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

[Image: see text] 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 commercia...

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Autores principales: Busatto, Serena, Ruiter, Mariska de, Jastrzebski, Johann T. B. H., Albrecht, Wiebke, Pinchetti, Valerio, Brovelli, Sergio, Bals, Sara, Moret, Marc-Etienne, de Mello Donega, Celso
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7596776/
https://www.ncbi.nlm.nih.gov/pubmed/32915541
http://dx.doi.org/10.1021/acsnano.0c04744
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author Busatto, Serena
Ruiter, Mariska de
Jastrzebski, Johann T. B. H.
Albrecht, Wiebke
Pinchetti, Valerio
Brovelli, Sergio
Bals, Sara
Moret, Marc-Etienne
de Mello Donega, Celso
author_facet Busatto, Serena
Ruiter, Mariska de
Jastrzebski, Johann T. B. H.
Albrecht, Wiebke
Pinchetti, Valerio
Brovelli, Sergio
Bals, Sara
Moret, Marc-Etienne
de Mello Donega, Celso
author_sort Busatto, Serena
collection PubMed
description [Image: see text] 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., InCl(3), Sb[NMe(2)](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.
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spelling pubmed-75967762020-10-30 Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor Busatto, Serena Ruiter, Mariska de Jastrzebski, Johann T. B. H. Albrecht, Wiebke Pinchetti, Valerio Brovelli, Sergio Bals, Sara Moret, Marc-Etienne de Mello Donega, Celso ACS Nano [Image: see text] 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., InCl(3), Sb[NMe(2)](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. American Chemical Society 2020-09-11 2020-10-27 /pmc/articles/PMC7596776/ /pubmed/32915541 http://dx.doi.org/10.1021/acsnano.0c04744 Text en This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Busatto, Serena
Ruiter, Mariska de
Jastrzebski, Johann T. B. H.
Albrecht, Wiebke
Pinchetti, Valerio
Brovelli, Sergio
Bals, Sara
Moret, Marc-Etienne
de Mello Donega, Celso
Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title_full Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title_fullStr Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title_full_unstemmed Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title_short Luminescent Colloidal InSb Quantum Dots from In Situ Generated Single-Source Precursor
title_sort luminescent colloidal insb quantum dots from in situ generated single-source precursor
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7596776/
https://www.ncbi.nlm.nih.gov/pubmed/32915541
http://dx.doi.org/10.1021/acsnano.0c04744
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