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Nano Research 2023, 16(1): 1576-1585 https://doi.org/10.1007/s12274-022-4784-6
Research Article | Issue | Published: 27 August 2022

Enabling ultranarrow blue emission linewidths in colloidal alloy quantum dots by decreasing the exciton fine structure splitting and exciton–phonon coupling

Show Author's Information Jinke Bai1,  Linfeng Wang1,  Tingting Zhang2,  Tianyi Hou2,  Meilun Zhang2,  Bing Xu2,  Dongyu Li2,  Xiao Jin2( ),  Qinghua Li2,  Yuxiao Wang1,  Xueru Zhang1,  Yinglin Song1( )
Department of Physics, Harbin Institute of Technology, Harbin 150001, China
Guangdong Provincial Key Laboratory of Development and Education for Special Needs Children, Lingnan Normal University, Zhanjiang 524048, China
Keywords:
alloy quantum dots, spectral linewidth, light-heavy hole splitting, exciton–phonon coupling, homogeneous broadening
Topics:
Core shell nanoparticlesNanoparticlesSemiconductor quantum dots
Cite this article:
Bai J, Wang L, Zhang T, et al. Enabling ultranarrow blue emission linewidths in colloidal alloy quantum dots by decreasing the exciton fine structure splitting and exciton–phonon coupling. Nano Research, 2023, 16(1): 1576-1585. https://doi.org/10.1007/s12274-022-4784-6
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Abstract Full text Electronic supplementary material About this article

The realization of colloidal alloy quantum dots (QDs) with narrow spectral linewidths requires minimization of the contributions of inhomogeneous and homogeneous broadening to the ensemble spectrum. Recently, there has been remarkable progress in eliminating the inhomogeneous contribution by controlling the size distribution of the QDs. However, considerable challenges remain in suppressing the homogeneous broadening, in terms of both intrinsic principles and rational synthetic routes. We find that ground-state exciton fine structure splitting and exciton–phonon coupling play a pivotal role in the homogeneous broadening mechanism. Here we demonstrate that the elimination of the lattice mismatch strain by using a coherent strain structure can decrease the light-heavy hole splitting, thus suppressing the asymmetric broadening of the emission on the high energy side. Besides, the improvement of the uniformity of the alloy by using a stepwise ion exchange strategy can weaken the exciton–longitudinal optical (LO)-phonon interactions, further minimizing the homogeneous broadening. As a result, the final alloy QD products exhibit a widely tunable blue emission wavelength (445–470 nm) with the narrowest ensemble photoluminescence full width at half maximum (FWHM) of 10.1–13.5 nm (or 58.4–75.3 meV). Our study provides a potential strategy for other semiconductor nanocrystals with ultranarrow spectral linewidths.


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Electronic supplementary material
About this article

Enabling ultranarrow blue emission linewidths in colloidal alloy quantum dots by decreasing the exciton fine structure splitting and exciton–phonon coupling

Show Author's information Jinke Bai1, Linfeng Wang1, Tingting Zhang2, Tianyi Hou2, Meilun Zhang2, Bing Xu2, Dongyu Li2, Xiao Jin2( ), Qinghua Li2, Yuxiao Wang1, Xueru Zhang1, Yinglin Song1( )
Department of Physics, Harbin Institute of Technology, Harbin 150001, China
Guangdong Provincial Key Laboratory of Development and Education for Special Needs Children, Lingnan Normal University, Zhanjiang 524048, China

Abstract

The realization of colloidal alloy quantum dots (QDs) with narrow spectral linewidths requires minimization of the contributions of inhomogeneous and homogeneous broadening to the ensemble spectrum. Recently, there has been remarkable progress in eliminating the inhomogeneous contribution by controlling the size distribution of the QDs. However, considerable challenges remain in suppressing the homogeneous broadening, in terms of both intrinsic principles and rational synthetic routes. We find that ground-state exciton fine structure splitting and exciton–phonon coupling play a pivotal role in the homogeneous broadening mechanism. Here we demonstrate that the elimination of the lattice mismatch strain by using a coherent strain structure can decrease the light-heavy hole splitting, thus suppressing the asymmetric broadening of the emission on the high energy side. Besides, the improvement of the uniformity of the alloy by using a stepwise ion exchange strategy can weaken the exciton–longitudinal optical (LO)-phonon interactions, further minimizing the homogeneous broadening. As a result, the final alloy QD products exhibit a widely tunable blue emission wavelength (445–470 nm) with the narrowest ensemble photoluminescence full width at half maximum (FWHM) of 10.1–13.5 nm (or 58.4–75.3 meV). Our study provides a potential strategy for other semiconductor nanocrystals with ultranarrow spectral linewidths.

Keywords: alloy quantum dots, spectral linewidth, light-heavy hole splitting, exciton–phonon coupling, homogeneous broadening

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Publication history
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Acknowledgements

Publication history

Received: 05 May 2022
Revised: 24 June 2022
Accepted: 18 July 2022
Published: 27 August 2022
Issue date: January 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We gratefully acknowledge the financial support of the Natural Science Foundation of China (No. 12174169), the Natural Science Foundation of Guangdong Province (Nos. 2021A1515012292 and 2022A1515012448), the Scientific Research Foundation of the Higher Education Institutions of Guangdong Province (Nos. 2019KCXTD012, 2020ZDZX3034, 2019KZDZX2008, and 2020ZDZX2055), the Natural Science Foundation of Jiangxi Province (Nos. 20192ACBL21045 and 20181BBE50022), the Talent Project of Lingnan Normal University (Nos. ZL2021029 and ZL2021030), the Science and Technology Plan Project of Zhanjiang (Nos. 2020B01085, 2021A05233, 2020A03003, and 2021A05042), the Young Innovative Talents Project of University of Guangdong Province (No. 2018KQNCX153), and the Yanling Outstanding Yong Teacher Training Program Funded Project of Lingnan Normal University (No. YL20200102).

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