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<p>Amino-functionalized graphene quantum dots (af-GQDs) have been studied recently as luminescent materials. However, they exhibit poor PL quantum yield (PLQY), which is circumvented by heteroatom doping. Doping induces graphene-related edge defects (zigzag and armchair), offering favorable recombination centers for PL tuning. Additionally, the carbon network with attached functional groups (such as the amino (NH₂) group) offers a flexible coating on the core regardless of lattice mismatch. Herein, we introduced a novel strategy of employing heteroatom (S, N, B)-doped af-GQDs as a soft shell around a ZnSe core to modify the electron density (ED) and edge defects (zigzag and armchair). In contrast to our previous ZnSe/af-GQDs report, this strategy enables the heteroatom-induced controlled defect engineering, resulting in multicolor photoluminescence (PL) emission ranging from 458 to 750&#xa0;nm. Temperature-dependent photoluminescence (TDPL) spectroscopy was employed to study the charge recombination within the temperature range 80–300&#xa0;K. The TDPL analysis revealed the presence of active recombination centers participating in PL emission tuning. We achieved PL quantum yield (PLQY) up to 86% for S-doped core/shell QDs with dominant zigzag defects, which is higher than previously reported ZnSe/af-GQDs (PLQY ~ 83%). Heteroatoms not only altered the electron density (ED) of the af-GQDs but also tuned graphene-related edge defects (zigzag and armchair). The color chromaticity coordinates are positioned in the yellow-orange-red region on the Commission Internationale de l’éclairage (CIE) 1931 color space, demonstrating the strong color perception modulation and multicomponent color emission from a single emissive layer (SEL) ZnSe/af-XGQDs (S, N, B). This low-cost, nontoxic, and facile approach provides a platform for the realization of future SEL for white light-emitting diodes (LEDs) and display devices.</p>

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Temperature-dependent photoluminescence of heteroatom-doped edge tuned amino-functionalized GQDs nanoshells conjugated with ZnSe QDs

  • 期刊论文

  • 发表日期：

    2025年10月27日

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  • Faiza Mustafa,
  • Samia Aslam,
  • M. Ashfaq Ahmad,
  • Junaid Ali

摘要

Amino-functionalized graphene quantum dots (af-GQDs) have been studied recently as luminescent materials. However, they exhibit poor PL quantum yield (PLQY), which is circumvented by heteroatom doping. Doping induces graphene-related edge defects (zigzag and armchair), offering favorable recombination centers for PL tuning. Additionally, the carbon network with attached functional groups (such as the amino (NH₂) group) offers a flexible coating on the core regardless of lattice mismatch. Herein, we introduced a novel strategy of employing heteroatom (S, N, B)-doped af-GQDs as a soft shell around a ZnSe core to modify the electron density (ED) and edge defects (zigzag and armchair). In contrast to our previous ZnSe/af-GQDs report, this strategy enables the heteroatom-induced controlled defect engineering, resulting in multicolor photoluminescence (PL) emission ranging from 458 to 750 nm. Temperature-dependent photoluminescence (TDPL) spectroscopy was employed to study the charge recombination within the temperature range 80–300 K. The TDPL analysis revealed the presence of active recombination centers participating in PL emission tuning. We achieved PL quantum yield (PLQY) up to 86% for S-doped core/shell QDs with dominant zigzag defects, which is higher than previously reported ZnSe/af-GQDs (PLQY ~ 83%). Heteroatoms not only altered the electron density (ED) of the af-GQDs but also tuned graphene-related edge defects (zigzag and armchair). The color chromaticity coordinates are positioned in the yellow-orange-red region on the Commission Internationale de l’éclairage (CIE) 1931 color space, demonstrating the strong color perception modulation and multicomponent color emission from a single emissive layer (SEL) ZnSe/af-XGQDs (S, N, B). This low-cost, nontoxic, and facile approach provides a platform for the realization of future SEL for white light-emitting diodes (LEDs) and display devices.