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Design and Synthesis of CdHgSe/HgS/CdZnS Core/Multi-Shell Quantum Dots Exhibiting High-Quantum-Yield Tissue-Penetrating Shortwave Infrared Luminescence |
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| Authors: | Gyudong Lee Woo Hyeon Jeong Beomjoo Kim Sungwoong Jeon Andrew M. Smith Jongcheol Seo Kengo Suzuki Jin-young Kim Hyunki Lee Hongsoo Choi Dae Sung Chung Jongmin Choi Hyosung Choi Sung Jun Lim |
| Affiliation: | 1. Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science and Technology (DGIST), 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea Division of Nanotechnology, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;2. Division of Nanotechnology, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea Department of Chemistry and Research Institute for Natural Science, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763 Republic of Korea;3. Department of Robotics Engineering, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea DGIST-ETH Microrobotics Research Center, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;4. DGIST-ETH Microrobotics Research Center, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea IMsystem Corp., DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;5. Department of Bioengineering, University of Illinois Urbana-Champaign (UIUC), Urbana, IL, 61801 USA Department of Materials Science and Engineering, UIUC, Urbana, IL, 61801 USA Cancer Center at Illinois, UIUC, Urbana, IL, 61801 USA Carle Illinois College of Medicine, UIUC, Urbana, IL, 61801 USA;6. Department of Chemistry, POSTECH, 77 Cheongam-Ro, Nam-Gu, Pohang, Gyeongsangbuk-Do, 37673 Republic of Korea;7. Applied Spectroscopy System Department, Hamamatsu Photonics K.K., 812 Joko-Cho, Higashi-Ku, Hamamatsu City, 431-3196 Japan;8. DGIST-ETH Microrobotics Research Center, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea Division of Biotechnology, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;9. DGIST-ETH Microrobotics Research Center, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea Division of Intelligent Robot, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;10. DGIST-ETH Microrobotics Research Center, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea Department of Robotics Engineering, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;11. Department of Chemical Engineering, POSTECH, 77 Cheongam-Ro, Nam-Gu, Pohang, Gyeongsangbuk-Do, 37673 Republic of Korea;12. Department of Energy Science and Engineering, Daegu Gyeongbuk Institute of Science and Technology (DGIST), 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea;13. Department of Chemistry and Research Institute for Natural Science, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763 Republic of Korea;14. Division of Nanotechnology, DGIST, 333 Techno Jungang Daero, Hyeonpung-Eup, Dalseong-Gun, Daegu, 42988 Republic of Korea |
| Abstract: | CdxHg1−xSe/HgS/CdyZn1−yS core/multi-shell quantum dots (QDs) exhibiting bright tissue-penetrating shortwave infrared (SWIR; 1000–1700 nm) photoluminescence (PL) are engineered. The new structure consists of a quasi-type-II CdxHg1−xSe/HgS core/inner shell domain creating luminescent bandgap tunable across SWIR window and a wide-bandgap CdyZn1−yS outer shell boosting the PL quantum yield (QY). This compositional sequence also facilitates uniform and coherent shell growth by minimizing interfacial lattice mismatches, resulting in high QYs in both organic (40–80%) and aqueous (20–70%) solvents with maximum QYs of 87 and 73%, respectively, which are comparable to those of brightest visible-to-near infrared QDs. Moreover, they maintain bright PL in a photocurable resin (QY 40%, peak wavelength ≈ 1300 nm), enabling the fabrication of SWIR-luminescent composites of diverse morphology and concentration. These composites are used to localize controlled amounts of SWIR QDs inside artificial (Intralipid) and porcine tissues and quantitatively evaluate the applicability as luminescent probes for deep-tissue imaging. |
| Keywords: | deep-tissue imaging photoluminescence quantum yields quantum dots quantum dot–polymer composites shortwave infrared |