Versatile Spectral and Lifetime Multiplexing Nanoplatform with Excitation Orthogonalized Upconversion Luminescence.

Optical encoding together with color multiplexing benefits on-site detection, and enriching the components with narrow emissions from lanthanide could greatly increase the coding density. Here, we show a typical example to combine emission color and lifetime that are simultaneously integrated in a single lanthanide nanoparticle. With the multicompartment core/shell structure, the nanoparticles can activate different emitting pathways under varied excitation. This enables the nanoparticles to generate versatile excitation orthogonalized upconversion luminescence in both emission colors and lifetimes. As a typical example, green emission of Er3+ and blue emission of Tm3+ can be triggered with 808 and 980 nm lasers, respectively. Moreover, with incorporation of Tb3+, not only is emission from Tb3+ introduced but also the lifetime difference of 0.13 ms (Er3+) and 3.6 ms (Tb3+) is yielded for the green emission, respectively. Multiplexed fingerprint imaging and time-gated luminescence imaging were achieved in wavelength and lifetime dimensions. The spectral and lifetime encoding ability from lanthanide luminescence greatly broadens the scope of luminescent materials for optical multiplexing studies.

[1]  Wei Huang,et al.  Multicolour synthesis in lanthanide-doped nanocrystals through cation exchange in water , 2016, Nature Communications.

[2]  Ping Huang,et al.  Lanthanide-doped LiLuF(4) upconversion nanoprobes for the detection of disease biomarkers. , 2014, Angewandte Chemie.

[3]  Ya-Wen Zhang,et al.  High-quality sodium rare-earth fluoride nanocrystals: controlled synthesis and optical properties. , 2006, Journal of the American Chemical Society.

[4]  Chun-Hua Yan,et al.  Energy transfer in lanthanide upconversion studies for extended optical applications. , 2015, Chemical Society reviews.

[5]  Cunhai Dong,et al.  Self-focusing by Ostwald ripening: a strategy for layer-by-layer epitaxial growth on upconverting nanocrystals. , 2012, Journal of the American Chemical Society.

[6]  B. Cohen,et al.  Rationally Designed Energy Transfer in Upconverting Nanoparticles , 2015, Advanced materials.

[7]  Hans H Gorris,et al.  Photon-upconverting nanoparticles for optical encoding and multiplexing of cells, biomolecules, and microspheres. , 2013, Angewandte Chemie.

[8]  Wei Fan,et al.  Engineering the Upconversion Nanoparticle Excitation Wavelength: Cascade Sensitization of Tri‐doped Upconversion Colloidal Nanoparticles at 800 nm , 2013 .

[9]  T. Senden,et al.  Photonic effects on the radiative decay rate and luminescence quantum yield of doped nanocrystals. , 2015, ACS nano.

[10]  P. Prasad,et al.  Upconversion Nanoparticles: Design, Nanochemistry, and Applications in Theranostics , 2014, Chemical reviews.

[11]  Simon Dühnen,et al.  Synthesis of 10 nm β-NaYF4:Yb,Er/NaYF4 Core/Shell Upconversion Nanocrystals with 5 nm Particle Cores. , 2016, Angewandte Chemie.

[12]  Zhouping Wang,et al.  Simultaneous aptasensor for multiplex pathogenic bacteria detection based on multicolor upconversion nanoparticles labels. , 2014, Analytical chemistry.

[13]  Yixiao Zhang,et al.  An upconversion nanoparticle with orthogonal emissions using dual NIR excitations for controlled two-way photoswitching. , 2014, Angewandte Chemie.

[14]  Ling-Dong Sun,et al.  Efficient Tailoring of Upconversion Selectivity by Engineering Local Structure of Lanthanides in Na(x)REF(3+x) Nanocrystals. , 2015, Journal of the American Chemical Society.

[15]  Quan Yuan,et al.  Near-infrared-light-mediated imaging of latent fingerprints based on molecular recognition. , 2014, Angewandte Chemie.

[16]  Jie Shen,et al.  Rare-Earth nanoparticles with enhanced upconversion emission and suppressed rare-Earth-ion leakage. , 2012, Chemistry.

[17]  Hai Zhu,et al.  Upconverting near-infrared light through energy management in core-shell-shell nanoparticles. , 2013, Angewandte Chemie.

[18]  Wei Feng,et al.  High-Contrast Visualization of Upconversion Luminescence in Mice Using Time-Gating Approach. , 2016, Analytical chemistry.

[19]  P. Prasad,et al.  Alleviating Luminescence Concentration Quenching in Upconversion Nanoparticles through Organic Dye Sensitization. , 2016, Journal of the American Chemical Society.

