InP
based quantum dots (QDs) are coming in a big way as an alternative
to toxic Cd, or Pb based QDs. Unlike many literature reports in this
work, green-yellow-orange-red emitting highly photoluminescent (PLQY
as high as 65%) and photostable InP/ZnSeS core/alloy shell quantum
dots (CAS QDs) have been synthesized using a less toxic, air-stable
aminophosphine precursor (P(DMA)3). Unlike literature predictions
in this paper, we show that green-yellow-orange-red emitting InP based
alloyed QDs can be prepared with InCl3 only. We report
here the hitherto unobserved and quite interesting excitation wavelength
dependent PLQY for all of these green-yellow-orange-red emitting InP
based CAS QDs. PLQY increases monotonically with increasing excitation
wavelength. Significant deviation of the PL excitation spectrum from
the absorption spectrum has been observed in the shorter wavelength
region. This observation is perhaps because the surface mediated nonradiative
pathways predominate over radiative charge carrier recombination when
excited at shorter wavelength. PL decay for these QDs generally follows
a triexponential decay equation with the shortest lifetime of 3–10
ns, the moderate one with a lifetime of 24–30 ns, and the longest
one with a lifetime > 60 ns. Moderate and long lifetimes have been
shown to be associated with two mutually interdependent excited-state
decay channels, and the competition between these two decay channels
dictates the PLQY of these CAS QDs. The moderate lifetime has been
shown to be associated with an electron–hole recombination
process, and the long lifetime is associated with delayed emission
from the band edge due to interaction with the manifold of shallow
traps. Quite interestingly, amplitude of the moderate lifetime (dynamical
property) has been observed to be correlated with the PLQY (spectral
property). PL decay for all of these InP based CAS QDs has been observed
to be excitation wavelength independent. However, PL decay gets slower
with increasing monitoring wavelength. Thus, the presence of shallow
trap states is evidenced. Single particle blinking dynamics of InP
based CAS QDs has been investigated for the first time. We could achieve
the lowest reported magnitude of the m
ON exponent for InP based QDs and the value is 1.19, which speaks about
the much longer On-times or, in other words, superiority of our InP
based CAS QD system in comparison to other reported InP based QDs,
for example, InP core only, or InP/ZnS, InP/ZnSe/ZnS, InP/GaP/ZnS
core/shell or core/shell/shell QD systems.