Enhanced performance of lead sulfide quantum dot-sensitized solar cells by controlling the thickness of metal halide perovskite shells.

The metal halide perovskite CH3NH3PbI3 (MAP) can be applied as the shell layer of lead sulfide quantum dots (PbS QDs) for improving solar power conversion efficiency. However, basic physics for this PbS core/MAP shell QD system is still unclear and needs to be clarified to further improve efficiency. Therefore, in this study, we investigate how MAP shell thickness affects device performance and dynamics of charge carriers for PbS QD-sensitized solar cells. Covering the PbS QDs with the MAP shell layers of an appropriate thickness around 0.34 nm greatly suppresses charge carrier recombination at surface defects along with improved carrier transport to neighboring oxide and polymer layers. Therefore, this MAP shell thickness provides the highest open-circuit voltage, short-circuit current density, and fill factor for solar cells. Overall power conversion efficiencies of these solar cells reached about 4.1%, which is about six-fold higher than that for solar cells without MAP (about 0.7%). Additionally, use of the MAP shell layers can prevent oxidation of PbS QDs and, therefore, makes a degradation of solar cell performance slower in air.

Origins of High Performance and Degradation in the Mixed Perovskite Solar Cells.

The origins of the high device performance and degradation in the air are the greatest issues for commercialization of perovskite solar cells. Here this study investigates the possible origins of the mixed perovskite cells by monitoring defect states and compositional changes of the perovskite layer over the time. The results of deep-level transient spectroscopy analysis reveal that a newly identified defect formed by Br atoms exists at deep levels of the mixed perovskite film, and its defect state shifts when the film is aged in the air. The change of the defect state is originated from loss of the methylammonium molecules of the perovskite layer, which results in decreased JSC , deterioration of the power conversion efficiency and long-term stability of perovskite solar cells. The results provide a powerful strategy to diagnose and manage the efficiency and stability of perovskite solar cells.

Computational Analysis of the Interplay between Deep Level Traps and Perovskite Solar Cell Efficiency.

New deposition methods of halide perovskites are being developed with the aim of improving solar cell power conversion efficiency by controlling the physiochemical properties of the perovskite film. In the case of methylammonium lead iodide (MAPbI3), deep level traps limit efficiency by participating in charge carrier recombination. Prior work has shown that the solar cell efficiency of MAPbI3 solar cells varied significantly with deposition method; specifically, efficiencies of 13.5 and 17.7% were observed for MAPbI3 processed with a one- and two-step method, respectively. However, the origin of the difference in efficiency remains unclear. In this study, we analyze the interplay between deep level traps and efficiency by simulating the photoexcited charge carrier pathway across solar cells processed via the one- and two-step method using finite-element drift-diffusion modeling. We determined that in the case of one-step processing, the traps propagate throughout the bulk, while for two-step, the traps congregate at the interface where the MAPbI3 was grown (mesoporous TiO2). Composition and structural analysis are used to propose a plausible explanation as to why the difference in processing changes the spatial distribution of the traps.

High-Efficiency Air-Stable Colloidal Quantum Dot Solar Cells Based on a Potassium-Doped ZnO Electron-Accepting Layer.

High-efficiency colloidal quantum dot (CQD) solar cells (CQDSCs) with improved air stability were developed by employing potassium-modified ZnO as an electron-accepting layer (EAL). The effective potassium modification was achievable by a simple treatment with a KOH solution of pristine ZnO films prepared by a low-temperature solution process. The resulting K-doped ZnO (ZnO-K) exhibited EAL properties superior to those of a pristine ZnO-EAL. The Fermi energy level of ZnO was upshifted, which increased the internal electric field and amplified the depletion region (i.e., charge drift) of the devices. The surface defects of ZnO were effectively passivated by K modification, which considerably suppressed interfacial charge recombination. The CQDSC based on ZnO-K achieved improved power conversion efficiency (PCE) of ≈10.75% ( VOC of 0.67 V, JSC of 23.89 mA cm-2, and fill factor of 0.68), whereas the CQDSC based on pristine ZnO showed PCE of 9.97%. Moreover, the suppressed surface defects of ZnO-K substantially improved long-term stability under air. The device using ZnO-K exhibited superior long-term air storage stability (96% retention after 90 days) compared to that using pristine ZnO (88% retention after 90 days). The ZnO-K-based device also exhibited improved photostability under air. Under continuous light illumination for 600 min, the ZnO-K-based device retained 96% of its initial PCE, whereas the pristine ZnO-based device retained only 67%.

Efficient Planar Perovskite Solar Cells Using Passivated Tin Oxide as an Electron Transport Layer.

Planar perovskite solar cells using low-temperature atomic layer deposition (ALD) of the SnO2 electron transporting layer (ETL), with excellent electron extraction and hole-blocking ability, offer significant advantages compared with high-temperature deposition methods. The optical, chemical, and electrical properties of the ALD SnO2 layer and its influence on the device performance are investigated. It is found that surface passivation of SnO2 is essential to reduce charge recombination at the perovskite and ETL interface and show that the fabricated planar perovskite solar cells exhibit high reproducibility, stability, and power conversion efficiency of 20%.

Enhancing the Performance of Sensitized Solar Cells with PbS/CH3NH3PbI3 Core/Shell Quantum Dots.

We report on the fabrication of PbS/CH3NH3PbI3 (=MAP) core/shell quantum dot (QD)-sensitized inorganic-organic heterojunction solar cells on top of mesoporous (mp) TiO2 electrodes with hole transporting polymers (P3HT and PEDOT: PSS). The PbS/MAP core/shell QDs were in situ-deposited by a modified successive ionic layer adsorption and reaction (SILAR) process using PbI2 and Na2S solutions with repeated spin-coating and subsequent dipping into CH3NH3I (=MAI) solution in the final stage. The resulting device showed much higher efficiency as compared to PbS QD-sensitized solar cells without a MAP shell layer, reaching an overall efficiency of 3.2% under simulated solar illumination (AM1.5, 100 mW·cm(-2)). From the measurement of the impedance spectroscopy and the time-resolved photoluminescence (PL) decay, the significantly enhanced performance is mainly attributed to both reduced charge recombination and better charge extraction by MAP shell layer. In addition, we demonstrate that the MAP shell effectively prevented the photocorrosion of PbS, resulting in highly improved stability in the cell efficiency with time. Therefore, our approach provides method for developing high performance QD-sensitized solar cells.