Heterojunction Perovskite Solar Cells: Opto-Electro-Thermal Physics, Modeling, and Experiment.

Organic-inorganic heterojunction perovskite solar cell (PSC) is promising for low-cost and high-performance photovoltaics. To further promote the performance of PSCs, understanding and controlling the underneath photoconversion mechanisms are highly necessary. Here, we present a comprehensive opto-electro-thermal (OET) study on the heterojunction PSCs by quantitatively addressing the coupled optical, carrier transport and thermodynamic behaviors within the device. With achieving a well agreement with the experiment, we theoretically explore the thermodynamic mechanisms involving the energy conversions and focus especially on the origins of the various energy losses in PSCs. We summarize six categories of microscopic heat conversion processes in the heterojunction PSC, where the Joule and Peltier heats can be defined as the intrinsic losses in PSCs. Moreover, we also discuss the possible manipulation methods to decrease the energy losses, e.g., by tailoring the doping concentration and energy-level alignment. An exemplified OET optimization is also presented, which predicts that the PCE of the fabricated PSC can be enhanced from 21.37% to 23.84%.