Proceedings of nanoGe September Meeting 2015 (NFM15)
Publication date: 8th June 2015
Colloidal nanocrystals (NCs) of ternary semiconductors such as CuInX2 (X = S, Se and Te) are widely investigated as alternative for heavy-metal based NCs (CdX and PbX) due to their comparable optoelectronic properties that can be tuned from the visible to the near-infrared (NIR) by controlling the size and composition of the NC [1]. This makes them promising materials for several applications [1]. A major drawback of these ternary NCs is that their synthesis does not yet offer the same degree of freedom as that currently available for their Cd- and Pb-based counterparts. As a result, the size and shape control of ternary NCs is still limited, and only luminescent quasi-spherical CuInX2 NCs [2] and non-luminescent CuInS2 (CIS) nanorods (NRs) [3] have been reported.
Nanoscale cation exchange reactions have emerged as a promising alternative for direct synthesis protocols, since they allow post-synthetic control over the composition, while preserving the NC size and shape. This makes it possible to synthesize NCs that would otherwise not be attainable. Copper-based NCs are commonly used in cation exchange reactions, due to the easy exchangeability of Cu+ [4]. Recently, we have obtained luminescent CuInS2 NCs from parent Cu2-xS NCs by making use of self-limited partial In3+ for Cu+ exchange [4].
In this work, we further extend this strategy to the preparation of novel ternary core/shell NCs with unprecedented size, shape and composition control. To this end, we exploited the synthetic versatility of core/shell CdSe/CdS nanocrystals (NRs and spherical NCs) in combination with sequential cation exchange reactions (Cd2+ for Cu+ full exchange followed by Cu+ for In3+ partial exchange). This yielded ternary CuInSe2/CuInS2 (CISe/CIS) concentric core/shell NCs and dot core/rod shell nanorods with efficient photoluminescence in the near-infrared (NIR) around 1.0 eV. High Resolution Transmission Electron Microscopy (HRTEM) and tomographic reconstructions show that the core/shell structure of the parent NCs is preserved and that wurtzite CISe/CIS NRs are obtained.
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