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Luminescent Colloidal InSb Quantum Dots from in Situ-Generated Single-Source Precursor

Authors :
De Mello Donega, Celso
Busatto, Serena
De Ruiter, Mariska
Jastrzebski, Johann T.B.H.
Albrecht, Wiebke
Pinchetti, Valerio
Brovelli, Sergio
Bals, Sara
Moret, Marc Etienne
Sub Condensed Matter and Interfaces
Sub Physical and Colloid Chemistry
Sub Organic Chemistry and Catalysis
Condensed Matter and Interfaces
Physical and Colloid Chemistry
Organic Chemistry and Catalysis
Busatto, S
de Ruiter, M
TBH Jastrzebski, J
Albrecht, W
Pinchetti, V
Brovelli, S
Bals, S
Moret, M
de Mello Donega, C
Sub Condensed Matter and Interfaces
Sub Physical and Colloid Chemistry
Sub Organic Chemistry and Catalysis
Condensed Matter and Interfaces
Physical and Colloid Chemistry
Organic Chemistry and Catalysis
Source :
ACS Nano, 14(10), 13146. American Chemical Society, ACS Nano, ACS nano
Publication Year :
2020
Publisher :
American Chemical Society, 2020.

Abstract

Despite recent advances, the synthesis of colloidal InSb quantum dots (QDs) remains underdeveloped, mostly due to the lack of suitable precursors. In this work, we use Lewis acid–base interactions between Sb(III) and In(III) species formed at room temperature in situ from commercially available compounds (viz., InCl3, Sb[NMe2]3 and a primary alkylamine) to obtain InSb adduct complexes. These complexes are successfully used as precursors for the synthesis of colloidal InSb QDs ranging from 2.8 to 18.2 nm in diameter by fast coreduction at sufficiently high temperatures (≥230 °C). Our findings allow us to propose a formation mechanism for the QDs synthesized in our work, which is based on a nonclassical nucleation event, followed by aggregative growth. This yields ensembles with multimodal size distributions, which can be fractionated in subensembles with relatively narrow polydispersity by postsynthetic size fractionation. InSb QDs with diameters below 7.0 nm have the zinc blende crystal structure, while ensembles of larger QDs (≥10 nm) consist of a mixture of wurtzite and zinc blende QDs. The QDs exhibit photoluminescence with small Stokes shifts and short radiative lifetimes, implying that the emission is due to band-edge recombination and that the direct nature of the bandgap of bulk InSb is preserved in InSb QDs. Finally, we constructed a sizing curve correlating the peak position of the lowest energy absorption transition with the QD diameters, which shows that the band gap of colloidal InSb QDs increases with size reduction following a 1/d dependence.

Details

Language :
English
ISSN :
19360851
Database :
OpenAIRE
Journal :
ACS Nano, 14(10), 13146. American Chemical Society, ACS Nano, ACS nano
Accession number :
edsair.doi.dedup.....9b7eefc2deb1204c27afc44ae30e87ad