Rare-Earth-Doped Orthogonal Luminescent Nanocrystals： From Fundamentals to Frontier Applications

doi:10.19894/j.issn.1000-0518.230185

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (11): 1475-1493.DOI: 10.19894/j.issn.1000-0518.230185

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Rare-Earth-Doped Orthogonal Luminescent Nanocrystals： From Fundamentals to Frontier Applications

Jun-Rong WANG¹^,², Qian-Qian SUN², Guo-Qing ZHU², Yan-Rong QIAN², Chun-Xia LI¹^,²()

^1.Institute of Shenzhen，Shangdong University，Shenzhen 518057，China
^2.Institute of Molecular Sciences and Engineering，Institute of Frontier and Interdisciplinary Science，Shangdong University，Qingdao 266237，China

Received:2023-06-29 Accepted:2023-10-17 Published:2023-11-01 Online:2023-12-01
Contact: Chun-Xia LI
About author:cxli@sdu.edu.cn
Supported by:
the Basic and Applied Basic Research Project of Guangdong Province(2022A1515010461);the National Natural Science Foundation of China(61775080);the Nature Foundation of Shandong Province(ZR2020ZD36)

Abstract

Abstract:

Lanthanide ion-doped upconversion luminescent nanomaterials with unique nonlinear Anti-Stokes luminescence have broad applications in life sciences， photonic transport， programmable control， and information encoding and decoding. Rare-earth-doped orthogonal luminescent nanocrystals are a major emerging research direction in the field of luminescence in recent years， which is based on the upconversion luminescence mechanism to realize the multifunctional integration of orthogonal luminescence on a single nanoparticle in a reasonable core-shell structure design， broadening the optional range and spatio-temporal tunability of spectra to further promote its application in related fields. This review summarizes the recent progress in the design optimization of synthetic rare-earth-doped orthogonal luminescent nanocrystals， and systematically discusses the regulation process of achieving orthogonal luminescence via energy transfer of rare-earth ions based on core-shell structures construction， as well as presents its applications in frontier fields such as information security anti-counterfeiting， bioimaging and therapy. Furthermore， the current challenges and future prospects of orthogonal luminescence are also summed up.

Key words: Rare-earth doping, Upconversion, Orthogonal luminescence, Core-shell structure, Photochromic modulation

CLC Number:

O611.6

Jun-Rong WANG, Qian-Qian SUN, Guo-Qing ZHU, Yan-Rong QIAN, Chun-Xia LI. Rare-Earth-Doped Orthogonal Luminescent Nanocrystals： From Fundamentals to Frontier Applications[J]. Chinese Journal of Applied Chemistry, 2023, 40(11): 1475-1493.

Figures/Tables 9

Fig.1 Schematic illustrations of excitation and emission in downshifting nanoparticles （a） and upconversion nanoparticles （b）?［36］； Schematic illustrations of luminescence mechanism in downshifting nanoparticles （c）?［37］ and upconversion nanoparticles （d）［3］

Fig.2 Suppression of surface quenching effect in upconversion nanomaterials based on core-shell structure design. （a） Luminescent photographs and spectral intensity variations of NaYF4∶Yb/Er（Tm） nanoparticles before and after coated with NaYF4 inert layer［50］；（b） Luminescent intensity of highly doped Er3+ nanoparticles at different NaLuF4 inert layer thicknesses［59］；（c） Luminescent intensity of Yb3+ highly doped lithium-based upconversion nanoparticles at different LiYF4 inert layer thickness［60］；（d） Luminescent spectra of aqueous NdF3 nanoparticles and NdF3@SiO2 nanoparticles at the excitation of 730 nm［61］；（e） Luminescent photographs and spectra of oily nanoparticles （left） and aqueous nanoparticles coated with two layers of SiO2 （right）［62］

Fig.3 Enhancement of excitation fluorescence absorption in upconversion nanomaterials based on core-shell structure design. （a） Luminescent photographs and spectral intensity variations of NaGdF4∶Yb/Er nanoparticles coated with NaGdF4 inert layer and NaGdF4∶Yb active layer， respectively［63］；（b） Comparison of luminescence in active core-luminescent layer-active shell structure nanoparticles and other structure types nanoparticles［64］；（c） Schematic illustration for the sensitization of nanoparticle with dye coupling and luminescent intensity before and after coupling with IR-808 dye［65］；（d） Spectral variations of nanoparticles containing Er， Tm and Ho activators after sensitization with ICG dye［66］

