Eszter Voroshazi

Solution-Processed MoO3 Thin Films As a Hole-Injection Layer for Organic Solar Cells

We report on a sol-gel-based technique to fabricate MoO(3) thin films as a hole-injection layer for solution-processed or thermally evaporated organic solar cells. The solution-processed MoO(3) (sMoO(3)) films are demonstrated to have equal performance to hole-injection layers composed of either PEDOT:PSS or thermally evaporated MoO(3) (eMoO(3)), and the annealing temperature at which the sol-gel layer begins to work is consistent with the thermodynamic analysis of the process. Finally, the shelf lifetime of devices made with the sMoO(3) is similar to equivalent devices prepared with a eMoO(3) hole-injection layer.

The ISOS-3 inter-laboratory collaboration focused on the stability of a variety of organic photovoltaic devices

Seven distinct sets (n ≥ 12) of state of the art organic photovoltaic devices were prepared by leading research laboratories in a collaboration planned at the Third International Summit on Organic Photovoltaic Stability (ISOS-3). All devices were shipped to RISO DTU and characterized simultaneously up to 1830 h in accordance with established ISOS-3 protocols under three distinct illumination conditions: accelerated full sun simulation; low level indoor fluorescent lighting; and dark storage with daily measurement under full sun simulation. Three nominally identical devices were used in each experiment both to provide an assessment of the homogeneity of the samples and to distribute samples for a variety of post soaking analytical measurements at six distinct laboratories enabling comparison at various stages in the degradation of the devices. Over 100 devices with more than 300 cells were used in the study. We present here design and fabrication details for the seven device sets, benefits and challenges associated with the unprecedented size of the collaboration, characterization protocols, and results both on individual device stability and uniformity of device sets, in the three illumination conditions.

Novel bis-C60 derivative compared to other fullerene bis-adducts in high efficiency polymer photovoltaic cells

We report the application of novel mono- and bis-o-quino-dimethane C60 (oQDMC60) adducts in bulk heterojunction photovoltaic devices. When blended with poly(3-hexylthiophene), the fullerene adducts presented here have an enhanced open-circuit voltage of 640 mV and 820 mV, while preserving high short-circuit current and fill factor, resulting in efficiencies of 4.1% and 5.2%, respectively. Detailed assessment of material properties relevant to photovoltaic devices such as energy levels, charge carrier mobility, absorption and solubility further complements the evaluation. Increased fullerene solubility hindering phase segregation in blends with bis-oQDMC60 has been circumvented by an in-depth morphology optimization assisted by absorption spectroscopy, X-ray reflectivity and atomic force microscopy. This optimized preparation could also serve as a guide for implementation of similar fullerene derivatives. Furthermore, we compare bis-oQDMC60 to previously reported fullerene bis-adducts to provide insight into this emerging class of materials.

Efficient truxenone-based acceptors for organic photovoltaics

Two electron-deficient truxenone derivatives are designed and synthesised for organic photovoltaic applications. The promise of this class of compounds as acceptor materials is illustrated by the fabrication of efficient bilayer solar cells with a subphthalocyanine (SubPc) donor, clearly outperforming reference cells with a soluble fullerene derivative as the acceptor.

Electron-deficient truxenone derivatives and their use in organic photovoltaics

A series of electron-deficient truxenone derivatives are investigated as fullerene alternatives in organic photovoltaic applications. These new electron-accepting molecules have easily tunable absorption profiles, more than ten-fold higher absorptivities than PCBM, slightly higher electron affinities than PCBM and clearly defined and highly reversible reductive characteristics. Fabrication of efficient bilayer solar cells with a subphthalocyanine (SubPc) donor illustrates the promise of this class of materials as electron acceptors in organic solar cells.

Nafion-modified MoOx as effective room-temperature hole injection layer for stable, high-performance inverted organic solar cells.

We present a hole injection layer processed from solution at room temperature for inverted organic solar cells. Bis(2,4-pentanedionato) molybdenum(VI) dioxide (MoO2(acac)2) is used as the precursor for MoOx. Small amounts of Nafion in the precursor solution allow it to form continuous films with good wetting onto the active layers. The hydrolysis of MoO2(acac)2 and the effects of adding Nafion to the precursor solution are studied by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The devices with solution-processed MoOx including Nafion exhibited comparable performance to the reference devices based on the commonly used hole injection layers such as poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) or evaporated MoO3. Inverted poly(3-hexylthiophene):[6,6]-phenyl C61-butyric acid methyl ester devices with Nafion-modified MoOx maintain 80% of their initial power conversion efficiency upon exposure to ambient air for ∼5000 h, outperforming devices with PEDOT:PSS or with evaporated MoO3.

