Inorganic perovskite CsPbBr nanocrystals (NCs) are emerging, highly attractive light emitters with high color purity and good thermal stability for light-emitting diodes (LEDs). Their high photo/electroluminescence efficiencies are very important for fabricating efficient LEDs. Here, we propose a novel strategy to enhance the photo/electroluminescence efficiency of CsPbBr NCs through doping of heterovalent Ce ions via a facile hot-injection method. The Ce cation was chosen as the dopant for CsPbBr NCs by virtue of its similar ion radius and formation of higher energy level of conduction band with bromine in comparison with the Pb cation to maintain the integrity of perovskite structure without introducing additional trap states. It was found that by increasing the doping amount of Ce in CsPbBr NCs to 2.88% (atomic percentage of Ce compared to Pb) the photoluminescence quantum yield (PLQY) of CsPbBr NCs reached up to 89%, a factor of 2 increase in comparison with the native, undoped ones. The ultrafast transient absorption and time-resolved photoluminescence (PL) spectroscopy revealed that Ce-doping can significantly modulate the PL kinetics to enhance the PL efficiency of doped CsPbBr NCs. As a result, the LED device fabricated by adopting Ce-doped CsPbBr NCs as the emitting layers exhibited a pronounced improvement of electroluminescence with external quantum efficiency (EQE) from 1.6 to 4.4% via Ce-doping.
Cubic phase CsPbI3 quantum dots (α-CsPbI3 QDs) as a newly emerging
type of semiconducting QDs hold tremendous
promise for fundamental research and optoelectronic device applications.
However, stable and sub-5 nm-sized α-CsPbI3 QDs have
rarely been demonstrated so far due to their highly labile ionic structure
and low phase stability. Here, we report a novel strontium-substitution
along with iodide passivation strategy to stabilize the cubic phase
of CsPbI3, achieving the facile synthesis of α-CsPbI3 QDs with a series of controllable sizes down to sub-5 nm.
We demonstrate that the incorporation of strontium ions can significantly
increase the formation energies of α-CsPbI3 QDs and
hence reduce the structure distortion to stabilize the cubic phase
at the few-nanometer size. The size ranging from 15 down to sub-5
nm of as-prepared stable α-CsPbI3 QDs allowed us
to investigate their unique size-dependent optical properties. Strikingly,
the few-nanometer-sized α-CsPbI3 QDs turned out to
retain high photoluminescence and highly close packing in solid state
thin films, and the fabricated red light emitting diodes exhibited
high brightness (1250 cd m–2 at 9.2 V) and good
operational stability (L50 > 2 h driven by 6 V). The
developed
cation-substitution strategy will provide an alternative method to
prepare uniform and finely size-controlled colloidal lead halide perovskite
QDs for various optoelectronic applications.
A practical strategy is proposed to facilitate the migration of holes in semiconductor (the low rate of which limits photocatalytic efficiency) by taking advantage of the Schottky barrier between p-type semiconductor and metal. A high work function is found to serve as an important selection rule for building such desirable Schottky junction between semiconductor surface facets and metal. The intrinsic charge spatial distribution has to be taken into account when selecting the facets, as it results in accumulation of photoexcited electrons and holes on certain semiconductor facets. Importantly, the facets have a high work function, the same characteristic required for the formation of Schottky junction in a p-type semiconductor-metal hybrid structure. As a result, the semiconductor crystals in the hybrid design may be better enclosed by single facets with high work function, so as to synergize the two effects: Schottky barrier versus charge spatial separation.
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