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Peer-reviewedCC BY-NC-NDMaterials today. Advances

Facile synthesis of large-Stokes-shift giant CdHgSe/CdHgSeS near-infrared quantum dots via chlorine-mediated Ostwald ripening.

14 affiliations
  1. 1Division of Nanotechnology, Daegu Gyeongbuk Institute of Science and Technology (DGIST), Daegu, 42988, Republic of Korea.
  2. 2DGIST-ETH Microrobotics Research Center, DGIST, Daegu, 42988, Republic of Korea.
  3. 3Institute for Molecular Metabolism Innovation, Soonchunhyang University, Asan, Chungcheongnam-do, 31538, Republic of Korea.
  4. 4Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang, Gyeongsangbuk-Do, 37673, Republic of Korea.
  5. 5Division of Interdisciplinary Bioscience and Bioengineering, POSTECH, Pohang, Gyeongsangbuk-Do, 37673, Republic of Korea.
  6. 6Department of Bioengineering, University of Illinois Urbana-Champaign (UIUC), Urbana, IL, 61801, USA.
  7. 7Holonyak Micro and Nanotechnology Laboratory, UIUC, Urbana, IL, 61801, USA.
  8. 8Cancer Center at Illinois, UIUC, Urbana, IL, 61801, USA.
  9. 9Carl R. Woese Institute for Genomic Biology, UIUC, Urbana, IL, 61801, USA.
  10. 10Department of Materials Science and Engineering, UIUC, Urbana, IL, 61801, USA.
  11. 11Carle Illinois College of Medicine, Urbana, IL, 61801, USA.
  12. 12Department of Energy Science and Engineering, DGIST, Daegu, 42988, Republic of Korea.
  13. 13Department of Robotics and Mechatronics Engineering, DGIST, Daegu, 42988, Republic of Korea.
  14. 14Department of Biomedical Engineering, Institute for Applied Life Sciences, University of Massachusetts, Amherst, MA, 01003, USA.

Abstract

Giant core/shell quantum dots (GQDs) offer advantages for optoelectronics, including suppressed blinking and reduced Auger recombination, yet thick-shell growth often requires laborious successive ion layer adsorption and reaction (SILAR) cycles. Here we demonstrate a chlorine-mediated controlled Ostwald ripening strategy that transforms NIR-emitting CdHgSe/CdS core/shell seed QDs into giant CdHgSe/CdHgSeS core/gradient-shell QDs in a single post-synthetic step. Seed QDs are prepared by growing a thin (~1.6-monolayer) CdS shell on CdHgSe alloy cores. Injection of CHCl₃ at 240 °C triggers rapid ripening, in which most seeds dissolve while a minor population grows into GQDs. During ripening, the band-edge absorption feature is strongly attenuated and absorption below ~610 nm increases markedly, whereas NIR emission remains centered near ~900 nm, yielding a large effective Stokes shift that can mitigate reabsorption in luminescent solar concentrators. HAADF-STEM/EDS and XRD support a compositionally graded shell, while mass spectrometry and numerical simulations are consistent with chlorine-modified surface chemistry and altered monomer solubility/surface tension that accelerate ripening. As a proof of concept, embedding the GQDs in PMMA affords a transparent luminescent solar concentrator prototype with retained NIR emission and favorable spectral overlap with silicon photovoltaics.

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BibTeX
@article{lee2026facile,
  title = {{Facile synthesis of large-Stokes-shift giant CdHgSe/CdHgSeS near-infrared quantum dots via chlorine-mediated Ostwald ripening.}},
  author = {Gyudong Lee and Sanghwang Park and Jongcheol Seo and Wonseok Lee and Opeyemi H Arogundade and Andrew M Smith and Jongmin Choi and Hongsoo Choi and Sung Jun Lim},
  journal = {Materials today. Advances},
  year = {2026},
  month = aug,
  doi = {10.1016/j.mtadv.2026.100968},
  url = {https://europepmc.org/article/MED/42968830},
  note = {CC BY-NC-ND},
}
RIS
TY  - JOUR
TI  - Facile synthesis of large-Stokes-shift giant CdHgSe/CdHgSeS near-infrared quantum dots via chlorine-mediated Ostwald ripening.
AU  - Gyudong Lee
AU  - Sanghwang Park
AU  - Jongcheol Seo
AU  - Wonseok Lee
AU  - Opeyemi H Arogundade
AU  - Andrew M Smith
AU  - Jongmin Choi
AU  - Hongsoo Choi
AU  - Sung Jun Lim
PY  - 2026
DA  - 2026/08/01
JO  - Materials today. Advances
DO  - 10.1016/j.mtadv.2026.100968
UR  - https://europepmc.org/article/MED/42968830
AB  - Giant core/shell quantum dots (GQDs) offer advantages for optoelectronics, including suppressed blinking and reduced Auger recombination, yet thick-shell growth often requires laborious successive ion layer adsorption and reaction (SILAR) cycles. Here we demonstrate a chlorine-mediated controlled Ostwald ripening strategy that transforms NIR-emitting CdHgSe/CdS core/shell seed QDs into giant CdHgSe/CdHgSeS core/gradient-shell QDs in a single post-synthetic step. Seed QDs are prepared by growing a thin (~1.6-monolayer) CdS shell on CdHgSe alloy cores. Injection of CHCl₃ at 240 °C triggers rapid ripening, in which most seeds dissolve while a minor population grows into GQDs. During ripening, the band-edge absorption feature is strongly attenuated and absorption below ~610 nm increases markedly, whereas NIR emission remains centered near ~900 nm, yielding a large effective Stokes shift that can mitigate reabsorption in luminescent solar concentrators. HAADF-STEM/EDS and XRD support a compositionally graded shell, while mass spectrometry and numerical simulations are consistent with chlorine-modified surface chemistry and altered monomer solubility/surface tension that accelerate ripening. As a proof of concept, embedding the GQDs in PMMA affords a transparent luminescent solar concentrator prototype with retained NIR emission and favorable spectral overlap with silicon photovoltaics.
SN  - 2590-0498
ER  -