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All-polymer solar cells (all-PSCs) offer improved morphological and mechanical stability compared with those containing small-molecule-acceptors (SMAs). They can be processed with a broader range of conditions, making them desirable for printing techniques. In this study, we report a high-performance polymer acceptor design based on bithiazole linker (PY-BTz) that are on par with SMAs. We demonstrate that bithiazole induces a more coplanar and ordered conformation compared to bithiophene due to the synergistic effect of non-covalent backbone planarization and reduced steric encumbrances. As a result, PY-BTz shows a significantly higher efficiency of 16.4% in comparison to the polymer acceptors based on commonly used thiophene-based linkers (i.e., PY-2T, 9.8%). Detailed analyses reveal that this improvement is associated with enhanced conjugation along the backbone and closer interchain π-stacking, resulting in higher charge mobilities, suppressed charge recombination, and reduced energetic disorder. Remarkably, an efficiency of 14.7% is realized for all-PSCs that are solution-sheared in ambient conditions, which is among the highest for devices prepared under conditions relevant to scalable printing techniques. This work uncovers a strategy for promoting backbone conjugation and planarization in emerging polymer acceptors that can lead to superior all-PSCs. All-polymer solar cells comprising both polymeric donors and acceptors offer better morphological and mechanical stability, and a broader processing window for printing. Here, the authors report a polymer acceptor based on bithiazole linker with more coplanar and ordered molecular conformation. [ABSTRACT FROM AUTHOR]

Performance of nonfullerene‐based organic solar cells is largely dependent on the donor:acceptor blend morphology, which is initially tuned by composition. However, morphological design rules are difficult to identify due to the complex relationship between composition‐dependent phase behavior and performance properties. In this study, the authors are able to establish a direct link between PM6:Y6 film morphology and device properties by combining grazing‐incidence wide‐angle X‐ray scattering with highly sensitive Fourier transform photocurrent spectroscopy. By analyzing properties across the full composition range, interfacial microstructure and the corresponding charge transfer (CT) states are identified and direct structure–property relationships are established. The results indicate that open‐circuit voltage is controlled by the CT state at amorphous‐PM6:crystalline‐Y6 interfaces. Crystalline Y6 is found to increase both transport and non‐radiative recombination, suggesting that morphological tradeoffs may be necessary for overall device optimization. [ABSTRACT FROM AUTHOR]

Abstract: Poly (3‐hexylthiophene) (P3HT) was an early frontrunner in the development of donor polymers to be used in organic photovoltaics. A relatively straightforward and inexpensive synthesis suggests that it may be the most viable donor polymer to use in large‐scale commercial organic solar cells. Replacing fullerenes with new electron acceptors has led to significant improvements in device performance and stability, with devices now able to exceed an efficiency of 7%. Past studies have reported a dependence of device performance on the molecular weight of the polymer in fullerene‐containing blends, however, with nonfullerene acceptors now showing promise a similar study was needed. P3HT blends, with two nonfullerene acceptors (O‐IDTBR and EH‐IDTBR), were probed using a number of polymer batches with varying molecular weights. O‐IDTBR was shown to exhibit a dependence on the polymer molecular weight, with optimal performance achieved with a 34 kDa polymer, while EH‐IDTBR displayed an independence in performance with varying polymer molecular weight. Probing the thermal and morphological behavior of the P3HT:O‐IDTBR blends suggests that an optimal morphology with pronounced donor and acceptor domains was only achieved with the 34 kDa polymer, and a greater degree of mixing was exhibited in the other blends, likely leading to poorer device performance. [ABSTRACT FROM AUTHOR]

In organic solar cells (OSCs), the energy of the charge-transfer (CT) complexes at the donor-acceptor interface, ECT, determines the maximum open-circuit voltage ( VOC). The coexistence of phases with different degrees of order in the donor or the acceptor, as in blends of semi-crystalline donors and fullerenes in bulk heterojunction layers, influences the distribution of CT states and the VOC enormously. Yet, the question of how structural heterogeneities alter CT states and the VOC is seldom addressed systematically. In this work, we combine experimental measurements of vacuum-deposited rubrene/C60 bilayer OSCs, with varying microstructure and texture, with density functional theory calculations to determine how relative molecular orientations and extents of structural order influence ECT and VOC. We find that varying the microstructure of rubrene gives rise to CT bands with varying energies. The CT band that originates from crystalline rubrene lies up to ≈0.4 eV lower in energy compared to the one that arises from amorphous rubrene. These low-lying CT states contribute strongly to VOC losses and result mainly from hole delocalization in aggregated rubrene. This work points to the importance of realizing interfacial structural control that prevents the formation of low ECT configurations and maximizes VOC. [ABSTRACT FROM AUTHOR]

