Colloidal
halide perovskite nanocrystals of CsPbCl3 doped
with Yb3+ have demonstrated remarkably high sensitized
photoluminescence quantum yields (PLQYs), approaching 200%, attributed
to a picosecond quantum-cutting process in which one photon absorbed
by the nanocrystal generates two photons emitted by the Yb3+ dopants. This quantum-cutting process is thought to involve a charge-neutral
defect cluster within the nanocrystal’s internal volume. We
demonstrate that Yb3+-doped CsPbCl3 nanocrystals
can be converted postsynthetically to Yb3+-doped CsPb(Cl1–x
Br
x
)3 nanocrystals without compromising the desired high PLQYs.
Nanocrystal energy gaps can be tuned continuously from E
g ≈ 3.06 eV (405 nm) in CsPbCl3 down
to E
g ≈ 2.53 eV (∼490 nm)
in CsPb(Cl0.25Br0.75)3 while retaining
a constant PLQY above 100%. Reducing E
g further causes a rapid drop in PLQY, interpreted as reflecting an
energy threshold for quantum cutting at approximately twice the energy
of the Yb3+
2F7/2 → 2F5/2 absorption threshold. These data demonstrate that
very high quantum-cutting energy efficiencies can be achieved in Yb3+-doped CsPb(Cl1–x
Br
x
)3 nanocrystals, offering the
possibility to circumvent thermalization losses in conventional solar
technologies. The presence of water during anion exchange is found
to have a deleterious effect on the Yb3+ PLQYs but does
not affect the nanocrystal shapes or morphologies, or even reduce
the excitonic PLQYs of analogous undoped CsPb(Cl1–x
Br
x
)3 nanocrystals.
These results provide valuable information relevant to the development
and application of these unique materials for spectral-shifting solar
energy conversion technologies.
We have synthesized unique colloidal nanoplatelets of the ferromagnetic twodimensional (2D) van der Waals material CrI 3 and have characterized these nanoplatelets structurally, magnetically, and by magnetic circular dichroism spectroscopy. The isolated CrI 3 nanoplatelets have lateral dimensions of ~25 nm and ensemble thicknesses of only ~4 nm, corresponding to just a few CrI 3 monolayers. Magnetic and magneto-optical measurements demonstrate robust 2D ferromagnetic ordering in these nanoplatelets with Curie temperatures similar to those observed in bulk CrI 3 , despite the strong spatial confinement. These data also show magnetization steps akin to those observed in micron-sized few-layer 2D sheets and associated with concerted spin-reversal of individual CrI 3 layers within few-layer van der Waals stacks. Similar data have also been obtained for CrBr 3 and anion-alloyed Cr(I 1-x Br x ) 3 nanoplatelets. These results represent the first example of laterally confined 2D van der Waals ferromagnets of any composition. The demonstration of robust ferromagnetism at nanometer lateral dimensions opens new doors for miniaturization in spintronics devices based on van der Waals ferromagnets.
Overcoming the challenges of patterning
luminescent materials will
unlock additive and more sustainable paths for the manufacturing of
next-generation on-chip photonic devices. Electrohydrodynamic (EHD)
inkjet printing is a promising method for deterministically placing
emitters on these photonic devices. However, the use of this technique
to pattern luminescent lead halide perovskite nanocrystals (NCs),
notable for their defect tolerance and impressive optical and spin
coherence properties, for integration with optoelectronic devices
remains unexplored. In this work, we additively deposit nanoscale
CsPbBr3 NC features on photonic structures via EHD inkjet
printing. We perform transmission electron microscopy of EHD inkjet
printed NCs to demonstrate that the NCs’ structural integrity
is maintained throughout the printing process. Finally, NCs are deposited
with sub-micrometer control on an array of parallel silicon nitride
nanophotonic cavities and demonstrate cavity–emitter coupling
via photoluminescence spectroscopy. These results demonstrate EHD
inkjet printing as a scalable, precise method to pattern luminescent
nanomaterials for photonic applications.
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