Thermodynamic Processes of Perovskite Photovoltaic Devices: Mechanisms, Simulation, and Manipulation

Abstract

AbstractPerovskite‐based single‐junction and tandem solar cells have recently attracted considerable attention due to their remarkable advantages in power conversion efficiency (PCE) and fabrication cost; however, their commercialization remains challenging. One crucial limiting factor is the incompetent thermal management, which is inclined to degrade the PCE and stability of the device. Here, a rigorous opto–electro–thermal (OET) simulation is performed to disclose the internal energy conversion and heat mechanisms within devices. Taking a low‐bandgap PSC as an example, the microscopic energy conversion processes concerning the contributions from thermalization, Joule, Peltier, and bulk/interface recombination heats are quantitatively identified. Then various thermal manipulation strategies are proposed, including external (cooling effect) and internal (transport layer materials, photoluminescence colorants, and tandem strategy) methods with the purposes of reducing the heat generation and device temperature. Through the joint OET optimization, the predicted temperature of the considered single‐junction (tandem) PSC is reduced to 44.3 °C (33.5 °C) with the possible PCE up to 22.35% (29.08%). Based on the simulation, a tandem PSC (under two‐terminal configuration) is fabricated and a PCE of 25.03% is realized. This study offers an effective approach for energy analysis and manipulation to realize higher‐performance PSCs with lower operation temperatures.