posted on 2023-11-03, 13:05authored byIssatay Nadinov, Khulud Almasabi, Luis Gutiérrez-Arzaluz, Simil Thomas, Bashir E. Hasanov, Osman M. Bakr, Husam N. Alshareef, Omar F. Mohammed
One of the most effective
approaches to optimizing the performance
of perovskite solar cells is to fully understand the ultrafast carrier
dynamics at the interfaces between absorber and transporting layers
at both the molecular and atomic levels. Here, the injection dynamics
of hot and relaxed charge carriers at the interface between the hybrid
perovskite, formamidinium lead bromide (FAPbBr3), and the
organic electron acceptor, IEICO-4F, are investigated and deciphered
by using femtosecond (fs) mid-infrared (IR), transient absorption
(TA), and fluorescence spectroscopies. The visible femtosecond-TA
measurements reveal the generation of hot carriers and their transition
to free carriers in the pure FAPbBr3 film. Meanwhile, the
efficient extraction of hot carriers in the mixed FAPbBr3/IEICO-4F film is clearly evidenced by the complete disappearance
of their spectral signature. More specifically, the time-resolved
results reveal that hot carriers are injected from FAPbBr3 to IEICO-4F within 150 fs, while the transfer time for the relaxed
carriers is about 205 fs. The time-resolved mid-IR experiments also
demonstrate the ultrafast formation of two peaks at 2115 and 2233
cm–1, which can be attributed to the CN
symmetrical and asymmetrical vibrational modes of anionic IEICO-4F,
thus providing crystal clear evidence for the electron transfer process
between the donor and acceptor units. Moreover, photoluminescence
(PL) lifetime measurements reveal an approximately 10-fold decrease
in the donor lifetime in the presence of IEICO-4F, thereby confirming
the efficient electron injection from the perovskite to the acceptor
unit. In addition, the efficient electron injection at the FAPbBr3/IEICO-4F interface and its impact on the CN bond
character are experimentally evidenced and align with density functional
theory (DFT) calculations. This work offers new insights into the
electron injection process at the FAPbBr3/IEICO-4F interface,
which is crucial for developing efficient optoelectronic devices.