Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells. Nature Materials.
Ternary organic solar cells based on polymer donor and nonfullerene acceptors (NFAs) are delivering high power conversion efficiencies (PCE). Now, further improvement needs to be directed to enhance the operational lifetime of organic photovoltaics. Here, we selected three NFAs with different electron affinities and structural properties and found that the most crystalline third component, O-IDTBR, is selectively miscible within the acceptor phase. This reduced trap-assisted recombination and delivered a PCE of 16.6% and a fill factor of 0.76, compared to PM6:Y6 binary devices (15.2% PCE). Charge transport and recombination analyses revealed that O-IDTBR acts as a charge relay for improved charge transfer of both donor and acceptor materials leading to a more ordered transport. We find that minimizing traps formation in ternary devices deactivates light-induced traps upon full sun illumination (AM1.5G). As a result, ternary devices do not show any PCE drop in 225h, in comparison to binary cells which lose more than 60% of their initial performances.
Thermoelectric (TE) generators that are capable of providing sustainable energy conversion under dynamic mechanical stresses have been explored for realizing autonomous wearable electronics. However, finding extremely deformable, efficient, and air-stable TE materials is still a major challenge. Here, we report highly stretchable and efficient organic TE materials from aqueous composites of poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) and ionic liquids (ILs). In this composite, ILs simultaneously enhance the Seebeck coefficient and electrical conductivity of PEDOT:PSS (up to 35 μV K–1 and 538 S cm–1, respectively) by controlling its oxidation level and nanostructure. Moreover, the resulting fibrous structure with IL-assisted soft domains leads to outstanding mechanical deformability and durability, enabling that the PEDOT:PSS/IL films simply coated on elastomeric substrates maintain the TE functionality under tensile strain (ε) up to 70% and repetitive stretching cycles with 30% ε without severe degradation in TE performance. Furthermore, we also demonstrate the long-term TE stability of PEDOT:PSS/IL composites maintaining >80% of the initial performance after 10 days under ambient conditions. Our finding proves the potential of this novel composite as a stretchable and air-stable organic TE material.
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...
Here, we show ternary organic solar cells with a power conversion efficiency of 14%. By a careful selection of a third component (BIT-4F-T), we obtain an enhancement of all photovoltaic parameters compared to the binary devices (PTB7-Th:IEICO-4F). This is because of a dual effect of the third component acting not only as sensitizer but also as a solid processing aid, which is beneficial for charge generation and transport.
Conjugated polymer semiconductors offer unique advantages over conventional semiconductors but tend to suffer from electro-optic performance roll-off, mainly due to reduced photofastness. Here, we demonstrate that the commodity nickel chelate nickel(II) dibutyldithiocarbamate, Ni(dtc) 2 , effectively inhibits photooxidation across a wide range of prototypical p-conjugated polymer semiconductors and blends. The addition of 2-10 wt% of Ni(dtc) 2 increases the resilience of otherwise quickly photobleaching semiconducting thin films, even in the presence of detrimental, radical forming processing additives. Using electron spin resonance spectroscopy and sensitive oxygen probes, we found that Ni(dtc) 2 acts as a broadband stabilizer that inhibits both the formation of reactive radicals and singlet oxygen. The mechanism of stabilization is of sacrificial nature, but contains non-sacrificial contributions in polymers where singlet oxygen is a key driver of photooxidation. Ultrafast pump-probe spectroscopy reveals quenching of triplet excited states as the central mechanism of non-sacrificial stabilization. When introduced into the active layer of organic photovoltaic devices, Ni(dtc) 2 retards the short circuit current loss in air without affecting the sensitive morphology of bulk heterojunctions and without major sacrifices in semiconductor properties. Antioxidants based on nickel complexes thus constitute functional stabilizers for elucidating degradation mechanisms in organic semiconductors and represent a cost-effective route toward organic electronic appliances with extended longevity. Broader contextOrganic semiconductors based on conjugated polymers bear exceptional opportunities for many disruptive technologies, including light and power generation, sensor technology and electronic circuitry, which could potentially be realized in a sustainable fashion using highly efficient and low-cost approaches. However, conjugated polymers suffer from photo-oxidation-induced performance loss and need to be carefully encapsulated, compromising both applicability and cost benefits. In the present work, we introduce a nickel chelate, nickel(II) dibutyldithiocarbamate, as a universal antioxidant for increasing the longevity of conjugated polymers. We carried out a mechanistic study that quantitatively describes the stabilization of conjugated polymer moieties with technological relevance for OLEDs, OPVs and OFETs. We introduce for the first time a figure of merit (FOM) as a stabilization metric for antioxidants in conjugated polymers. This FOM serves likewise to distinguish between sacrificial and non-sacrificial protective mechanisms. We draw wide ranging conclusions that reflect on how conjugated polymer and polymer:fullerene blends photo-oxidize and how the underlying mechanisms can be significantly suppressed in the presence of nickel chelates. Finally, we demonstrate its beneficial use in a broad range of organic photovoltaic devices.
Halide perovskites are emerging as a new class of materials for thermoelectric applications owing to their low thermal conductivity and high Seebeck coefficient (thermopower). In this work, the thermoelectric parameters of vapor-deposited hybrid perovskite thin films are explored for the first time. We establish a relationship between the chemical composition and thermoelectric properties of sequentially vapor-deposited CH3NH3PbI3 films. A composition-dependent grain size and in-plane electrical conductivity evolution is observed and its influence on thermoelectric properties is analyzed. An ultralow in-plane thermal conductivity of 0.32 ± 0.03 W m–1 K–1 at room temperature is recorded for CH3NH3PbI3 using a chip-based 3ω method. Thermal conductivity measurement of a series of CH3NH3PbI3 films reveals that the thermal transport is governed by the Pb–I lattice at room temperature. Furthermore, n- and p-type CH3NH3PbI3 films achieved by compositional tuning exhibit high negative (6500 μV/K) and positive (5500 μV/K) thermopower.
While photovoltaic blends based on non-fullerene acceptors are touted for their thermal stability, this type of acceptor tends to crystallize, which can result in a gradual decrease in photovoltaic performance and affects the reproducibility of the devices. Two halogenated indacenodithienothiophene-based acceptors that readily co-crystallize upon mixing are studied, which indicates that the use of an acceptor mixture alone does not guarantee the formation of a disordered mixture. The addition of the donor polymer to the acceptor mixture readily suppresses the crystallization, which results in a fine-grained ternary blend with nanometer-sized domains that do not coarsen due to a high T g ≈ 200 °C. As a result, annealing at temperatures of up to 170 °C does not markedly affect the photovoltaic performance of ternary devices, in contrast to binary devices that suffer from acceptor crystallization in the active layer. The results indicate that the ternary approach enables the use of high-temperature processing protocols, which are needed for upscaling and high-throughput fabrication of organic solar cells. Further, ternary devices display a stable photovoltaic performance at 130 °C for at least 205 h, which indicates that the use of acceptor mixtures allows to fabricate devices with excellent thermal stability.
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