Solution-processed
lead sulfide quantum dots (PbS QDs) are very
attractive as NIR-active semiconductors for the fabrication of cost-efficient
optoelectronic devices. To control the thin film carrier transport,
as well as stability, surface passivation is of crucial importance.
Here, we present the successful surface passivation of PbS QDs by
the formamidinium lead iodide (FAPbI3) ligand. An effective
procedure for the fabrication of FAPbI3-passivated PbS
QDs through a binary-phase ligand exchange protocol in hexane and n-methylformamide is demonstrated. It is shown that this
solution-processed ligand exchange drastically changes the photoluminescence
intensity, exciton recombination dynamics, and carrier lifetime of
the nanocrystals. The solution casting of the ligand-exchanged nanocrystals
into thin films results in the periodic ordering of QDs in a square
superlattice with close contacts. Planar graphene/QD photodetectors
fabricated with PbS QDs passivated with FAPbI3 show substantially
increased thermal stability as compared to similar devices using PbS
QDs passivated with commonly used methylammonium lead iodide.
Metal
halide perovskite nanoparticles have recently attracted immense
interest for photodetectors due to their outstanding optical and electronic
properties such as high carrier diffusion length, tunable band gap
(light absorption range), and high photoluminescence (PL) efficiency.
Although significant progress has been achieved in the development
of perovskites, their stability is yet to be addressed. To improve
the stability and quantum efficiency of FAPbI3 perovskite
nanocrystals, we present a room temperature protocol to fabricate
fully passivated and stable FAPbI3 nanocrystals via 2D
growth in the presence of amine ligands and an excess amount of the
organic cations. The crystallization mechanism of 2D colloidal quantum
wells (QWs) with long-time stability is ascribed to the excess amount
of large organic cations which isolate the inorganic lattice octahedral
layers. It is demonstrated that the QW films (130 nm) hold 90% of
their PL intensity after 30 days, which is ∼8 times more stable
than FAPbI3 quantum dot (QD) films. We also show the enhanced
photoresponsivity of QW photodetectors (up to 100%) as compared with
QD devices. The long-term ambient performance of perovskite QW photodetectors
on account of their hydrophobicity is demonstrated. The findings can
shed light on a way to develop ambient stable QW nanoparticle perovskite
optoelectronic devices.
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