Shuzi HAYASE (早瀬 修二)

Abstract

All‐perovskite tandem solar cells are regarded as the next generation of devices capable of enhancing the solar energy utilization rate. Unlike single‐junction perovskite solar cells (PSCs), the efficacy of tandem cells is contingent upon the performance of both the top and bottom cells. In this study, we employed a simultaneous co‐modification strategy to incorporate phenylethylammonium iodide (PEAI) at both the top and bottom interfaces of the perovskite film, aiming to boost the top cell's performance. Both experimental and theoretical findings indicate that PEAI not only elevates the perovskite film quality through chemical interactions but also mitigates nonradiative recombination within the device. Consequently, the efficiency of the wide‐bandgap (1.77 eV) PSCs based on nickel oxide (NiO_x) attained a level of 16.5%. Simultaneously, the all‐perovskite tandem solar cells achieved an efficiency of 26.81% and demonstrated superior stability.

Carbazole-based self-assembled monolayers have received considerable attention as hole-selective layers (HSLs) in inverted perovskite solar cells. As an HSL, the electron-blocking capability is important and directly related to electron affinity (EA). Low-energy inverse photoelectron spectroscopy (LEIPS) is the most reliable method for EA measurement. However, the intense electron-impact-induced fluorescence from carbazole interferes with their measurement. By improving the photon detector, we were able to measure 2PACz and MeO-2PACz LEIPS spectra and determine their respective EAs of 1.72 and 1.48 eV. These small EA values ensure effective electron-blocking capability of HSLs regardless of the type of perovskite layer.

Abstract

Nowadays, the extensively used lead sulfide (PbS) quantum dot (QD) hole transport layer (HTL) relies on layer‐by‐layer method to replace long chain oleic acid (OA) ligands with short 1,2‐ethanedithiol (EDT) ligands for preparation. However, the inevitable significant volume shrinkage caused by this traditional method will result in undesired cracks and disordered QD arrangement in the film, along with adverse increased defect density and inhomogeneous energy landscape. To solve the problem, a novel method for EDT passivated PbS QD (PbS‐EDT) HTL preparation using small‐sized benzoic acid (BA) as intermediate ligands is proposed in this work. BA is substituted for OA ligands in solution followed by ligand exchange with EDT layer by layer. With the new method, smoother PbS‐EDT films with more ordered and closer QD packing are gained. It is demonstrated stronger coupling between QDs and reduced defects in the QD HTL owing to the intermediate BA ligand exchange. As a result, the suppressed nonradiative recombination and enhanced carrier mobility are achieved, contributing to ≈20% growth in short circuit current density (J_sc) and a 23.4% higher power conversion efficiency (PCE) of 13.2%. This work provides a general framework for layer‐by‐layer QD film manufacturing optimization.