Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells. Nature Materials.
while fullerene-based OSCs are only 10% efficient. [13] To achieve this milestone, various design strategies have been explored, for example, modification/manipulation of the Y6 acceptor side chain design, [7] the use of ternary mixtures with a vertical phase distribution, [9] the chemical modification via chlorination [8] or a variation of a fused-ring acceptor block of the donor polymer. [10] Currently, NFAs match their inorganic counterparts in terms of current generation, but are lacking with regard to their open-circuit voltage. [14] Efficiency losses can be traced back to energy losses during the photon to free charge conversion, and are in generally lower than in the fullerene-based cells. [15][16][17] Free charge generation in organic solar cells is comprised of two steps. During the first step, a photogenerated exciton dissociates at the donor-acceptor interface into an interfacial charge transfer (CT) state. During this process, the ionization energy or electron affinity offset at the heterojunction provides the driving force for the hole or electron transfer. It is known that this offset should exceed a threshold value in order to enable efficient dissociation of the excited state. [18][19][20] For NFAs, only ionization energy offsets are relevant, because of the fast energy transfer from donors to acceptors. [20] During the second step of charge separation, the interfacial CT state dissociates into a pair of free charges, or the charge separated (CS) state. This dissociation is expected to be an endothermic process, and the exact mechanism behind the driving force for this process is still under debate. [21][22][23][24][25][26] It is, however, one of the key processes in OSCs, since the energetics and dynamics of the dissociating CT state determines the open circuit voltage of organic heterojunctions. [25,[27][28][29] Both steps involved in the free charge generation can be optimized by an appropriate design of the donor-acceptor pair. The main difficulty in formulating generic chemical design rules for OSC materials is that any changes to the chemical structure simultaneously modify the open-circuit voltage, V oc , the short-circuit current, J sc , and the fill factor of the solar cell. [30][31][32][33][34][35] Without knowing how these changes correlate with each other, it is impossible to formulate clear design rules and hence speed up the discovery of efficient donor-acceptor combinations.In this work, we identify the microscopic origin of such correlations and propose clear chemical design rules for NFAs. Efficiencies of organic solar cells have practicallydoubled since the development of non-fullerene acceptors (NFAs). However, generic chemical design rules for donor-NFA combinations are still needed. Such rules are proposed by analyzing inhomogeneous electrostatic fields at the donor-acceptor interface. It is shown that an acceptor-donor-acceptor molecular architecture, and molecular alignment parallel to the interface, results in energy level bending that destabilizes the charge transfer state...
Looking beyond energy harvesting, metal-halide perovskites offer great opportunities to revolutionise large-area photodetection technologies due to their high absorption coefficients, long diffusion lengths, low trap densities and simple processability. However, successful extraction of photocarriers from perovskites and their conversion to electrical signals remain challenging due to the interdependency of photogain and dark current density. Here we report hybrid hetero-phototransistors by integrating perovskites with organic semiconductor transistor channels to form either “straddling-gap” type-I or “staggered-gap” type-II heterojunctions. Our results show that gradual transforming from type-II to type-I heterojunctions leads to increasing and tuneable photoresponsivity with high photogain. Importantly, with a preferential edge-on molecular orientation, the type-I heterostructure results in efficient photocarrier cycling through the channel. Additionally, we propose the use of a photo-inverter circuitry to assess the phototransistors’ functionality and amplification. Our study provides important insights into photocarrier dynamics and can help realise advanced device designs with “on-demand” optoelectronic properties.
Organic solar cells incorporating non-fullerene acceptors (NFAs) have reached remarkable power conversion efficiencies of over 18%. Unlike fullerene derivatives, NFAs tend to crystallize from solutions, resulting in bulk heterojunctions that include a crystalline acceptor phase. This must be considered in any morphology-function models. Here, it is confirmed that high-performing solution-processed indacenodithienothiophene-based NFAs, i.e., ITIC and its derivatives ITIC-M, ITIC-2F, and ITIC-Th, exhibit at least two crystalline forms. In addition to highly ordered polymorphs that form at high temperatures, NFAs arrange into a low-temperature metastable phase that is readily promoted via solution processing and leads to the highest device efficiencies. Intriguingly, the low-temperature forms seem to feature a continuous network that favors charge transport despite of a poorly order along the π-π stacking direction. As the optical absorption of the structurally more disordered low-temperature phase can surpass that of the more ordered polymorphs while displaying comparable-or even higher-charge transport properties, it is argued that such a packing structure is an important feature for reaching highest device efficiencies, thus, providing guidelines for future materials design and crystal engineering activities.
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