Core-shell lanthanide upconversion nanophosphors as four-modal probes for tumor angiogenesis imaging.

Multimodality imaging overcomes the shortage and incorporates the advantages of different imaging tools. Lanthanide-based nanoprobes are unique and have rich optical, magnetic, radioactive, and X-ray attenuation properties; however, simple doping of different lanthanide cations into one host can result in a material with multifunction but not the optimized properties. In this study, using NaLuF4:Yb,Tm as the core and 4 nm of (153)Sm(3+)-doped NaGdF4 (half-life of (153)Sm = 46.3 h) as the shell, we developed a lanthanide-based core-shell nanocomposite as an optimized multimodal imaging probe with enhanced imaging ability. The lifetime of upconversion luminescence (UCL) at 800 nm and relaxation rate (1/T1) were at 1044 μs and 18.15 s(-1)·mM(-1), respectively; however, no significant decrease in the attenuation coefficient was observed, which preserved the excellent X-ray imaging ability. The nanomaterial NaLuF4:Yb,Tm@NaGdF4((153)Sm) was confirmed to be effective and applicable for UCL imaging, X-ray computed tomography (CT), magnetic resonance imaging, and single-photon emission computed tomography (SPECT) in vivo. Furthermore, the NaLuF4:Yb,Tm@NaGdF4((153)Sm) nanoparticles were applied in tumor angiogenesis analysis by combining multimodality imaging of CT, SPECT, and confocal UCL imaging, which shows its value of multifunctional nanoparticles NaLuF4:Yb,Tm@NaGdF4((153)Sm) in tumor angiogenesis imaging.

[1]  Wei Feng,et al.  Upconversion luminescence imaging of cells and small animals , 2013, Nature Protocols.

[2]  Yongsheng Liu,et al.  Lanthanide-doped luminescent nanoprobes: controlled synthesis, optical spectroscopy, and bioapplications. , 2013, Chemical Society reviews.

[3]  Chunhua Yan,et al.  Basic understanding of the lanthanide related upconversion emissions. , 2013, Nanoscale.

[4]  I. García,et al.  Glyconanoparticles as multifunctional and multimodal carbohydrate systems. , 2013, Chemical Society reviews.

[5]  Yongsheng Liu,et al.  Optical/magnetic multimodal bioprobes based on lanthanide-doped inorganic nanocrystals. , 2013, Chemistry.

[6]  Wei Feng,et al.  Upconversion Nanophosphors Naluf4:Yb,Tm for Lymphatic Imaging In Vivo by Real-Time Upconversion Luminescence Imaging under Ambient Light and High-Resolution X-ray CT , 2013, Theranostics.

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

[8]  Hongseok Yun,et al.  Designing tripodal and triangular gadolinium oxide nanoplates and self-assembled nanofibrils as potential multimodal bioimaging probes. , 2013, ACS nano.

[9]  Wei Feng,et al.  Radioisotope post-labeling upconversion nanophosphors for in vivo quantitative tracking. , 2013, Biomaterials.

[10]  V. Dravid,et al.  Multimodal bioimaging using rare earth doped Gd2O2S: Yb/Er phosphor with upconversion luminescence and magnetic resonance properties. , 2013, Journal of materials chemistry. A.

[11]  Yongsheng Liu,et al.  Lanthanide-doped luminescent nano-bioprobes: from fundamentals to biodetection. , 2013, Nanoscale.

[12]  Xiaogang Qu,et al.  Long-circulating Gd(2)O(3):Yb(3+), Er(3+) up-conversion nanoprobes as high-performance contrast agents for multi-modality imaging. , 2013, Biomaterials.

[13]  Sang Moo Lim,et al.  RGD Peptide–Conjugated Multimodal NaGdF4:Yb3+/Er3+ Nanophosphors for Upconversion Luminescence, MR, and PET Imaging of Tumor Angiogenesis , 2013, The Journal of Nuclear Medicine.

[14]  侯毅.  NaGdF4 Nanoparticle-Based Molecular Probes for Magnetic Resonance Imaging of Intraperitoneal Tumor Xenografts In Vivo , 2013 .

[15]  Taeghwan Hyeon,et al.  Theranostic Probe Based on Lanthanide‐Doped Nanoparticles for Simultaneous In Vivo Dual‐Modal Imaging and Photodynamic Therapy , 2012, Advanced materials.

[16]  Lehui Lu,et al.  Nanoparticulate X-ray computed tomography contrast agents: from design validation to in vivo applications. , 2012, Accounts of chemical research.

[17]  Paras N. Prasad,et al.  (α-NaYbF4:Tm(3+))/CaF2 core/shell nanoparticles with efficient near-infrared to near-infrared upconversion for high-contrast deep tissue bioimaging. , 2012, ACS nano.

