This thesis discusses vacuum deposited organic solar cells. It focuses on the investigation of new donor molecules blended with the standard electron acceptor C60. These donor-acceptor heterojunctions form the photoactive system of organic solar cells. In addition, the influence of the processing conditions on the morphology of the blend layers is investigated, as the morphology is crucial for an efficient generation of free charge carriers upon photon absorption.
Bulk heterojunction solar cells with the donor DTDCTB are deposited at different substrate temperatures. We identify three substrate temperature regimes, discriminated by the behavior of the fill factor (FF ) as a function of the blend layer thickness. Devices deposited at RT have a maximum FF between 50 and 70 nm blend thickness, while devices deposited at 110 °C have a monotonically decreasing FF. At Tsub=85 °C, the devices have an S-kinked current-voltage curve. Grazing incidence wide angle X-ray scattering measurements show that this peculiar behavior of the FF is not correlated with a change in the crystallinity of the DTDCTB, which stays amorphous. Absorption measurements show that the average alignment of the molecules inside the blend also remains unchanged. Charge extraction measurements (OTRACE) reveal a mobility for the 110 °C device that is an order of magnitude higher than for the RT device. The difference in mobility can be explained by a higher trap density for the RT samples as measured by impedance spectroscopy. Despite slightly higher carrier lifetimes for the RT device obtained by transient photovoltage measurements, its mobility-lifetime product is still lower than for the 110 °C devices.
Based on DTDCTB, three new donor materials are designed to have a higher thermal stability in order to achieve higher yields upon material purification using gradient sublimation. For PRTF, the thermal stability is increased demonstrated by a higher yield upon sublimation. However, all new materials have a reduced absorption as compared to DTDCTB, which limits the short current density, and the FF is more sensitive to an increase of the blend layer thickness. The highest power conversion efficiency is achieved for a PRTF:C60 solar cell with 3.8%. Interestingly, PRTF:C60 solar cells show exceptionally low nonradiative voltage losses of only 0.26 V.
Another absorber molecule is the push-pull chromophore QM1. Scanning electron microscope (SEM) measurements show a growth of the molecule in nanowires on several substrates. The nanowires have lengths up to several micrometers and are several tens of nanometers wide. The formation of the nanowires is accompanied by a strong blue shift (650 meV) of the thin film absorption spectrum in comparison to the absorption in solution, which is attributed to H-aggregation of the molecules. Furthermore, the thin film absorption onset reaches up to 1100 nm, making the material a suitable candidate for a near infrared absorber in organic solar cells. For a solar cell in combination with C60, a power conversion efficiency of 1.9% was achieved with an external quantum efficiency of over 19% for the spectral range between 600 and 1000 nm.
The method of “co-evaporant induced crystallization” as a means to increase the crystallinity of blend layers without increasing the substrate temperature during the deposition is investigated. Mass spectrometry (LDI-ToF-MS) measurements show that polydimethylsiloxane (PDMS), which is used as a co-evaporant, decomposes during the evaporation and only lighter oligomers evaporate. Quartz crystal microbalance (QCM) measurements prove that the detection of PDMS saturates at higher amounts of evaporated material. LDI-ToF-MS measurements show further that the determination of the volatilization temperature by QCM measurements is highly error prone. The method was applied to zinc phthalocyanine (ZnPc) :C60 solar cells, accepting the insertion of PDMS into the blend layer. Diffraction (GIXRD) measurements show a large increase in crystallinity. ZnPc:C60 solar cells produced by applying the method reveal a similar behavior as solar cells processed at a higher substrate temperature
