Philipp Rieder

Identification of Trap States in Perovskite Solar Cells.

Thermally stimulated current (TSC) measurements are used to characterize electronic trap states in methylammonium lead iodide perovsite solar cells. Several TSC peaks were observed over the temperature range from 20 K to room temperature. To elucidate the origins of these peaks, devices with various organic charge transport layers and devices without transport layers were tested. Two peaks appear at very low temperatures, indicating shallow trap states that are mainly attributed to the PCBM/C60 electron transport bilayer. However, two additional peaks appear at higher temperatures, that is, they are deeper in energy, and are assigned to the perovskite layer. At around T = 163 K, a sharp peak, also present in the dark TSC measurements, is assigned to the orthorhombic-tetragonal phase transition in the perovskite. However, a peak at around T = 191 K is assigned to trap states with activation energies of around 500 meV but with a rather low concentration of 1 × 10(21) m(-3).

Improved charge carrier lifetime in planar perovskite solar cells by bromine doping

The charge carrier lifetime is an important parameter in solar cells as it defines, together with the mobility, the diffusion length of the charge carriers, thus directly determining the optimal active layer thickness of a device. Herein, we report on charge carrier lifetime values in bromine doped planar methylammonium lead iodide (MAPbI3) solar cells determined by transient photovoltage. The corresponding charge carrier density has been derived from charge carrier extraction. We found increased lifetime values in solar cells incorporating bromine compared to pure MAPbI3 by a factor of ~2.75 at an illumination intensity corresponding to 1 sun. In the bromine containing solar cells we additionally observe an anomalously high value of extracted charge, which we deduce to originate from mobile ions.

Single-crystal-like optoelectronic-properties of MAPbI3 perovskite polycrystalline thin films

Our understanding of the crystallization process of hybrid halide perovskites has propelled the efficiency of state-of-the-art photovoltaic devices to over 22%. Further improvements to the performance will likely arise from reducing the number of grain boundaries. Here, current methods lead to grain sizes in the 1 micrometer range and the resulting optoelectronic properties suffer as compared to single-crystal materials. In this work, we introduce a new synthesis procedure with MAPbI3 leading to crystal sizes in the tens of microns range. This approach is based on the pre-crystallization of an intermediate phase (IP) based on the solid-state reaction of a lead-acetate trihydrate precursor mixture in a highly polar solvent. Beyond large grain sizes, the crystal orientation is also tightly controlled, leading to perovskite crystallites which remain perfectly aligned with the c-axis of the tetragonal structure parallel to the substrate as evidenced by grazing incidence wide angle X-ray scattering (GIWAXS). Furthermore, we demonstrate the high crystallinity and large grain size of the developed films via high-resolution transmission electron microscopy (HRTEM). The charge carrier mobilities are significantly improved with larger grain size and approach mobility values of about 40 cm2 V−1 s−1, moving toward the values observed for single crystals. We capitalize on the enhanced optoelectronic properties of the developed films by incorporating them into planar heterojunction solar cells which reach power conversion efficiencies of 18.5%, higher than MAPbI3-based device prepared from standard methods in a like-to-like comparison.

Influence of Fermi Level Alignment with Tin Oxide on the Hysteresis of Perovskite Solar Cells

We tune the Fermi level alignment between the SnO x electron transport layer (ETL) and Cs0.05(FA0.83MA0.17)0.95Pb(I0.83Br0.17)3 and highlight that this parameter is interlinked with current-voltage hysteresis in perovskite solar cells (PSCs). Furthermore, thermally stimulated current measurements reveal that the depth of trap states in the ETL or at the ETL-perovskite interface correlates with Fermi level positions, ultimately linking it to the energy difference between the Fermi level and conduction band minimum. In the presence of deep trap states, charge accumulation and recombination at the interface are promoted, affecting the charge collection efficiency adversely, which increases the hysteresis of PSCs.

Impact of Interfaces and Laser Repetition Rate on Photocarrier Dynamics in Lead Halide Perovskites

We studied charge carrier recombination in methylammonium lead iodide (MAPbI3) perovskite and the impact of interfaces on the charge carrier lifetime using time-resolved photoluminescence. Pristine films and those covered with organic electron and hole transport materials (ETM and HTM) were investigated at various laser repetition rates ranging from 10 kHz to 10 MHz in order to separate the bulk and interface-affected recombination. We revealed two different components in the PL decay. The fast component (shorter than 300 ns) is assigned to interfacial processes and the slow one to bulk recombination. A high repetition pulse train was shown to shorten PL decay in pristine perovskite while significantly prolonging the photocarrier lifetime in MAPbI3 covered by TMs. This effect can be qualitatively explained with a kinetic model taking interface traps into account. We demonstrate a significant influence of the excitation repetition rate on photocarrier lifetime, which should be considered when studying charge carrier dynamics in perovskites.