[18]  Yun Sun,et al.  Water-stable NaLuF4-based upconversion nanophosphors with long-term validity for multimodal lymphatic imaging. , 2012, Biomaterials.

[19]  J. Hao,et al.  A strategy for simultaneously realizing the cubic-to-hexagonal phase transition and controlling the small size of NaYF4:Yb3+,Er3+ nanocrystals for in vitro cell imaging. , 2012, Small.

[20]  Wei Feng,et al.  Core-shell Fe3O4@NaLuF4:Yb,Er/Tm nanostructure for MRI, CT and upconversion luminescence tri-modality imaging. , 2012, Biomaterials.

[21]  Zhuang Liu,et al.  Upconversion nanophosphors for small-animal imaging. , 2012, Chemical Society reviews.

[22]  Ick Chan Kwon,et al.  Multifunctional nanoparticles for multimodal imaging and theragnosis. , 2012, Chemical Society reviews.

[23]  Gang Han,et al.  Controlled synthesis and single-particle imaging of bright, sub-10 nm lanthanide-doped upconverting nanocrystals. , 2012, ACS nano.

[24]  Lehui Lu,et al.  A high-performance ytterbium-based nanoparticulate contrast agent for in vivo X-ray computed tomography imaging. , 2012, Angewandte Chemie.

[25]  Yanqing Hua,et al.  Multifunctional nanoprobes for upconversion fluorescence, MR and CT trimodal imaging. , 2012, Biomaterials.

[26]  Mingdong Huang,et al.  Amine-functionalized lanthanide-doped KGdF4 nanocrystals as potential optical/magnetic multimodal bioprobes. , 2012, Journal of the American Chemical Society.

[27]  Daxiang Cui,et al.  Dual Phase‐Controlled Synthesis of Uniform Lanthanide‐Doped NaGdF4 Upconversion Nanocrystals Via an OA/Ionic Liquid Two‐Phase System for In Vivo Dual‐Modality Imaging , 2011 .

[28]  Lianzhou Wang,et al.  Positive and Negative Lattice Shielding Effects Co‐existing in Gd (III) Ion Doped Bifunctional Upconversion Nanoprobes , 2011 .

[29]  Wei Feng,et al.  Sub-10 nm hexagonal lanthanide-doped NaLuF4 upconversion nanocrystals for sensitive bioimaging in vivo. , 2011, Journal of the American Chemical Society.

[30]  Jianhua Hao,et al.  Tunable multicolor upconversion emissions and paramagnetic property of monodispersed bifunctional lanthanide-doped NaGdF4 nanorods , 2011 .

[31]  Kai Yang,et al.  Facile preparation of multifunctional upconversion nanoprobes for multimodal imaging and dual-targeted photothermal therapy. , 2011, Angewandte Chemie.

[32]  Paras N. Prasad,et al.  Monodisperse NaYbF4:Tm3+/NaGdF4 core/shell nanocrystals with near-infrared to near-infrared upconversion photoluminescence and magnetic resonance properties. , 2011, Nanoscale.

[33]  Qian Liu,et al.  18F-Labeled magnetic-upconversion nanophosphors via rare-Earth cation-assisted ligand assembly. , 2011, ACS nano.

[34]  Qing Peng,et al.  Lanthanide-doped nanocrystals: synthesis, optical-magnetic properties, and applications. , 2011, Accounts of chemical research.

[35]  Geoffrey A Ozin,et al.  Synthesis of ligand-free colloidally stable water dispersible brightly luminescent lanthanide-doped upconverting nanoparticles. , 2011, Nano letters.

[36]  Helmut Schäfer,et al.  Upconverting nanoparticles. , 2011, Angewandte Chemie.

[37]  Juan Wang,et al.  Direct evidence of a surface quenching effect on size-dependent luminescence of upconversion nanoparticles. , 2010, Angewandte Chemie.

[38]  Yongsheng Liu,et al.  A Strategy to Achieve Efficient Dual‐Mode Luminescence of Eu3+ in Lanthanides Doped Multifunctional NaGdF4 Nanocrystals , 2010, Advanced materials.

[39]  Guanying Chen,et al.  Ultrasmall monodisperse NaYF(4):Yb(3+)/Tm(3+) nanocrystals with enhanced near-infrared to near-infrared upconversion photoluminescence. , 2010, ACS nano.

[40]  Angelique Louie,et al.  Multimodality imaging probes: design and challenges. , 2010, Chemical reviews.

[41]  Yun Sun,et al.  Dual-modality in vivo imaging using rare-earth nanocrystals with near-infrared to near-infrared (NIR-to-NIR) upconversion luminescence and magnetic resonance properties. , 2010, Biomaterials.