Fig.4 Orthogonal luminescence based on core-shell structure design. Design of double-emitting layer （a）， single-emitting layer with steady-state emission （b）， single-emitting layer with non-steady-state emission （c） for upconversion orthogonal luminescence and double-emitting layer （d） for upconversion/downshifting orthogonal luminescence［69］

Fig.5 Dual-color upconversion orthogonal luminescence based on core-shell structure design. The schematic illustration of the four-layer core-shell structure and upconversion orthogonal blue-green luminescent spectra of Tm3+ ions and Ho3+ ions under 976/808 nm excitation （a）［73］， the schematic illustration of the three-layer core-shell structure and upconversion orthogonal blue-green luminescent spectra of Tm3+ ions and Er3+ ions at the excition of 808 nm and different 980 nm powers （b）［22］， and the five-layer core-shell structure energy transition illustration and upconversion orthogonal blue-green luminescent spectra of Tm3+ and Er3+ ions at 980/796 nm excitation without dependence on excitation power （c）［21］ in the double-emitting layer design；（d） Upconversion orthogonal red-green luminescent spectra of simple core-shell structure with Er3+ ions under 980/530 nm excitation in the single-emitting layer design with steady-state emission［74］. （e） Upconversion orthogonal red-green luminescent spectra of simple core-shell structured with Er3+ ions at different pulse widths of 980 nm in the single-emitting layer design with non-steady-state emission［75］

Fig.6 RGB upconversion orthogonal luminescence based on core-shell structure design. （a） Schematic illustration of the four-layer core-shell structure， TEM diagram， spectral modulation and luminescent photographs as well as color coordinates under different excitation conditions in the double-emitting layer design with non-steady-state/steady-state emission［34］；（b） Schematic illustration of the four-layer core-shell structure and luminescent photographs as well as red-green ratios at different excitation power densities of 808/980 nm in the double-emitting layer design with steady-state emission［76］； The schematic illustration of the five-layer core-shell structure and luminescent photographs as well as spectra under the excitation of 1560/808/980 nm （c）［70］， the energy level transition illustration of the seven-layer core-shell structure， corresponding TEM and luminescent photographs （d）［77］， the schematic illustration of the six-layer core-shell structure and luminescent photographs as well as spectra under the excitation of 1532/980/800 nm （e）［78］ and the schematic illustration as well as energy level transition illustration of the six-layer core-shell structure （f） in the tri-emitting layer design［79］

Fig.7 Upconversion/downshifting dual-mode orthogonal luminescence based on core-shell structure design. （a） Multimode luminescent properties of LiLuF4∶Yb/A@LiYF4∶B （A=Er， Ho， Tm； B=Eu， Tb） core-shell nanoparticles［30］；（b） Schematic illustration of energy transfer and energy level transition of NaYF4∶Yb/Er@NaYF4∶Ce/Tb/Eu core-shell nanoparticles achieving upconversion/downshifting dual-mode emission［31］；（c） Core-shell structure design of NaGdF4∶Yb/Ho/Ce@NaYF4∶A （A=Eu， Tb， Sm， Dy） nanoparticles and construction with different types of core-shell structures［29］；（d） Schematic design of core-shell structure of LiYbF4∶Y@LiGdF4∶Yb/Tm@LiYF4∶A@LiGdF4∶Ce （A=Eu， Tb， Dy， Sm， Nd）［28］ and （e） luminescent photographs as well as spectra at different excitation wavelengths［28］

Fig.8 Information anti-counterfeiting application of orthogonal luminescent nanocrystals. （a） Dual-color upconversion orthogonal luminescence for anti-counterfeit images［21］；（b） Dual-color upconversion orthogonal luminescence with time gating for anti-counterfeit images［23］；（c） Tri-color upconversion orthogonal luminescence for logic encryption anti-counterfeiting and （d） cell phone assisted anti-counterfeiting［79］

Fig.9 Bioimaging and therapeutic applications of orthogonal luminescence nanocrystals. （a） Dual-color upconversion orthogonal luminescence for PDT via UCL monitoring［71］；（b） Dual-color upconversion orthogonal luminescence of a single activator for PDT via UCL real-time monitoring［81］；（c） Dual-color upconversion orthogonal luminescence of a single activator for PDT via PAI real-time monitoring［82］；（d） Dual-color upconversion orthogonal luminescence of a single activator for PDT via NIR-IIb imaging monitoring［87］

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Rare-Earth-Doped Orthogonal Luminescent Nanocrystals： From Fundamentals to Frontier Applications

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