Extraction and utilization of hot carriers are considered viable approaches to surpass the Shockley–Queisser limit of perovskite solar cells (PSCs). Here, we introduce N,N′-bis(4-trifluoromethoxybenzyl) naphthalene-1,4,5,8-tetracarboxylic acid diimide (denoted as NDI-BOCF3) to modify the buried SnO2/perovskite interface, simultaneously accelerating hot-electron extraction and passivating interfacial defects. The NDI-BOCF3-modified SnO2 (denoted as SnO2–NDI-BOCF3) exhibits improved surface uniformity and optimized energy-level alignment and passivates oxygen vacancies (VO), thereby providing ∼22% enhancement in hot-electron extraction. Nonadiabatic molecular dynamics simulations confirmed that NDI-BOCF3 enhances hot-electron extraction via higher-frequency lattice vibrations and more ordered nonadiabatic couplings at the interface. In addition, NDI-BOCF3 passivates multisite defects across various perovskite terminations. As a result, SnO2–NDI-BOCF3 devices achieve a power conversion efficiency (PCE) of 25.06%, compared to 23.96% for a device with pristine SnO2. An increase of PCE from 8.81 to 17.50% for SnO2-free devices is also achieved. Furthermore, due to passivation, the activation barrier for positively charged iodine vacancies (VI+) increases from 0.80 to 0.87 eV, resulting in an enhancement in the thermal and photostability of the perovskite thin films.
Xu et al. (Tue,) studied this question.