InAs-based Quantum Dots Prepared with Aminoarsine: Synthesis, Optical Properties and Implementation in LEDs
Dongxu Zhu a, Manuela De Franco b, Houman Bahmani Jalali a b, Francesco Di Stasio b, Luca De Trizio a, Liberato Manna a
a Department of Nanochemistry, Istituto Italiano di Tecnologia, Via Morego 30, 16163 Genova, Italy.
b Photonic Nanomaterials group, Istituto Italiano di Tecnologia, Via Morego 30, 16163 Genova, Italy
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
#NCFun23 - Fundamental Processes in Nanocrystals and 2D Materials
VALÈNCIA, Spain, 2023 March 6th - 10th
Organizers: Valerio Pinchetti and Shalini Singh
Poster, Dongxu Zhu, 305
Publication date: 22nd December 2022

InAs quantum dots (QDs) are characterized by absorption and photoluminescence (PL) in the near-infrared (NIR) region of the electromagnetic spectrum and they are RoHS-compliant (European Union’s “Restriction of Hazardous Substances” directives).1 For these reasons InAs QDs are promising candidates for NIR-related applications ranging from photovoltaics, lasing and light-emitting diodes (LEDs). The most developed synthesis approach to InAs QDs is based on tris-trimethylsilyl (or tris-trimethylgermil) arsine precursor (TMS-As/TMGe-As). Such As precursors are toxic, highly pyrophoric and not commercially available, therefore being not ideal for a large-scale production of InAs QDs. Recently, the search for alternative less toxic and commercially available precursors spotted tris(dimethylamino)arsine (amino-As) as a promising As precursor, renewing the research interest InAs QDs. Currently, InAs QCs obtained with amine-As need to be improved in terms of size distribution and optical properties to reach the standards achieved with TMS-As/TMGe-As precursors. In this regard, we employed ZnCl2 as an additive in the amino-As-based synthesis of InAs QDs and studied the corresponding effects.2 We found that ZnCl2 can bind the surface of InAs QDs behaving as a Z-type ligand, improving their PL quantum yield (QY) and the control over their size distribution. Furthermore, the presence of ZnCl2 on the QDs’ surface and in the raw reaction solution allows for the in-situ growth of a ZnSe shell via a simple injection of the Se precursor. Under our reaction conditions, we obtained InAs@ZnSe core@shell QDs having a ZnSe shell thickness of ~2ML, which show a PL emission centered at ~860 nm with a PLQY as high as 42±4%. Because the lattice mismatch between InAs and ZnSe is around 6%, and this high value usually leads to strained core@shell structure and decreases the PLQY. In our peculiar in-situ growth condition, an intermediate In-Zn-Se layer between InAs core and ZnSe shell is formed, and it helps to reduce the lattice strain and lead to a high PLQY. Given the high PLQY of these QDs, they were employed for the fabrication of NIR LEDs. Obtained NIR LEDs featured an external quantum efficiency (EQE) of 5.5% at 947 nm and an operational lifetime of ∼32 h before reaching 50% of their initial luminance.3 The research results presented here are only a starting point to improve the synthesis of InAs-based QDs with amino-As with outstanding optical properties, and develop the more efficient NIR LEDs.

We acknowledge support from the Project IEMAP - Italian Research Program "Mission Innovation" (agreement 21A033302 GU n. 133/5-6-2021), European Research Council via the ERC-StG “NANOLED” (Grant 851794) and European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie project “INFLED” (Grant 101024823).

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