Sarah M. Vorpahl

Bio: Sarah M. Vorpahl is an academic researcher from University of Washington. The author has contributed to research in topics: Perovskite (structure) & Grain boundary. The author has an hindex of 8, co-authored 9 publications receiving 1955 citations. Previous affiliations of Sarah M. Vorpahl include Washington State University.

Impact of microstructure on local carrier lifetime in perovskite solar cells

Abstract: The remarkable performance of hybrid perovskite photovoltaics is attributed to their long carrier lifetimes and high photoluminescence (PL) efficiencies. High-quality films are associated with slower PL decays, and it has been claimed that grain boundaries have a negligible impact on performance. We used confocal fluorescence microscopy correlated with scanning electron microscopy to spatially resolve the PL decay dynamics from films of nonstoichiometric organic-inorganic perovskites, CH3NH3PbI3(Cl). The PL intensities and lifetimes varied between different grains in the same film, even for films that exhibited long bulk lifetimes. The grain boundaries were dimmer and exhibited faster nonradiative decay. Energy-dispersive x-ray spectroscopy showed a positive correlation between chlorine concentration and regions of brighter PL, whereas PL imaging revealed that chemical treatment with pyridine could activate previously dark grains.

Lithium-doping inverts the nanoscale electric field at the grain boundaries in Cu2ZnSn(S,Se)4 and increases photovoltaic efficiency

Abstract: Passive grain boundaries (GBs) are essential for polycrystalline solar cells to reach high efficiency. However, the GBs in Cu2ZnSn(S,Se)4 have less favorable defect chemistry compared to CuInGaSe2. Here, using scanning probe microscopy we show that lithium doping of Cu2ZnSn(S,Se)4 changes the polarity of the electric field at the GB such that minority carrier electrons are repelled from the GB. Solar cells with lithium-doping show improved performance and yield a new efficiency record of 11.8% for hydrazine-free solution-processed Cu2ZnSn(S,Se)4. We propose that lithium competes for copper vacancies (forming benign isoelectronic LiCu defects) decreasing the concentration of ZnCu donors and competes for zinc vacancies (forming a LiZn acceptor that is likely shallower than CuZn). Both phenomena may explain the order of magnitude increase in conductivity. Further, the effects of lithium doping reported here establish that extrinsic species are able to alter the nanoscale electric fields near the GBs in Cu2ZnSn(S,Se)4. This will be essential for this low-cost Earth abundant element semiconductor to achieve efficiencies that compete with CuInGaSe2 and CdTe.

Zr Incorporation into TiO2 Electrodes Reduces Hysteresis and Improves Performance in Hybrid Perovskite Solar Cells while Increasing Carrier Lifetimes

Abstract: We investigate zirconium (Zr) incorporation into the titanium dioxide (TiO2) electron-transporting layer used in organometal halide perovskite photovoltaics. Compared to Zr-free controls, solar cells employing electrodes containing Zr exhibit increased power conversion efficiency (PCE) and decreased hysteresis. We use transient photovoltage and photocurrent extraction to measure carrier lifetimes and densities and observe longer carrier lifetimes and higher charge densities in devices on Zr-containing electrodes at microsecond times as well as longer persistent photovoltages extending from ∼milliseconds to tens of seconds. We characterize the surface stoichiometry and change in work function and reduction potential of the TiO2 upon incorporation of Zr and discuss the charge recombination at the TiO2 interface in the context of these variables. Finally, we show that the combination of Zr–TiO2 electrode modification with device pyridine treatment leads to a cumulative improvement in performance.

Photodecomposition and Morphology Evolution of Organometal Halide Perovskite Solar Cells

Abstract: We study the photoinduced degradation of hybrid organometal perovskite photovoltaics under illumination and ambient atmosphere using UV–vis absorption, atomic force microscopy, and device performance. We correlate the structural changes in the surface of the perovskite film with changes in the optical and electronic properties of the devices. The photodecomposition of the methylammonium lead triiodide perovskite layer itself proceeds much more slowly than the photodegradation of the performance of devices with fullerene/bathocuproine/aluminum top contacts, indicating that the active layer alone is more stable than the interface with the electrodes in this geometry. The evolution of the perovskite active layer performance proceeded through several phases: (1) an initial improvement in device characteristics, (2) a plateau with very slow degradation, and (3) a catastrophic decline in material performance accompanied by marked changes in film morphology. The rapid increase in surface roughness of the active ...

Orientation of Ferroelectric Domains and Disappearance upon Heating Methylammonium Lead Triiodide Perovskite from Tetragonal to Cubic Phase

Abstract: We study the spontaneous polarization of the archetypal semiconducting halide perovskite methylammonium lead triiodide (CH3NH3PbI3) that is currently being investigated for use in thin film solar cells and light-emitting diodes. Using both lateral and vertical piezoresponse force microscopy (PFM) to image polycrystalline thin films, we observed domains in the piezoresponse that reversibly appear and disappear below and above the tetragonal-to-cubic phase transition temperature. Importantly, we observe these domains to exhibit a piezoresponse that is predominantly in-plane for films with the (110) plane oriented parallel to the substrate, providing a measure of the polarization associated with specific crystal planes. We characterize the polarization and its temporal response using both local switching spectroscopy and time-dependent PFM spectra. These data show hysteresis loops with the polarization switching with bias but relaxing back on time scales of several minutes. Our results suggest the existence ...

