4.8 Article

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

Journal

ACS NANO
Volume 14, Issue 10, Pages 13146-13160

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c04744

Keywords

indium antimonide; colloidal quantum dots; near-infrared emission; semiconductor nanocrystals; single-source precursor; III-V semiconductors

Funding

  1. division of Chemical Sciences (CW) of The Netherlands Organization for Scientific Research (NWO) [TOP.715.016.001]
  2. Marie Sklodowska-Curie actions (MSCA) under the EU's Horizon 2020 program [797153]
  3. European Commission [EUSMI E180900184]
  4. European Research Council (ERC Consolidator Grant) [815128 - REALNANO]
  5. Marie Curie Actions (MSCA) [797153] Funding Source: Marie Curie Actions (MSCA)

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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 lat 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 degrees C). Our findings allow us to propose a formation mechanism for the QDs synthesized in our work, which is based on a nonclassical nucleation l 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 Mende 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 lin 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.

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