Arman Mahboubi Soufiani

Optical Properties of Photovoltaic Organic-Inorganic Lead Halide Perovskites.

Over the last several years, organic-inorganic lead halide perovskites have rapidly emerged as a new photovoltaic contender. Although energy conversion efficiency above 20% has now been certified, improved understanding of the material properties contributing to these high performance levels may allow the progression to even higher efficiency, stable cells. The optical properties of these new materials are important not only to device design but also because of the insight they provide into less directly accessible properties, including energy-band structures, binding energies, and likely impact of excitons, as well as into absorption and inverse radiative recombination processes.

Polaronic exciton binding energy in iodide and bromide organic-inorganic lead halide perovskites

The last 4 years have seen the rapid emergence of a new solar cell technology based on organic-inorganic lead halide perovskites, primarily CH3NH3PbI3 and related halides involving Cl and Br. Debate continues on the role of excitons and free carriers in these materials. Recent studies report values of exciton binding energy for the iodide ranging from 0.7 meV to 200 meV, with vastly different implications for device operation and design. In the present work, previously neglected polarons are shown likely to have a major impact in determining excitonic properties. Polaronic exciton binding energies calculated using effective longitudinal optical phonon energies, deduced from permittivity measurements, are shown consistent with experimental energies for good quality samples of CH3NH3PbI3 and CH3NH3PbBr3, as determined over a large temperature range from optical absorption data. Bandgaps determined simultaneously show a discontinuity at the orthorhombic to tetragonal phase transition for the iodide, but not ...

Temperature dependent optical properties of CH3NH3PbI3 perovskite by spectroscopic ellipsometry

Mixed organic-inorganic halide perovskites have emerged as a promising new class of semiconductors for photovoltaics with excellent light harvesting properties. Thorough understanding of the optical properties of these materials is important for photovoltaic device optimization and the insight this provides for the knowledge of energy band structures. Here we present an investigation of the sub-room temperature dependent optical properties of polycrystalline thin films of CH3NH3PbI3 perovskites that are of increasing interest for photovoltaics. The complex dielectric function of CH3NH3PbI3 in the energy range of 0.5–4.1 eV is determined between 77 K and 297 K using spectroscopic ellipsometry. An increase in optical permittivity as the temperature decreases is illustrated for CH3NH3PbI3. Optical transitions and critical points were analyzed using the energy dependent second derivative of these dielectric functions as a function of temperature.

Impact of microstructure on the electron–hole interaction in lead halide perovskites

Despite the remarkable progress in the performance of devices based on the lead halide perovskite semiconductor family, there is still a lack of consensus on their fundamental photophysical properties. Here, using magneto-optical transmission spectroscopy we elucidate the impact of the microstructure on the Coulomb interaction between photo-created electron–hole pairs in methylammonium lead triiodide (MAPbI3) and the triple-cation lead mixed-halide composition, Cs0.05(MA0.17FA0.83)0.95Pb(I0.83Br0.17)3 (Cs: cesium, MA: methylammonium, FA: formamidinium) by investigating thin films with a wide range of grain sizes from tens of nanometers to microns. At low temperatures, in which thermal fluctuations of the interactions are frozen and the rotational disorder of the organic cation is negligible, the exciton binding energy and reduced effective mass of carriers remain effectively unchanged with grain size. We conclude that the microstructure plays a negligible role in the Coulomb interaction of the photo-created electron–hole pairs, in contrast to previous reports. This renewed understanding of the relationship between these fundamental electronic properties and the microstructure is critical for future fundamental studies and improving device design.

Solution-Processed Lithium-Doped ZnO Electron Transport Layer for Efficient Triple Cation (Rb, MA, FA) Perovskite Solar Cells

The current work reports the lithium (Li) doping of a low-temperature processed zinc oxide (ZnO) electron transport layer (ETL) for highly efficient, triple-cation-based MA0.57FA0.38Rb0.05PbI3 (MA: methylammonium, FA: formamidinium, Rb: rubidium) perovskite solar cells (PSCs). Lithium intercalation in the host ZnO lattice structure is dominated by interstitial doping phenomena, which passivates the intrinsic defects in ZnO film. In addition, interstitial Li doping also downshifts the Fermi energy position of Li-doped ETL by 30 meV, which contributes to the reduction of the electron injection barrier from the photoactive perovskite layer. Compared to the pristine ZnO, the power conversion efficiency (PCE) of the PSCs incorporating lithium-doped ZnO (Li-doped) is raised from 14.07 to 16.14%. The superior performance is attributed to the reduced current leakage, enhanced charge extraction characteristics, and mitigated trap-assisted recombination phenomena in Li-doped devices, thoroughly investigated by means of electrochemical impedance spectroscopy (EIS) analysis. Li-doped PSCs also exhibit lower photocurrent hysteresis than ZnO devices, which is investigated with regard to the electrode polarization phenomena of the fabricated devices.