Photoinduced Self-Gating of Perovskite Photovoltaic Cells in Ionic Liquid.

We demonstrate that the power conversion efficiency (PCE), photocurrent, and fill factor (FF) of perovskite solar cells (PSC) can be significantly improved by the photoinduced self-gating in ionic liquids (ILs) via n-doping of the carbon nanotube (CNT) top electrode on the fullerene electron transport layer (ETL). CNTs, graphene, and other carbon electrodes have been proven to be stable electrodes for PSC, but efficiency was not high. We have previously shown that the performance of PSCs with CNT electrodes can be improved by IL gating with gate voltage (Vg) applied from an external power source. Here we demonstrate that effective self-gating in ILs is possible by a photoinduced process, without an external source. The open circuit voltage (Voc) generated by the PSC itself can be applied to the CNT/C60 electrode as Vg leading to photogating. This self-gating with Voc is compared to photocharging of CNTs in ILs without any gating for two types of fullerene ETLs: C60 and C70, Two types of ILs, DEME-TFSI and BMIM-BF4, are tested for two types of nanotubes electrodes: single wall (SWCNT), and multiwall (MWCNT). The resulting improvements are analyzed using the effective diode-circuit (DC) and the drift-diffusion (DD) models. Self-gating allows the PCE improvement from 3-5% to 10-11% for PSCs with a thick ETL, while for optimal combination of a thin SWCNT/ETL with added layers for improved stability, the PCE reached 13.2% in DEME-TFSI IL.

Surface Energy-Driven Preferential Grain Growth of Metal Halide Perovskites: Effects of Nanoimprint Lithography Beyond Direct Patterning.

Hybrid organic-inorganic lead halide perovskites have attracted much attention in the field of optoelectronic devices because of their desirable properties such as high crystallinity, smooth morphology, and well-oriented grains. Recently, it was shown that thermal nanoimprint lithography (NIL) is an effective method not only to directly pattern but also to improve the morphology, crystallinity, and crystallographic orientations of annealed perovskite films. However, the underlining mechanisms behind the positive effects of NIL on perovskite material properties have not been understood. In this work, we study the kinetics of perovskite grain growth with surface energy calculations by first-principles density functional theory (DFT) and reveal that the surface energy-driven preferential grain growth during NIL, which involves multiplex processes of restricted grain growth in the surface-normal direction, abnormal grain growth, crystallographic reorientation, and grain boundary migration, is the enabler of the material quality enhancement. Moreover, we develop an optimized NIL process and prove its effectiveness by employing it in a perovskite light-emitting electrochemical cell (PeLEC) architecture, in which we observe a fourfold enhancement of maximum current efficiency and twofold enhancement of luminance compared to a PeLEC without NIL, reaching a maximum current efficiency of 0.07598 cd/A at 3.5 V and luminance of 1084 cd/m2 at 4 V.