[42]  Yuan Gao,et al.  Water-soluble NaYF4:Yb/Er upconversion nanophosphors: Synthesis, characteristics and application in bioimaging , 2010 .

[43]  C. S. Lim,et al.  Simultaneous phase and size control of upconversion nanocrystals through lanthanide doping , 2010, Nature.

[44]  Taeghwan Hyeon,et al.  Nonblinking and Nonbleaching Upconverting Nanoparticles as an Optical Imaging Nanoprobe and T1 Magnetic Resonance Imaging Contrast Agent , 2009 .

[45]  Fuyou Li,et al.  High contrast upconversion luminescence targeted imaging in vivo using peptide-labeled nanophosphors. , 2009, Analytical chemistry.

[46]  Christopher G. Morgan,et al.  The Active‐Core/Active‐Shell Approach: A Strategy to Enhance the Upconversion Luminescence in Lanthanide‐Doped Nanoparticles , 2009 .

[47]  Shiwei Wu,et al.  Non-blinking and photostable upconverted luminescence from single lanthanide-doped nanocrystals , 2009, Proceedings of the National Academy of Sciences.

[48]  Xiaogang Liu,et al.  Recent Advances in the Chemistry of Lanthanide‐Doped Upconversion Nanocrystals , 2009 .

[49]  Tymish Y. Ohulchanskyy,et al.  Combined Optical and MR Bioimaging Using Rare Earth Ion Doped NaYF4 Nanocrystals , 2009 .

[50]  Cunhai Dong,et al.  Cation exchange in lanthanide fluoride nanoparticles. , 2009, ACS nano.

[51]  Taeghwan Hyeon,et al.  Multifunctional nanostructured materials for multimodal imaging, and simultaneous imaging and therapy. , 2009, Chemical Society reviews.

[52]  Shyam Bahadur Rai,et al.  Er3+/Yb3+ codoped Gd2O3 nano-phosphor for optical thermometry , 2009 .

[53]  Tymish Y. Ohulchanskyy,et al.  High contrast in vitro and in vivo photoluminescence bioimaging using near infrared to near infrared up-conversion in Tm3+ and Yb3+ doped fluoride nanophosphors. , 2008, Nano letters.

[54]  P. Acton,et al.  Small-Animal SPECT and SPECT/CT: Important Tools for Preclinical Investigation* , 2008, Journal of Nuclear Medicine.

[55]  Zhengquan Li,et al.  An efficient and user-friendly method for the synthesis of hexagonal-phase NaYF4:Yb, Er/Tm nanocrystals with controllable shape and upconversion fluorescence , 2008, Nanotechnology.

[56]  Weibo Cai,et al.  Multimodality Molecular Imaging of Tumor Angiogenesis , 2008, Journal of Nuclear Medicine.

[57]  Yong Zhang,et al.  Upconversion fluorescence imaging of cells and small animals using lanthanide doped nanocrystals. , 2008, Biomaterials.

[58]  Z. Fayad,et al.  Molecular imaging of tumor angiogenesis using αvβ3-integrin targeted multimodal quantum dots , 2008, Angiogenesis.

[59]  Andrei Iagaru,et al.  Molecular imaging can accelerate anti-angiogenic drug development and testing , 2007, Nature Clinical Practice Oncology.

[60]  A. Jubb,et al.  Predicting benefit from anti-angiogenic agents in malignancy , 2006, Nature Reviews Cancer.

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

[62]  Peter Carmeliet,et al.  Angiogenesis in life, disease and medicine , 2005, Nature.

[63]  N. Rofsky,et al.  MR imaging relaxation times of abdominal and pelvic tissues measured in vivo at 3.0 T: preliminary results. , 2004, Radiology.

[64]  T. Mihaljevic,et al.  Near-infrared fluorescent type II quantum dots for sentinel lymph node mapping , 2004, Nature Biotechnology.

[65]  F. Auzel.  Upconversion and anti-Stokes processes with f and d ions in solids. , 2004, Chemical reviews.

[66]  R. Lauffer,et al.  Gadolinium(III) Chelates as MRI Contrast Agents: Structure, Dynamics, and Applications. , 1999, Chemical reviews.

[67]  R. A. Holmes,et al.  Samarium-153-EDTMP: pharmacokinetic, toxicity and pain response using an escalating dose schedule in treatment of metastatic bone cancer. , 1992, Journal of nuclear medicine : official publication, Society of Nuclear Medicine.

[68]  R. A. Brooks,et al.  Principles of computer assisted tomography (CAT) in radiographic and radioisotopic imaging , 1976, Physics in medicine and biology.