[20]  Wei Huang,et al.  Temporal full-colour tuning through non-steady-state upconversion. , 2015, Nature nanotechnology.

[21]  Wei Feng,et al.  Nd3+-Sensitized Upconversion Nanostructure as a Dual-Channel Emitting Optical Probe for Near Infrared-to-Near Infrared Fingerprint Imaging. , 2016, Inorganic chemistry.

[22]  Amol D. Punjabi,et al.  Tailoring dye-sensitized upconversion nanoparticle excitation bands towards excitation wavelength selective imaging. , 2015, Nanoscale.

[23]  Dayong Jin,et al.  Controlling upconversion nanocrystals for emerging applications. , 2015, Nature nanotechnology.

[24]  Emory M. Chan,et al.  Combinatorial approaches for developing upconverting nanomaterials: high-throughput screening, modeling, and applications. , 2015, Chemical Society reviews.

[25]  Markus P. Hehlen,et al.  Hexagonal Sodium Yttrium Fluoride Based Green and Blue Emitting Upconversion Phosphors , 2004 .

[26]  Fan Zhang,et al.  Single-band upconversion nanoprobes for multiplexed simultaneous in situ molecular mapping of cancer biomarkers , 2015, Nature Communications.

[27]  Qiang Sun,et al.  Mechanistic investigation of photon upconversion in Nd(3+)-sensitized core-shell nanoparticles. , 2013, Journal of the American Chemical Society.

[28]  Patrick S Doyle,et al.  Universal process-inert encoding architecture for polymer microparticles. , 2014, Nature materials.

[29]  Chunhua Yan,et al.  Luminescence‐Driven Reversible Handedness Inversion of Self‐Organized Helical Superstructures Enabled by a Novel Near‐Infrared Light Nanotransducer , 2015, Advanced materials.

[30]  M. Pawlyta,et al.  Energy Migration Up-conversion of Tb3+ in Yb3+ and Nd3+ Codoped Active-Core/Active-Shell Colloidal Nanoparticles , 2016 .

[31]  Xianping Fan,et al.  Establishing the Structural Integrity of Core-Shell Nanoparticles against Elemental Migration using Luminescent Lanthanide Probes. , 2015, Angewandte Chemie.

[32]  Ling-Dong Sun,et al.  Nd(3+)-sensitized upconversion nanophosphors: efficient in vivo bioimaging probes with minimized heating effect. , 2013, ACS nano.

[33]  Yuliang Zhao,et al.  Elimination of Photon Quenching by a Transition Layer to Fabricate a Quenching‐Shield Sandwich Structure for 800 nm Excited Upconversion Luminescence of Nd3+‐Sensitized Nanoparticles , 2014, Advanced materials.

[34]  S. Lau,et al.  Constructing Interfacial Energy Transfer for Photon Up- and Down-Conversion from Lanthanides in a Core-Shell Nanostructure. , 2016, Angewandte Chemie.

[35]  Wei Fan,et al.  Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications. , 2016, ACS nano.

[36]  Gang Han,et al.  Combinatorial discovery of lanthanide-doped nanocrystals with spectrally pure upconverted emission. , 2012, Nano letters.

[37]  Chunhua Yan,et al.  Photon upconversion in Yb3+–Tb3+ and Yb3+–Eu3+ activated core/shell nanoparticles with dual-band excitation , 2016 .

[38]  J. Paul Robinson,et al.  Tunable lifetime multiplexing using luminescent nanocrystals , 2013, Nature Photonics.

[39]  Fiorenzo Vetrone,et al.  Synthesis of colloidal upconverting NaYF4 nanocrystals doped with Er3+, Yb3+ and Tm3+, Yb3+ via thermal decomposition of lanthanide trifluoroacetate precursors. , 2006, Journal of the American Chemical Society.

[40]  J. Dawes,et al.  Single-nanocrystal sensitivity achieved by enhanced upconversion luminescence. , 2013, Nature nanotechnology.

[41]  Peng Shi,et al.  Anti-counterfeiting patterns encrypted with multi-mode luminescent nanotaggants. , 2017, Nanoscale.

[42]  Xian Chen,et al.  Photon upconversion in core-shell nanoparticles. , 2015, Chemical Society reviews.

[43]  Fan Zhang,et al.  Filtration Shell Mediated Power Density Independent Orthogonal Excitations-Emissions Upconversion Luminescence. , 2016, Angewandte Chemie.

[44]  Deming Liu,et al.  Three-dimensional controlled growth of monodisperse sub-50 nm heterogeneous nanocrystals , 2016, Nature Communications.