Luminescent
solar concentrators (LSCs) show promise because of
their potential for low-cost, large-area, and high-efficiency energy
harvesting. Stokes shift engineering of luminescent quantum dots (QDs)
is a favorable approach to suppress reabsorption losses in LSCs; however,
the use of highly toxic heavy metals in QDs constitutes a serious
concern for environmental sustainability. Here, we report LSCs based
on cadmium-free InP/ZnO core/shell QDs with type-II band alignment
that allow for the suppression of reabsorption by Stokes shift engineering.
The spectral emission and absorption overlap was controlled by the
growth of a ZnO shell on an InP core. At the same time, the ZnO layer
also facilitates the photostability of the QDs within the host matrix.
We analyzed the optical performance of indium-based LSCs and identified
the optical efficiency as 1.45%. The transparency, flexibility, and
cadmium-free content of the LSCs hold promise for solar window applications.
The most developed approaches for the synthesis of InAs nanocrystals (NCs) rely on pyrophoric, toxic, and not readily available tris-trimethylsilyl (or tris-trimethylgermil) arsine precursors. Less toxic and commercially available chemicals, such as tris(dimethylamino)arsine, have recently emerged as alternative As precursors. Nevertheless, InAs NCs made with such compounds need to be further optimized in terms of size distribution and optical properties in order to meet the standard reached with tristrimethylsilyl arsine. To this aim, in this work we investigated the role of ZnCl 2 used as an additive in the synthesis of InAs NCs with tris(dimethylamino)arsine and alane N,N-dimethylethylamine as the reducing agent. We discovered that ZnCl 2 helps not only to improve the size distribution of InAs NCs but also to passivate their surface acting as a Z-type ligand. The presence of ZnCl 2 on the surface of the NCs and the excess of Zn precursor used in the synthesis enable the subsequent in situ growth of a ZnSe shell, which is realized by simply adding the Se precursor to the crude reaction mixture. The resulting InAs@ZnSe core@shell NCs exhibit photoluminescence emission at ∼860 nm with a quantum yield as high as 42±4%, which is a record for such heterostructures, given the relatively high mismatch (6%) between InAs and ZnSe. Such bright emission was ascribed to the formation, under our peculiar reaction conditions, of an In−Zn−Se intermediate layer between the core and the shell, as indicated by X-ray photoelectron spectroscopy and elemental analyses, which helps to release the strain between the two materials.
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