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Interface polarization in heterovalent core–shell nanocrystals

Nature Materials volume 21, pages 246–252 (2022)Cite this article

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Abstract

The potential profile and the energy level offset of core–shell heterostructured nanocrystals (h-NCs) determine the photophysical properties and the charge transport characteristics of h-NC solids. However, limited material choices for heavy metal-free III-V–II-VI h-NCs pose challenges in comprehensive control of the potential profile. Herein, we present an approach to such a control by steering dipole densities at the interface of III-V–II-VI h-NCs. The controllable heterovalency at the interface is responsible for interfacial dipole densities that result in the vacuum-level shift, providing an additional knob for the control of optical and electrical characteristics of h-NCs. The synthesis of h-NCs with atomic precision allows us to correlate interfacial dipole moments with the NCs’ photochemical stability and optoelectronic performance.

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Fig. 1: Formation of bond dipoles at the InP–ZnSe interface and their impact on the potential profile of h-NCs.
Fig. 2: Electronic and photophysical characteristics of InP–ZnSe h-NCs for various In:P ratios (that is, for varying interfacial dipole densities, ρ).
Fig. 3: Universal polarization effect at the interface on electronic and optical characteristics of III-V–II-VI h-NCs.
Fig. 4: Impact of the interfacial polarization on transport characteristics of charge carriers across InP–ZnSe heterovalent h-NCs.

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Data availability

The authors declare that all data supporting this work are contained in graphics displayed in the main text or in supplementary information. Numerical data for figures are available in this repository: Jeong et al., Interface polarization in heterovalent core/shell NCs (Materials Cloud Archive 2021.X, 2021); https://doi.org/10.24435/materialscloud:xk-xk. Source data are provided with this paper. Additional information is available from the corresponding authors on request.

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Acknowledgements

We thank S.M. Park and S. Jeong for the synthesis and characterization of InAs NCs. This was supported by the National Research Foundation of Korea (NRF) grant funded by the Ministry of Science, ICT, and Future Planning (nos. 2020R1A2C2011478, 2021M3H4A3A01062964, 2020M3D1A2101319 and 2021M3H4A1A01004332), and Electronics and Telecommunications Research Institute (ETRI) grant funded by the Korean government (no. 20ZB1200, Development of ICT Materials, Components and Equipment Technologies). This research was also supported by Samsung Display.

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Author notes

  1. These authors contributed equally: Byeong Guk Jeong, Jun Hyuk Chang, Donghyo Hahm.

Authors and Affiliations

  1. SKKU Advanced Institute of Nano Technology and Department of Nano Engineering, Sungkyunkwan University, Suwon, Republic of Korea

    Byeong Guk Jeong, Jun Hyuk Chang, Donghyo Hahm, Seunghyun Rhee, Youngdu Kim, Doyoon Shin, Jeong Woo Park, Euyheon Hwang & Wan Ki Bae

  2. Samsung Display Research Center, Samsung Display, Yongin, Republic of Korea

    Myeongjin Park, Sooho Lee & Changhee Lee

  3. Department of Chemical and Biomolecular Engineering, KAIST Institute for the Nanocentury, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, Republic of Korea

    Doh C. Lee

  4. Display Research Center, Korea Electronics Technology Institute (KETI), Seongnam, Republic of Korea

    Kyoungwon Park

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Contributions

B.G.J., J.H.C., D.H., S.R., D.C.L., K.P., E.H. and W.K.B. conceived the original idea and designed the experiments. B.G.J., J.H.C., D.H., D.S. and J.W.P. conducted synthesis and characterization of NCs and analysed the experimental data. J.H.C., Y.K., K.P. and E.H. carried out the computational calculation. S.R., S.L., M.P. and C.L. fabricated all devices and analysed the data. All authors contributed to the preparation of the paper.

Corresponding authors

Correspondence to Doh C. Lee, Euyheon Hwang or Wan Ki Bae.

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Supplementary Information

Supplementary Notes 1–8, Figs. 1–23 and Tables 1–7.

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Numerical source data for Fig. 1b.

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Numerical source data for Fig. 2a,c–e.

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Numerical source data for Fig. 3b,c.

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Numerical source data for Fig. 4a,b,e.

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Jeong, B.G., Chang, J.H., Hahm, D. et al. Interface polarization in heterovalent core–shell nanocrystals. Nat. Mater. 21, 246–252 (2022). https://doi.org/10.1038/s41563-021-01119-8

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