Organic ternary heterojunction photovoltaic blends are sometimes observed to undergo a gradual evolution in open-circuit voltage (Voc) with increasing amounts of a second donor or an acceptor. The Voc is strongly correlated with the energy of the charge transfer state in the blend, but this value depends on both local and mesoscopic orders. In this work, the behavior of Voc in the presence of a wide range of interfacial electronic states is investigated. The key charge transfer state interfaces responsible for Voc in several model systems with varying morphology are identified. Systems consisting of one donor with two fullerene molecules and of one acceptor with a donor polymer of varying regio-regularity are used. The effects from the changing energetic disorder in the material and from the variation due to a law of simple mixtures are quantified. It has been found that populating the higher-energy charge transfer states is not responsible for the observed change in Voc upon the addition of a third component. Aggregating polymers and miscible fullerenes are compared, and it has been concluded that in both cases charge delocalization, aggregation, and local polarization effects shift the lowestenergy charge transfer state distribution. [ABSTRACT FROM AUTHOR]

The conjugated polymer, poly(2,5-bis(3-hexadecylthiophen-2-yl)thieno[3,2-b]thiophene) (pBTTT-C16), allows a systematic tuning of the blend morphology by varying the acceptor type and fraction, making it a well-suited structural model for studying the fundamental processes in organic bulk heterojunction solar cells. To analyze the role of intercalated and pure fullerene domains on charge carrier photogeneration, time delayed collection field (TDCF) measurements and Fourier-transform photocurrent spectroscopy (FTPS) are performed on pBTTT-C16:[6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) solar cells with various stoichiometries. A weak influence of excess photon energy on photogeneration along with a photogeneration having a weaker field dependence at increasing fullerene loading is found. The findings are assigned to a dissociation via thermalized charge transfer (CT) states supported by an enhanced electron delocalization along spatially extended PC61BM nanophases that form in addition to a bimolecular crystal (BMC) for PC61BM rich blends. The highly efficient transfer of charge carriers from the BMC into the pure domains are studied further by TDCF measurements performed on non-intercalated pBTTT-C16:bisPC61BM blends. They reveal a field dependent charge generation similar to the 1:4 PC61BM blend, demonstrating that the presence of pure acceptor phases is the major driving force for an efficient, field independent CT dissociation. [ABSTRACT FROM AUTHOR]

Cost-effective, solution-processable organic photovoltaics (OPV) present an interesting alternative to inorganic silicon-based solar cells. However, one of the major remaining challenges of OPV devices is their lack of long-term operational stability, especially at elevated temperatures. The synthesis of a fullerene dumbbell and its use as an additive in the active layer of a PCDTBT:PCBM-based OPV device is reported. The addition of only 20 % of this novel fullerene not only leads to improved device efficiencies, but more importantly also to a dramatic increase in morphological stability under simulated operating conditions. Dynamic secondary ion mass spectrometry (DSIMS) and TEM are used, amongst other techniques, to elucidate the origins of the improved morphological stability. [ABSTRACT FROM AUTHOR]

New polymers with high electron mobilities have spurred research in organic solar cells using polymeric rather than fullerene acceptors due to their potential of increased diversity, stability, and scalability. However, all-polymer solar cells have struggled to keep up with the steadily increasing power conversion efficiency of polymer:fullerene cells. The lack of knowledge about the dominant recombination process as well as the missing concluding picture on the role of the semi-crystalline microstructure of conjugated polymers in the free charge carrier generation process impede a systematic optimization of all-polymer solar cells. These issues are examined by combining structural and photo-physical characterization on a series of poly(3-hexylthiophene) (donor) and P(NDI2OD-T2) (acceptor) blend devices. These experiments reveal that geminate recombination is the major loss channel for photo-excited charge carriers. Advanced X-ray and electron-based studies reveal the effect of chloronaphthalene co-solvent in reducing domain size, altering domain purity, and reorienting the acceptor polymer crystals to be coincident with those of the donor. This reorientation correlates well with the increased photocurrent from these devices. Thus, efficient split-up of geminate pairs at polymer/polymer interfaces may necessitate correlated donor/acceptor crystal orientation, which represents an additional requirement compared to the isotropic fullerene acceptors. [ABSTRACT FROM AUTHOR]

Polymer aggregation and phase separation of polymer–polymer blends are effectively tuned from self‐stratified to laterally phase‐separated by adjusting the relative solubility of the two polymers in the mixture. This is found to dramatically alter the charge transport characteristics from a preferential in‐plane to an out‐of‐plane direction, revealing the critical dependence of the resulting device performance on the film morphology and structure of the active layer. [ABSTRACT FROM AUTHOR]

Interfaces between organic electron-donating (D) and electron-accepting (A) materials have the ability to generate charge carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold via weakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer:fullerene, small-molecule:C60 and polymer:polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy. [ABSTRACT FROM AUTHOR]

