octyl side chains in the poly(dithienosilole-thienopyrrolodione) system. Density functional theory calculations confirm that the polar groups do not affect the polymer electronic structure but can lead to an increase in overall dipole moment depending on the polymer chain conformation. Despite the increased dielectric constant (from 2.7 to 4.3 for cyano-octyl side chains and from 2.7 to 3.2 for the cyano-butyl analogues), the device characteristics employing the cyano-containing polymers are inferior to those of the devices made with unfunctionalized alkyl chains. It is found that the hole mobilities for the cyano-containing polymers are two orders of magnitude lower compared to those for the parent polymers and suggest this is due to an increase in energetic disorder caused by the strong local permanent dipoles associated with the cyano groups. The study highlights the complexity in the relationship between the dielectric constant of organic materials, the morphologies that are induced, and their photovoltaic performance.
Understanding the correlation between polymer aggregation, miscibility, and device performance is important to establish a set of chemistry design rules for donor polymers with nonfullerene acceptors (NFAs). Employing a donor polymer with strong temperature‐dependent aggregation, namely PffBT4T‐2OD [poly[(5,6‐difluoro‐2,1,3‐benzothiadiazol‐4,7‐diyl)‐alt‐(3,3″′‐di(2‐octyldodecyl)‐2,2′;5′,2″;5″,2″′‐quaterthiophen‐5,5‐diyl)], also known as PCE‐11 as a base polymer, five copolymer derivatives having a different thiophene linker composition are blended with the common NFA O‐IDTBR to investigate their photovoltaic performance. While the donor polymers have similar optoelectronic properties, it is found that the device power conversion efficiency changes drastically from 1.8% to 8.7% as a function of thiophene content in the donor polymer. Results of structural characterization show that polymer aggregation and miscibility with O‐IDTBR are a strong function of the chemical composition, leading to different donor–acceptor blend morphology. Polymers having a strong tendency to aggregate are found to undergo fast aggregation prior to liquid–liquid phase separation and have a higher miscibility with NFA. These properties result in smaller mixed donor–acceptor domains, stronger PL quenching, and more efficient exciton dissociation in the resulting cells. This work indicates the importance of both polymer aggregation and donor–acceptor interaction on the formation of bulk heterojunctions in polymer:NFA blends.
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