PEDOT:PSS is widely used as a hole
transport layer (HTL) in perovskite
solar cells (PSCs) due to its facile processability, industrial scalability,
and commercialization potential. However, PSCs utilizing PEDOT:PSS
suffer from strong recombination losses compared to other organic
HTLs. This results in lower open-circuit voltage (
V
OC
) and power conversion efficiency (PCE). Most studies
focus on doping PEDOT:PSS to improve charge extraction, but it has
been suggested that a high doping level can cause strong recombination
losses. Herein, we systematically dedope PEDOT:PSS with aqueous NaOH,
raising its Fermi level by up to 500 meV, and optimize its layer thickness
in p-i-n devices. A significant reduction of recombination losses
at the dedoped PEDOT:PSS/perovskite interface is evidenced by a longer
photoluminescence lifetime and higher magnitude of surface photovoltage,
leading to an increased device
V
OC
, fill
factor, and PCE. These results provide insights into the relationship
between doping level of HTLs and interfacial charge carrier recombination
losses.