Transparent top electrodes for solid-state dye-sensitized solar cells (ssDSCs) allow for fabrication of mechanically stacked ssDSC tandems, partially transparent ssDSCs for building integration, and ssDSCs on metal foil substrates. A solution-processed, highly transparent, conductive electrode based on PEDOT:PSS [poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)] and spray-deposited silver nanowires (Ag NWs) is developed as an effective top contact for ssDSCs. The electrode is solution-deposited using conditions and solvents that do not damage or dissolve the underlying ssDSC and achieves high performance: a peak transmittance of nearly 93% at a sheet resistance of 18 Ω/square - all without any annealing that would harm the ssDSC. The role of the PEDOT:PSS in the electrode is twofold: it ensures ohmic contact between the ssDSC 2,2′,7,7′-tetrakis-( N, N-di-p-methoxyphenylamine)9,9′-spirobifluorene (Spiro-OMeTAD) overlayer and the silver nanowires and it decreases the series resistance of the device. Semitransparent ssDSCs with D35 dye fabricated using this Ag NW/PEDOT:PSS transparent electrode show power conversion efficiencies of 3.6%, nearly as high as a reference device using an evaporated silver electrode (3.7%). In addition, the semitransparent ssDSC shows high transmission between 700-1100 nm, a necessity for use in efficient tandem devices. Such an electrode, in combination with efficient ssDSCs or hybrid perovskite-sensitized solar cells, can allow for the fabrication of efficient, cost-effective tandem photovoltaics. [ABSTRACT FROM AUTHOR]

The performance of polymer:fullerenesolar cells is strongly affectedby the active layer morphology and polymer microstructure. In thisPerspective, we review ongoing research on how structural factorsinfluence the photogeneration and collection of charge carriers aswell as charge carrier recombination and the related open-circuitvoltage. We aim to highlight unexplored research opportunities andprovide some guidelines for the synthesis of new conjugated polymersfor high-efficiency solar cells. [ABSTRACT FROM AUTHOR]

• A metal-oxide pyramid texture is converted into the non-resonant optical metasurfaces. • Metasurfaces are realized through the templated growth electrodeposition of nanowires. • A J SC gain of 10-25% is achieved as compared to the planar device. • Energy conversion efficiencies of perovskite/perovskite TSCs can reach over 30%. • Optics of solar cells is investigated by FDTD optical simulations. The short-circuit current density and energy conversion efficiency of single-junction perovskite and perovskite/perovskite tandem solar cells can be increased by photon management. In this study, optical metasurfaces were investigated as potential light trapping structures oppose to commonly used pyramidal surface textures. Herein, metal oxide-based non-resonant metasurfaces were investigated as potential light-trapping structures in perovskite solar cells. The zinc oxide nanowire-based building blocks of the metasurface can be prepared by a templated electrodeposition through a mask of resist. The phase of the incident light can be controlled by the edge length of the subwavelength large zinc oxide nanowires. An array of zinc oxide nanowires was prepared and characterized in the current study. Three-dimensional (3D) finite-difference time-domain (FDTD) optical simulations were used to compare solar cells covered with non-resonant metasurfaces with commonly used light trapping structures. As compared to the solar cells covered with zinc oxide pyramid surface texture, solar cells with the integrated non-resonant metasurfaces exhibit almost identical quantum efficiencies and short-circuit current densities. Investigations of such metasurfaces will not only improve the photon absorption in perovskite solar cells but also reveal a pathway to make high-efficiency next-generation solar cells. Detailed guidelines for the realization of non-resonant metal oxide metasurfaces will be provided. [ABSTRACT FROM AUTHOR]

Systematically moving the alkyl-chain branching position away from the polymer backbone afforded two new thieno[3,2-b]thiophene-diketopyrrolopyrrole (DPPTT-T) polymers. When used as donor materials in polymer:fullerene solar cells, efficiencies exceeding 7% were achieved without the use of processing additives. The effect of the position of the alkyl-chain branching point on the thin-film morphology was investigated using X-ray scattering techniques and the effects on the photovoltaic and charge-transport properties were also studied. For both solar cell and transistor devices, moving the branching point further from the backbone was beneficial. This is the first time that this effect has been shown to improve solar cell performance. Strong evidence is presented for changes in microstructure across the series, which is most likely the cause for the photocurrent enhancement. [ABSTRACT FROM AUTHOR]

Recent evidence has demonstrated that amorphous mixed phases are ubiquitous within mesostructured polythiophene-fullerene mixtures. Nevertheless, the role of mixing within nanophases on charge transport of organic semiconductor mixtures is not fully understood. To this end, we have examined the electron mobility in amorphous blends of poly(3-hexylthiophene) and phenyl-C61-butyric acid methyl ester. Our studies reveal that the miscibility of the components strongly affects electron transport within blends. Immiscibility promotes efficient electron transport by promoting percolating pathways within organic semiconductor mixtures. As a consequence, partial miscibility may be important for efficient charge transport in polythiophene-fullerene mixtures and organic solar cell performance. [ABSTRACT FROM AUTHOR]