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The photoinduced open-circuit voltage ( Voc) loss commonly observed in bulk heterojunction organic solar cells made from amorphous polymers is investigated. It is observed that the total charge carrier density and, importantly, the recombination dynamics are unchanged by photoinduced burn-in. Charge extraction is used to monitor changes in the density of states (DOS) during degradation of the solar cells, and a broadening over time is observed. It is proposed that the Voc losses observed during burn-in are caused by a redistribution of charge carriers in a broader DOS. The temperature and light intensity dependence of the Voc losses can be described with an analytical model that contains the amount of disorder broadening in a Gaussian DOS as the only fit parameter. Finally, the Voc loss in solar cells made from amorphous and crystalline polymers is compared and an increased stability observed in crystalline polymer solar cells is investigated. It is found that solar cells made from crystalline materials have a considerably higher charge carrier density than those with amorphous materials. The effects of a DOS broadening upon aging are suppressed in solar cells with crystalline materials due to their higher carrier density, making crystalline materials more stable against Voc losses during burn-in. [ABSTRACT FROM AUTHOR]

Long-term stability of polymer solar cells is determined by many factors, one of which is thermal stability. Although many thermal stability studies occur far beyond the operating temperature of a solar cell which is almost always less than 65 °C, thermal degradation is studied at temperatures that the solar cell would encounter in real-world operating conditions. At these temperatures, movement of the polymer and fullerenes, along with adhesion of the polymer to the back contact, creates a barrier for electron extraction. The polymer barrier can be removed and the performance can be restored by peeling off the electrode and depositing a new one. X-ray photoelectron spectroscopy measurements reveal a larger amount of polymer adhered to electrodes peeled from aged devices than electrodes peeled from fresh devices. The degradation caused by hole-transporting polymer adhering to the electrode can be suppressed by using an inverted device where instead of electrons, holes are extracted at the back metal electrode. The problem can be ultimately eliminated by choosing a polymer with a high glass transition temperature. [ABSTRACT FROM AUTHOR]

The bulk heterojunction (BHJ) solar cell performance of many polymers depends on the polymer molecular weight ( Mn) and the solvent additive(s) used for solution processing. However, the mechanism that causes these dependencies is not well understood. This work determines how Mn and solvent additives affect the performance of BHJ solar cells made with the polymer poly(di(2-ethylhexyloxy)benzo[1,2- b:4,5- b′]dithiophene- co-octylthieno[3,4- c]pyrrole-4,6-dione) (PBDTTPD). Low Mn PBDTTPD devices have exceedingly large fullerene-rich domains, which cause extensive charge-carrier recombination. Increasing the Mn of PBDTTPD decreases the size of these domains and significantly improves device performance. PBDTTPD aggregation in solution affects the size of the fullerene-rich domains and this effect is linked to the dependency of PBDTTPD solubility on Mn. Due to its poor solubility high Mn PBDTTPD quickly forms a fibrillar polymer network during spin-casting and this network acts as a template that prevents large-scale phase separation. Furthermore, processing low Mn PBDTTPD devices with a solvent additive improves device performance by inducing polymer aggregation in solution and preventing large fullerene-rich domains from forming. These findings highlight that polymer aggregation in solution plays a significant role in determining the morphology and performance of BHJ solar cells. [ABSTRACT FROM AUTHOR]

Most optimized donor-acceptor (D-A) polymer bulk heterojunction (BHJ) solar cells have active layers too thin to absorb greater than ∼80% of incident photons with energies above the polymer's band gap. If the thickness of these devices could be increased without sacrificing internal quantum efficiency, the device power conversion efficiency (PCE) could be significantly enhanced. We examine the device characteristics of BHJ solar cells based on poly(di(2-ethylhexyloxy)benzo[1,2- b:4,5- b′]dithiophene- co-octylthieno[3,4- c]pyrrole-4,6-dione) (PBDTTPD) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) with 7.3% PCE and find that bimolecular recombination limits the active layer thickness of these devices. Thermal annealing does not mitigate these bimolecular recombination losses and drastically decreases the PCE of PBDTTPD BHJ solar cells. We characterize the morphology of these BHJs before and after thermal annealing and determine that thermal annealing drastically reduces the concentration of PCBM in the mixed regions, which consist of PCBM dispersed in the amorphous portions of PBDTTPD. Decreasing the concentration of PCBM may reduce the number of percolating electron transport pathways within these mixed regions and create morphological electron traps that enhance charge-carrier recombination and limit device quantum efficiency. These findings suggest that (i) the concentration of PCBM in the mixed regions of polymer BHJs must be above the PCBM percolation threshold in order to attain high solar cell internal quantum efficiency, and (ii) novel processing techniques, which improve polymer hole mobility while maintaining PCBM percolation within the mixed regions, should be developed in order to limit bimolecular recombination losses in optically thick devices and maximize the PCE of polymer BHJ solar cells. [ABSTRACT FROM AUTHOR]

Polymer:fullerene solar cells are demonstrated with power conversion efficiencies over 7% with blends of PBDTTPD and PC61BM. These devices achieve open-circuit voltages ( Voc) of 0.945 V and internal quantum efficiencies of 88%, making them an ideal candidate for the large bandgap junction in tandem solar cells. Voc's above 1.0 V are obtained when the polymer is blended with multiadduct fullerenes; however, the photocurrent and fill factor are greatly reduced. In PBDTTPD blends with multiadduct fullerene ICBA, fullerene emission is observed in the photoluminescence and electroluminescence spectra, indicating that excitons are recombining on ICBA. Voltage-dependent, steady state and time-resolved photoluminescence measurements indicate that energy transfer occurs from PBDTTPD to ICBA and that back hole transfer from ICBA to PBDTTPD is inefficient. By analyzing the absorption and emission spectra from fullerene and charge transfer excitons, we estimate a driving free energy of -0.14 ± 0.06 eV is required for efficient hole transfer. These results suggest that the driving force for hole transfer may be too small for efficient current generation in polymer:fullerene solar cells with Voc values above 1.0 V and that non-fullerene acceptor materials with large optical gaps (>1.7 eV) may be required to achieve both near unity internal quantum efficiencies and values of Voc exceeding 1.0 V. [ABSTRACT FROM AUTHOR]

Understanding the stability and degradation mechanisms of organic solar materials is critically important to achieving long device lifetimes. Here, an investigation of the photodegradation of polymer:fullerene blend films exposed to ambient conditions for a variety of polymer and fullerene derivative combinations is presented. Despite the wide range in polymer stabilities to photodegradation, the rate of irreversible polymer photobleaching in blend films is found to consistently and dramatically increase with decreasing electron affinity of the fullerene derivative. Furthermore, blends containing fullerenes with the smallest electron affinities photobleached at a faster rate than films of the pure polymer. These observations can be explained by a mechanism where both the polymer and fullerene donate photogenerated electrons to diatomic oxygen to form the superoxide radical anion which degrades the polymer. [ABSTRACT FROM AUTHOR]