Surface passivation of perovskite film for efficient solar cells

Abstract: In recent years, the power conversion efficiency of perovskite solar cells has increased to reach over 20%. Finding an effective means of defect passivation is thought to be a promising route for bringing further increases in the power conversion efficiency and the open-circuit voltage (VOC) of perovskite solar cells. Here, we report the use of an organic halide salt phenethylammonium iodide (PEAI) on HC(NH2)2–CH3NH3 mixed perovskite films for surface defect passivation. We find that PEAI can form on the perovskite surface and results in higher-efficiency cells by reducing the defects and suppressing non-radiative recombination. As a result, planar perovskite solar cells with a certificated efficiency of 23.32% (quasi-steady state) are obtained. In addition, a VOC as high as 1.18 V is achieved at the absorption threshold of 1.53 eV, which is 94.4% of the Shockley–Queisser limit VOC (1.25 V). Planar perovskite solar cells that have been passivated using the organic halide salt phenethylammonium iodide are shown to have suppressed non-radiative recombination and operate with a certified power conversion efficiency of 23.3%.

High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells

Abstract: Three-dimensional organic-inorganic perovskites have emerged as one of the most promising thin-film solar cell materials owing to their remarkable photophysical properties, which have led to power conversion efficiencies exceeding 20 per cent, with the prospect of further improvements towards the Shockley-Queisser limit for a single‐junction solar cell (33.5 per cent). Besides efficiency, another critical factor for photovoltaics and other optoelectronic applications is environmental stability and photostability under operating conditions. In contrast to their three-dimensional counterparts, Ruddlesden-Popper phases--layered two-dimensional perovskite films--have shown promising stability, but poor efficiency at only 4.73 per cent. This relatively poor efficiency is attributed to the inhibition of out-of-plane charge transport by the organic cations, which act like insulating spacing layers between the conducting inorganic slabs. Here we overcome this issue in layered perovskites by producing thin films of near-single-crystalline quality, in which the crystallographic planes of the inorganic perovskite component have a strongly preferential out-of-plane alignment with respect to the contacts in planar solar cells to facilitate efficient charge transport. We report a photovoltaic efficiency of 12.52 per cent with no hysteresis, and the devices exhibit greatly improved stability in comparison to their three-dimensional counterparts when subjected to light, humidity and heat stress tests. Unencapsulated two-dimensional perovskite devices retain over 60 per cent of their efficiency for over 2,250 hours under constant, standard (AM1.5G) illumination, and exhibit greater tolerance to 65 per cent relative humidity than do three-dimensional equivalents. When the devices are encapsulated, the layered devices do not show any degradation under constant AM1.5G illumination or humidity. We anticipate that these results will lead to the growth of single-crystalline, solution-processed, layered, hybrid, perovskite thin films, which are essential for high-performance opto-electronic devices with technologically relevant long-term stability.

Efficient and stable solution-processed planar perovskite solar cells via contact passivation.

Abstract: Planar perovskite solar cells (PSCs) made entirely via solution processing at low temperatures (<150°C) offer promise for simple manufacturing, compatibility with flexible substrates, and perovskite-based tandem devices. However, these PSCs require an electron-selective layer that performs well with similar processing. We report a contact-passivation strategy using chlorine-capped TiO2 colloidal nanocrystal film that mitigates interfacial recombination and improves interface binding in low-temperature planar solar cells. We fabricated solar cells with certified efficiencies of 20.1 and 19.5% for active areas of 0.049 and 1.1 square centimeters, respectively, achieved via low-temperature solution processing. Solar cells with efficiency greater than 20% retained 90% (97% after dark recovery) of their initial performance after 500 hours of continuous room-temperature operation at their maximum power point under 1-sun illumination (where 1 sun is defined as the standard illumination at AM1.5, or 1 kilowatt/square meter).

Halide Perovskite Photovoltaics: Background, Status, and Future Prospects

Abstract: The photovoltaics of organic–inorganic lead halide perovskite materials have shown rapid improvements in solar cell performance, surpassing the top efficiency of semiconductor compounds such as CdTe and CIGS (copper indium gallium selenide) used in solar cells in just about a decade. Perovskite preparation via simple and inexpensive solution processes demonstrates the immense potential of this thin-film solar cell technology to become a low-cost alternative to the presently commercially available photovoltaic technologies. Significant developments in almost all aspects of perovskite solar cells and discoveries of some fascinating properties of such hybrid perovskites have been made recently. This Review describes the fundamentals, recent research progress, present status, and our views on future prospects of perovskite-based photovoltaics, with discussions focused on strategies to improve both intrinsic and extrinsic (environmental) stabilities of high-efficiency devices. Strategies and challenges regardi...

Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations

Abstract: The ionic defects at the surfaces and grain boundaries of organic–inorganic halide perovskite films are detrimental to both the efficiency and stability of perovskite solar cells. Here, we show that quaternary ammonium halides can effectively passivate ionic defects in several different types of hybrid perovskite with their negative- and positive-charged components. The efficient defect passivation reduces the charge trap density and elongates the carrier recombination lifetime, which is supported by density-function-theory calculation. The defect passivation reduces the open-circuit-voltage deficit of the p–i–n-structured device to 0.39 V, and boosts the efficiency to a certified value of 20.59 ± 0.45%. Moreover, the defect healing also significantly enhances the stability of films in ambient conditions. Our findings provide an avenue for defect passivation to further improve both the efficiency and stability of solar cells. Losses in solar cells can be caused by material defects in the bulk or at interfaces. Here, Zheng et al. use quaternary ammonium halides to passivate various perovskite absorbers and prepare solar cells with certified efficiency above 20%, suggesting that both anionic and cation defects are affected.