David McMeekin

Abstract:

Perovskite solar cells have shown phenomenal progress and have great potential to be manufactured as low‐cost large area modules. However, perovskite films often suffer from pinholes and the resulting contact between hole‐ and electron transporting layers provides lower resistance (shunt) pathways, leading to decreased open‐circuit voltage and fill factor. This problem is even more severe in large area cells and especially in the case of neutral color semitransparent cells, where a large absorber‐free area is required to provide the desired transparency. Herein, a simple, inexpensive, and scalable wet chemical method is presented to block these “shunting paths” via deposition of transparent, insulating molecular layers, which preferentially bind to the uncovered surface of the electron collecting oxide, without hindering charge extraction from the perovskite to the charge collection layers. It is shown that this method improves the performance in semitransparent cells, where the enhancement in open‐circuit voltage is up to 30% without negatively impacting the photocurrent. Using this method, we achieved an efficiency of 6.1% for a neutral color semitransparent perovskite cell with 38% average visible transmittance. This simple shunt blocking technique has applications in improving the yield as well as efficiency of large area perovskite solar cells and light emitting devices.

Abstract:

Metal halide perovskite photovoltaic cells could potentially boost the efficiency of commercial silicon photovoltaic modules from ∼20 toward 30% when used in tandem architectures. An optimum perovskite cell optical band gap of ~1.75 electron volts (eV) can be achieved by varying halide composition, but to date, such materials have had poor photostability and thermal stability. Here we present a highly crystalline and compositionally photostable material, [HC(NH2)2](0.83)Cs(0.17)Pb(I(0.6)Br(0.4))3, with an optical band gap of ~1.74 eV, and we fabricated perovskite cells that reached open-circuit voltages of 1.2 volts and power conversion efficiency of over 17% on small areas and 14.7% on 0.715 cm(2) cells. By combining these perovskite cells with a 19%-efficient silicon cell, we demonstrated the feasibility of achieving >25%-efficient four-terminal tandem cells.

Abstract:

High-efficiency perovskite solar cells typically employ an organic–inorganic metal halide perovskite material as light absorber and charge transporter, sandwiched between a p-type electron-blocking organic hole-transporting layer and an n-type hole-blocking electron collection titania compact layer. Some device configurations also include a thin mesoporous layer of TiO2 or Al2O3 which is infiltrated and capped with the perovskite absorber. Herein, we demonstrate that it is possible to fabricate planar and mesoporous perovskite solar cells devoid of an electron selective hole-blocking titania compact layer, which momentarily exhibit power conversion efficiencies (PCEs) of over 13%. This performance is however not sustained and is related to the previously observed anomalous hysteresis in perovskite solar cells. The “compact layer-free” meso-superstructured perovskite devices yield a stabilised PCE of only 2.7% while the compact layer-free planar heterojunction devices display no measurable steady state power output when devoid of an electron selective contact. In contrast, devices including the titania compact layer exhibit stabilised efficiency close to that derived from the current voltage measurements. We propose that under forward bias the perovskite diode becomes polarised, providing a beneficial field, allowing accumulation of positive and negative space charge near the contacts, which enables more efficient charge extraction. This provides the required built-in potential and selective charge extraction at each contact to temporarily enable efficient operation of the perovskite solar cells even in the absence of charge selective n- and p-type contact layers. The polarisation of the material is consistent with long range migration and accumulation of ionic species within the perovskite to the regions near the contacts. When the external field is reduced under working conditions, the ions can slowly diffuse away from the contacts redistributing throughout the film, reducing the field asymmetry and the effectiveness of the operation of the solar cells. We note that in light of recent publications showing high efficiency in devices devoid of charge selective contacts, this work reaffirms the absolute necessity to measure and report the stabilised power output under load when characterizing perovskite solar cells.