Recently a great deal of research on colloidal nanocrystals, so-called quantum dots (QDs), has shown their importance as a wavelength converter for solid-state lighting devices, due to the nanometer-sized particles' lack of optical scattering, excellent luminescence characteristics, and solution-based synthesis process. More specifically, it is also confirmed that layer by layer assembled QDs with a sequential stacking of green emitter on top of red emitter is highly desirable for efficient white-light generation when it comes to a wavelength converter for blue light-emitting diodes (LEDs). For example, S. Nizamoglu et al. reported that by stacking cyan/yellow/red nanocrystals-embedded polymer films on top of LEDs as a remote-type wavelength converter, re-absorption between the nanocrystals is reduced. In order to form a layer structured QDs-embedding film, the selfsegregation of luminophore guests in one host polymer is expected to be more desirable than physically contacting two luminophore layers, since there is no polymer-air-polymer inter-boundaries, and consequently, less light scattering and reflection. It is successfully demonstrated by V. Bulovic’s group that they could control the phase-segregation of a QDs upper layer from a QDs/polymer composite by using solvent evaporation during spin-coating, and they suggested application of this method be focused on an electroluminescence device. However, up until now there is no report on the formation of a self-segregated QDs upper-layer with a luminescent molecule-embedded polymer bottom layer, although it could be considered as an optimum structure for a film-type wavelength converter. Here, we report that by engineering the surface free energy of QDs and host film mixed with organic dye, an amorphous polymer film can be layer-type phase-segregated by thermal annealing, as shown in Scheme I. It is confirmed that the increase of concentration of the small molecule occurs in the bottom layer. Eventually, a double layer with green and red emission in separated layers is formed and the photoluminescence (PL) intensity of the film is increased after annealing. To our knowledge, this is the first report showing that a green and red wavelength-converting film can be fabricated with this desirable layer structure by a simple self-segregation method. Analysis was mainly focused on characterizing the structural and PL evolution of the film.
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