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.