Various phosphonic acid based self-assembled monolayers
(SAMs)
have been commonly used for interface modifications in inverted perovskite
solar cells. This typically results in significant enhancement of
the hole extraction and consequent increase in the power conversion
efficiency. However, the surface coverage and packing density of SAM
molecules can vary, depending on the chosen SAM material and underlying
oxide layer. In addition, different SAM molecules have diverse effects
on the interfacial energy level alignment and perovskite film growth,
resulting in complex relationships between surface modification, efficiency,
and lifetime. Here we show that ethanolamine surface modification
combined with [2-(9H-carbazol-9-yl)ethyl]phosphonic
acid (2PACz) results in significant improvement in device stability
compared to devices with 2PACz modification only. The significantly
smaller size of ethanolamine enables it to fill any gaps in 2PACz
coverage and provide improved interfacial defect passivation, while
its different chemical structure enables it to provide complementary
effects to 2PACz passivation. Consequently, the perovskite films are
more stable under illumination (slower photoinduced segregation),
and the devices exhibit significant stability enhancement. Despite
similar power conversion efficiencies (PCE) between 2PACz only and
combined ethanolamine-2PACz modification (PCE of champion devices
∼21.6–22.0% for rigid and ∼20.2–21.0%
for flexible devices), the T
80 lifetime
under simulated solar illumination in ambient is improved more than
15 times for both rigid and flexible devices.