The effect of anneal, solar irradiation and humidity on the adhesion/cohesion properties of P3HT:PCBM based inverted polymer solar cells

We use a thin-film adhesion technique that enables us to precisely measure the energy required to separate adjacent layers in OPV cells. We demonstrate the presence of weak interfaces in prototypical inverted polymer solar cells, either prepared by spin, spray or slot-die coating, including flexible and non flexible solar cells. In all cases, we observed adhesive failure at P3HT:PCBM/PEDOT:PSS interface, indicating the intrinsic material dependence of this mechanism. The impact of temperature, solar irradiation and humidity on the adhesion and cohesion properties of this particular interface is discussed. First, we have found that post-deposition annealing increases the adhesion significantly. Annealing changes the morphology in the photoactive layer and consequently alters the chemical properties at the interface. Second, solar irradiation on fully encapsulated solar cells has no damaging but in contrast an enhancing effect on the adhesion properties, due to the heat generated from IR radiation. Finally, the synergetic effect of stress and an environmental species like moisture greatly accelerates the decohesion rate in the weak hygroscopic PEDOT:PSS layer. This results in a loss of mechanical integrity and device performance. The insight into the mechanisms of delamination and decohesion yields general guidelines for the design of more reliable organic electronic devices.

Root-cause failure analysis of photocurrent loss in polythiophene:fullerene based inverted solar cells

Metal oxide transport layers have played a crucial role in recent progress in organic photovoltaic (OPV) device stability. Here, we measure the stability of inverted and encapsulated polythiophene:fullerene cells with MoO3/Ag/Al composite anode in operational conditions combining solar radiation and 65 °C. Performance loss of over 50% in the first 100 h of the aging is dominated by a drop in the short-circuit current (Jsc). We reveal a concurrent loss in reflectance from 85% to 50% above 650 nm, which is below the optical gap of the used photoactive materials, hence, excluding any major degradation in the bulk of this layer. Correlating the responses of aged devices to a series of test structures comprised of ITO/ZnO cathode, MoO3/Ag, and MoO3/Ag/Al anodes and their combinations with the active layer allowed us to identify that the presence of Al causes the reduced reflectance in these devices, independent of the presence of the active layer. Systematic single-stress aging on the test structures further indicates that elevated heat is the cause of the reflectance loss. Cross-section transmission electron microscopy coupled with elemental analysis revealed the unsuspected role of Al; notably, it diffuses through the entire 150 nm thick Ag layer and accumulates at the MoO3/Ag interface. Moreover, XRD analysis of the aged MoO3/Ag/Al anode indicates the formation of Ag2Al alloy. Depth profiling with X-ray photoelectron spectroscopy advanced our understanding by confirming the formation of Ag-Al intermetallic alloy and the presence of oxidized Al only at the MoO3/Ag interface suggesting a concomitant reduction of MoO3 to most probably MoO2. This latter compound is less reflective than MoO3, which can explain the reduced reflectance in aged devices as proven by optical simulations. On the basis of these results, we could estimate that 20% of the loss in Jsc is ascribed to reduction of MoO3 triggered by its direct contact with Al.

Role of Electron- and Hole-Collecting Buffer Layers on the Stability of Inverted Polymer: Fullerene Photovoltaic Devices

Systematic device performance and air stability comparison of inverted architecture polythiophene:fullerene photovoltaic cells with eight different electron-collecting layers (ECLs) and two hole-collecting layers are presented in this study. Regardless of the ECL, we achieved an efficiency of over 3.5% and lifetime of over 1000 h. These results indicate the relative interchangeability of various solution-processed ECLs. Long-term (>5000 h) air exposure revealed a secondary failure mechanism of inverted cells, which is assigned to hindered exciton harvesting. Notably, devices with a polymeric hole-collecting layer and Ag/Al electrode exhibited the longest lifetime (defined as 80% of the initial performance) of 4000 h, compared with 3000 h for MoO 3/Ag/Al.

Oxygen-Induced Degradation in C60-Based Organic Solar Cells: Relation Between Film Properties and Device Performance

Fullerene-based molecules are the archetypical electron-accepting materials for organic photovoltaic devices. A detailed knowledge of the degradation mechanisms that occur in C60 layers will aid in the development of more stable organic solar cells. Here, the impact of storage in air on the optical and electrical properties of C60 is studied in thin films and in devices. Atmospheric exposure induces oxygen-trap states that are 0.19 eV below the LUMO of the fullerene C60. Moreover, oxygen causes a 4-fold decrease of the exciton lifetime in C60 layers, resulting in a 40% drop of short-circuit current from optimized planar heterojunction solar cells. The presence of oxygen-trap states increases the saturation current of the device, resulting in a 20% loss of open-circuit voltage. Design guidelines are outlined to improve air stability for fullerene-containing devices.