The
minimum interface recombination and maximum carrier extraction
of perovskite solar cells (PSCs) are important for achieving a better
power conversion efficiency (PCE). According to the recent investigations,
3D/2D hybrid perovskite systems have been recognized as an effective
approach to improve the efficiency and stability of PSCs. However,
a large highest occupied molecular orbital energy level gap between
a 2D perovskite and the hole transport layer (HTL) spiro-OMeTAD would
cause energy losses at the interface, which limit open-circuit voltage
(V
oc) and thus PCE of the PSCs. In this
work, we utilized a thermally activated delayed fluorescence molecule
M1 stacked on the 3D/2D hybrid perovskite films to engineer the 3D/2D
perovskite/HTL interface. The ultrathin interfacial layer of M1 forms
a cascade energy alignment between 3D/2D perovskites and a HTL, as
a means to circumvent energy losses, which consequently improves the
efficiency of PSCs from 19.56 to 21.48% with an outstanding increase
of V
oc from 1.18 to 1.23 V. The charge
separation and carrier recombination in PSCs were analyzed by photoluminescence
and impedance characterization, from which, we deduce that a suitable
energy level structure can reduce interface charge recombination and
promote a minimal open-circuit voltage (V
oc) loss, which facilitate the improvement of PSC performances.