Metal halide perovskite
nanocrystals offer a range of interesting
properties and are being studied extensively for applications in solar
cells, photodetectors and light-emitting devices. This perspective
provides a number of best practices for the synthesis, purification,
and characterization of metal halide perovskite nanocrystals, with
detailed discussion of CsPbI3, CsPbBr3, CH3NH3PbI3 (MAPI), and Cs2AgBiBr6 as examples. The choice of reactants and ligands for hot-injection
reactions are discussed, as well as how various reaction conditions,
including temperature and time, affect yield, uniformity, and crystal
phase. We extensively discuss the use of antisolvent precipitation
methods for purification, since ligand coordination to most perovskite
nanocrystals is weak and the nanocrystals are sensitive to degradation.
Finally, we discuss some of the strategies for imaging these nanocrystals
using transmission electron microscopy (TEM).
We
report a detailed study on APbX3 (A = formamidinium
(FA+), Cs+; X = I–, Br–) perovskite quantum dots (PQDs) with combined A- and
X-site alloying that exhibits both a wide bandgap and high open-circuit
voltage (V
oc) for the application of a
potential top cell in tandem junction photovoltaic (PV) devices. The
nanocrystal alloying affords control over the optical bandgap and
is readily achieved by solution-phase cation and anion exchange between
previously synthesized FAPbI3 and CsPbBr3 PQDs.
Increasing only the Br– content of the PQDs widens
the bandgap but results in shorter carrier lifetimes and associated V
oc losses in devices. These deleterious effects
can be mitigated by replacing Cs+ with FA+,
resulting in wide-bandgap PQD absorbers with improved charge-carrier
mobility and PVs with higher V
oc. Although
further device optimization is required, these results demonstrate
the potential of FA1–x
Cs
x
Pb(I1–x
Br
x
)3 PQDs for wide-bandgap perovskite
PVs with high V
oc.
Halide perovskites have the potential
to disrupt the photovoltaics
market based on their high performance and low cost. However, the
decomposition of perovskites under moisture, oxygen, and light raises
concerns about service lifetime, especially because degradation mechanisms
and the corresponding rate laws that fit the observed data have thus
far eluded researchers. Here, we report a water-accelerated photooxidation
mechanism dominating the degradation kinetics of archetypal perovskite
CH3NH3PbI3 in air under >1% relative
humidity at 25 °C. From this mechanism, we develop a kinetic
model that quantitatively predicts the degradation rate as a function
of temperature, ambient O2 and H2O levels, and
illumination. Because water is a possible product of dry photooxidation,
these results highlight the
need for encapsulation schemes that rigorously block oxygen ingress,
as product water may accumulate beneath the encapsulant and initiate
the more rapid water-accelerated photooxidative decomposition.
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