InP
quantum dots (QDs) are the material of choice for
QD display
applications and have been used as active layers in QD light-emitting
diodes (QDLEDs) with high efficiency and color purity. Optimizing
the color purity of QDs requires understanding mechanisms of spectral
broadening. While ensemble-level broadening can be minimized by synthetic
tuning to yield monodisperse QD sizes, single QD line widths are broadened
by exciton–phonon scattering and fine-structure splitting.
Here, using photon-correlation Fourier spectroscopy, we extract average
single QD line widths of 50 meV at 293 K for red-emitting InP/ZnSe/ZnS
QDs, among the narrowest for colloidal QDs. We measure InP/ZnSe/ZnS
single QD emission line shapes at temperatures between 4 and 293 K
and model the spectra using a modified independent boson model. We
find that inelastic acoustic phonon scattering and fine-structure
splitting are the most prominent broadening mechanisms at low temperatures,
whereas pure dephasing from elastic acoustic phonon scattering is
the primary broadening mechanism at elevated temperatures, and optical
phonon scattering contributes minimally across all temperatures. Conversely
for CdSe/CdS/ZnS QDs, we find that optical phonon scattering is a
larger contributor to the line shape at elevated temperatures, leading
to intrinsically broader single-dot line widths than for InP/ZnSe/ZnS.
We are able to reconcile narrow low-temperature line widths and broad
room-temperature line widths within a self-consistent model that enables
parametrization of line width broadening, for different material classes.
This can be used for the rational design of more spectrally narrow
materials. Our findings reveal that red-emitting InP/ZnSe/ZnS QDs
have intrinsically narrower line widths than typically synthesized
CdSe QDs, suggesting that these materials could be used to realize
QDLEDs with high color purity.
Quantum confined lead halide perovskite nanoplatelets
are anisotropic
materials displaying strongly bound excitons with spectrally pure
photoluminescence. We report the controlled assembly of CsPbBr3 nanoplatelets through varying the evaporation rate of the
dispersion solvent. We confirm the assembly of superlattices in the
face-down and edge-up configurations by electron microscopy, as well
as X-ray scattering and diffraction. Polarization-resolved spectroscopy
shows that superlattices in the edge-up configuration display significantly
polarized emission compared to face-down counterparts. Variable-temperature
X-ray diffraction of both face-down and edge-up superlattices uncovers
a uniaxial negative thermal expansion in ultrathin nanoplatelets,
which reconciles the anomalous temperature dependence of the emission
energy. Additional structural aspects are investigated by multilayer
diffraction fitting, revealing a significant decrease in superlattice
order with decreasing temperature, with a concomitant expansion of
the organic sublattice and increase of lead halide octahedral tilt.
One-dimensional (1D) colloidal lead halide perovskites
(LHPs) have
potential as quantum emitters. Their study, however, has been hampered
by their previous instability, leaving a gap in our understanding
of structure–property relationships in colloidal LHPs with
anisotropic shapes. Here, we synthesize stable, highly-confined 1D
CsPbBr3 nanorods (NRs) and demonstrate their structural
details and photoluminescence (PL) properties at both the ensemble
and single particle levels. Using amino-terminated copolymers, we
are able to stabilize and characterize 1D CsPbBr3 NRs utilizing
transmission electron microscopy (TEM) and small angle scattering
(SAS). Scanning transmission electron microscopy reveals that these
NRs possess structural defects, including twists and inhomogeneity.
Solution-phase photon correlation spectroscopy shows low biexciton-to-exciton
quantum yield ratios (QYBX/QYX) and broad spectral
line widths dominated by homogeneous broadening.
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