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Understanding the Role of Single Molecular ZnS Precursors in the Synthesis of In(Zn)P/ZnS Nanocrystals

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    Research Article

    Understanding the Role of Single Molecular ZnS Precursors in the Synthesis of In(Zn)P/ZnS Nanocrystals
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    † †Semiconductor Nanoelectronics (PGI-9), §Ernst Ruska-Centre and Peter Grünberg Institut, and ⊥Central Institute for Engineering, Electronics and Analytics (ZEA-3), Forschungszentrum Jülich, 52425 Jülich, Germany
    ‡ Department of Physics, Chonbuk National University, Jeonju 561-756, Republic of Korea
    ∥ School of Materials Science and Engineering, Nanyang Technological University, 639798, Singapore
    # Institute of Materials in Electrical Engineering and Information Technology 2 (IWE2), JARA-FIT, RWTH, Aachen D-52056, Germany
    *E-mail: [email protected]. (Y.M.L.)
    *E-mail: [email protected]. (B.K.)
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2014, 6, 20, 18233–18242
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    https://doi.org/10.1021/am504988j
    Published September 24, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    Environmentally friendly nanocrystals (NCs) such as InP are in demand for various applications, such as biomedical labeling, solar cells, sensors, and light-emitting diodes (LEDs). To fulfill their potential applications, the synthesis of such high-quality “green” InP NCs required further improvement so as to achieve better stability, higher brightness NCs, and also to have a more robust synthesis route. The present study addresses our efforts on the synthesis of high-quality In(Zn)P/ZnS core–shell NCs using an air- and moisture-stable ZnS single molecular precursor (SMP) and In(Zn)P cores. The SMP method has recently emerged as a promising route for the surface overcoating of NCs due to its simplicity, high reproducibility, low reaction temperature, and flexibility in controlling the reaction. The synthesis involved heating the In(Zn)P core solution and Zn(S2CNR2) (where R = methyl, ethyl, butyl, or benzyl and referred to as ZDMT, ZDET, ZDBT, or ZDBzT, respectively) in oleylamine (OLA) to 90–250 °C for 0.5–2.5 h. In this work, we systematically studied the influence of different SMP end groups, the complex formation and stability between the SMP and oleylamine (OLA), the reaction temperature, and the amount of SMP on the synthesis of high-quality In(Zn)P/ZnS NCs. We found that thiocarbamate end groups are an important factor contributing to the low-temperature growth of high-quality In(Zn)P/ZnS NCs, as the end groups affect the polarity of the molecules and result in a different steric arrangement. We found that use of SMP with bulky end groups (ZDBzT) results in nanocrystals with higher photoluminescence quantum yield (PL QY) and better dispersibility than those synthesized with SMPs with the shorter alkyl chain groups (ZDMT, ZDET, or ZDBT). At the optimal conditions, the PL QY of red emission In(Zn)P/ZnS NCs is 55 ± 4%, which is one of the highest values reported. On the basis of structural (XAS, XPS, XRD, TEM) and optical characterization, we propose a mechanism for the growth of a ZnS shell on an In(Zn)P core.

    Copyright © 2014 American Chemical Society

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    Supporting Information

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    Additional tables, PL spectra, power spectrum of an HRTEM image, XRD patterns, XAS spectra, XPS surveys and elemental results, UV–vis spectra, FT-IR spectra, TGA curves, and calculations for shell growth (PDF). This material is available free of charge via the Internet at http://pubs.acs.org.

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    This article is cited by 27 publications.

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    Cite this: ACS Appl. Mater. Interfaces 2014, 6, 20, 18233–18242
    Click to copy citationCitation copied!
    https://doi.org/10.1021/am504988j
    Published September 24, 2014
    Copyright © 2014 American Chemical Society
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