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Dayong Jin
University of Technology Sydney
Corresponding Author
ORCiD: https://orcid.org/0000-0003-1046-2666
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Photon upconversion of near-infrared (NIR) irradiation into deep-ultraviolet (UV) emission offers many exciting opportunities for drug release in deep tissues, photodynamic therapy, solid-state lasing, energy storage, and photocatalysis. However, NIR-to-deep-UV upconversion remains a daunting challenge due to low quantum efficiency. Here, we report an unusual six-photon upconversion process in Gd3+/Tm3+-codoped nanoparticles comprising a heterogeneous, core-multishell nanostructure. This multishell design efficiently suppresses energy consumption induced by interior energy traps, maximizes cascade sensitizations of the NIR excitation, and promotes upconverted deep-UV emission from high-lying excited states. We released the intense six-photon-upconverted UV emissions at 253 nm under 808-nm excitation. This work provides new insight into mechanistic understanding of the upconversion process within the heterogeneous architecture, while offering exciting opportunities for developing nanoscale deep-UV emitters that can be remotely controlled in deep tissues upon NIR illumination.
Keywords
Photo Upconversion of Near-infrared Irradiation, Heterogeneous Core-multishell Nanostructure, Interior Energy Traps, Cascade Sensitizations
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This is a list of supplementary files associated with this preprint. Click to download.
- Scheme1.png
Scheme 1| Schematic illustration of upconverted excitation lock-in (UCEL) mechanism for deep UV generation within a nanoparticle. The proposed UCEL scheme involving a heterogeneous, core-multishell nanostructure (Gd-CSYS2S3). A multistep cascade energy transfer (Nd3+→Yb3+→Tm3+→Gd3+) leads to populate the excited states of Gd3+. The optical inert NaYF4 layer locating in the first shell layer of nanoparticles can lock-in the upconverted excitation energy of Gd3+ ions and prevent depopulation by deleterious energy traps within the nanoparticles, resulting in intense deep UV upconversion emission. S, M, E, R and T denote sensitizer Nd3+, migrator Yb3+, emitter Tm3+, recycler Gd3+, and energy traps, respectively.
- UpconvertedExcitonLockinforDeepUltravioletEnhancementSI.doc
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See the published version of this preprint at Nature Communications.
This is a preprint, a preliminary version of a manuscript that has not completed peer review at a journal. Research Square does not conduct peer review prior to posting preprints. The posting of a preprint on this server should not be interpreted as an endorsement of its validity or suitability for dissemination as established information or for guiding clinical practice.
Learn more about In Review
Article
Dayong Jin
University of Technology Sydney
Corresponding Author
ORCiD: https://orcid.org/0000-0003-1046-2666
Badges
Prescreen
This manuscript passed our Prescreen assessment
Complete author information
Appropriate declaration statements
Potential risks to human health
Prescreen
Peer Review Timeline
CURRENT STATUS: Published
View the published article at Nature Communications.
Version 1
Posted 28 Oct, 2020
Metrics
Comments: 0
PDF Downloads: ...
HTML Views: ...
Subject Areas
Nanoscience
License:
This work is licensed under a CC BY 4.0 License. Read Full License
View the published article at Nature Communications.
Photon upconversion of near-infrared (NIR) irradiation into deep-ultraviolet (UV) emission offers many exciting opportunities for drug release in deep tissues, photodynamic therapy, solid-state lasing, energy storage, and photocatalysis. However, NIR-to-deep-UV upconversion remains a daunting challenge due to low quantum efficiency. Here, we report an unusual six-photon upconversion process in Gd3+/Tm3+-codoped nanoparticles comprising a heterogeneous, core-multishell nanostructure. This multishell design efficiently suppresses energy consumption induced by interior energy traps, maximizes cascade sensitizations of the NIR excitation, and promotes upconverted deep-UV emission from high-lying excited states. We released the intense six-photon-upconverted UV emissions at 253 nm under 808-nm excitation. This work provides new insight into mechanistic understanding of the upconversion process within the heterogeneous architecture, while offering exciting opportunities for developing nanoscale deep-UV emitters that can be remotely controlled in deep tissues upon NIR illumination.
Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
There is NO Competing Interest.
This is a list of supplementary files associated with this preprint. Click to download.
- Scheme1.png
Scheme 1| Schematic illustration of upconverted excitation lock-in (UCEL) mechanism for deep UV generation within a nanoparticle. The proposed UCEL scheme involving a heterogeneous, core-multishell nanostructure (Gd-CSYS2S3). A multistep cascade energy transfer (Nd3+→Yb3+→Tm3+→Gd3+) leads to populate the excited states of Gd3+. The optical inert NaYF4 layer locating in the first shell layer of nanoparticles can lock-in the upconverted excitation energy of Gd3+ ions and prevent depopulation by deleterious energy traps within the nanoparticles, resulting in intense deep UV upconversion emission. S, M, E, R and T denote sensitizer Nd3+, migrator Yb3+, emitter Tm3+, recycler Gd3+, and energy traps, respectively.
- UpconvertedExcitonLockinforDeepUltravioletEnhancementSI.doc
Supporting Information
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