Quaternary Zn-Ag-In-Se quantum dots for biomedical optical imaging of RGD-modified micelles.

Exploring the synthesis of new biocompatible quantum dots (QDs) helps in overcoming the intrinsic toxicity of the existing QDs composed of highly toxic heavy metals (e.g., Cd, Hg, Pb, etc.) and is particularly interesting for the future practical application of QDs in biomedical imaging. Hence, in this report, a new one-pot approach to oil-soluble (highly toxic heavy metal-free) highly luminescent quaternary Zn-Ag-In-Se (ZAISe) QDs was designed. Their photoluminescence (PL) emission could be systematically tuned from 660 to 800 nm by controlling the Ag/Zn feed ratio, and their highest PL quantum yield is close to 50% after detailed optimization. Next, by using biodegradable RGD peptide (arginine-glycine-aspartic acid)-modified N-succinyl-N'-octyl-chitosan (RGD-SOC) micelles as a water transfer agent, the versatility of these quaternary ZAISe QDs for multiscale bioimaging of micelles (namely, in vitro and in vivo evaluating the tumor targeting of drug carriers) was further explored, as a promising alternative for Cd- and Pb-based QDs.

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

[2]  S. Gambhir,et al.  Quantum Dots for Live Cells, in Vivo Imaging, and Diagnostics , 2005, Science.

[3]  T. Pons,et al.  Synthesis and Characterization of Near-Infrared Cu−In−Se/ZnS Core/Shell Quantum Dots for In vivo Imaging , 2010 .

[4]  N. Pradhan,et al.  Mn-Doped Multinary CIZS and AIZS Nanocrystals. , 2012, The journal of physical chemistry letters.

[5]  Younan Xia,et al.  Chemical transformations of nanostructured materials , 2011 .

[6]  Benoit Dubertret,et al.  Cadmium-free CuInS2/ZnS quantum dots for sentinel lymph node imaging with reduced toxicity. , 2010, ACS nano.

[7]  Samuel Achilefu,et al.  Introduction to concepts and strategies for molecular imaging. , 2010, Chemical reviews.

[8]  S. Achilefu,et al.  Gold nanoparticles based molecular beacons for in vitro and in vivo detection of the matriptase expression on tumor. , 2013, Biosensors & bioelectronics.

[9]  Yueqing Gu,et al.  Targeted cancer therapy with a 2-deoxyglucose-based adriamycin complex. , 2013, Cancer research.

[10]  Sharon Bloch,et al.  Novel near-infrared fluorescent integrin-targeted DFO analogue. , 2008, Bioconjugate chemistry.

[11]  D. Sarma,et al.  Advances in Light-Emitting Doped Semiconductor Nanocrystals , 2011 .

[12]  N. Pradhan,et al.  Ultrasmall color-tunable copper-doped ternary semiconductor nanocrystal emitters. , 2011, Angewandte Chemie.

[13]  J. Frangioni In vivo near-infrared fluorescence imaging. , 2003, Current opinion in chemical biology.

[14]  Eugene Shi Guang Choo,et al.  Synthesis and characterization of AgInS2–ZnS heterodimers with tunable photoluminescence , 2011 .

[15]  Hao Zhang,et al.  Alkylthiol-enabled Se powder dissolution in oleylamine at room temperature for the phosphine-free synthesis of copper-based quaternary selenide nanocrystals. , 2012, Journal of the American Chemical Society.

[16]  Sangyoup Lee,et al.  Tuning solid-state fluorescence to the near-infrared: a combinatorial approach to discovering molecular nanoprobes for biomedical imaging. , 2013, ACS applied materials & interfaces.

[17]  Sharon Bloch,et al.  Multivalent carbocyanine molecular probes: synthesis and applications. , 2005, Bioconjugate chemistry.

[18]  Yueqing Gu,et al.  Folate-modified chitosan micelles with enhanced tumor targeting evaluated by near infrared imaging system , 2011 .

[19]  Wensheng Yang,et al.  A Simple Route for Highly Luminescent Quaternary Cu-Zn-In-S Nanocrystal Emitters , 2011 .

[20]  S. Achilefu,et al.  High-Quality CuInS2/ZnS Quantum Dots for In vitro and In vivo Bioimaging , 2012 .

[21]  J. Xue,et al.  Synthesis of Zn-Doped AgInS2 Nanocrystals and Their Fluorescence Properties , 2012 .

[22]  Tsukasa Torimoto,et al.  Facile synthesis of ZnS-AgInS2 solid solution nanoparticles for a color-adjustable luminophore. , 2007, Journal of the American Chemical Society.

[23]  Z. Jakubek,et al.  Low-temperature approach to highly emissive copper indium sulfide colloidal nanocrystals and their bioimaging applications. , 2013, ACS applied materials & interfaces.

[24]  Xiaogang Peng,et al.  Formation of high-quality I-III-VI semiconductor nanocrystals by tuning relative reactivity of cationic precursors. , 2009, Journal of the American Chemical Society.

[25]  Yueqing Gu,et al.  Facile synthesis of high-quality water-soluble N-acetyl-L-cysteine-capped Zn(1-x)Cd(x)Se/ZnS core/shell quantum dots emitting in the violet-green spectral range. , 2010, Journal of colloid and interface science.

[26]  V. Klimov,et al.  Efficient synthesis of highly luminescent copper indium sulfide-based core/shell nanocrystals with surprisingly long-lived emission. , 2011, Journal of the American Chemical Society.

[27]  Shuming Nie,et al.  Bioconjugated quantum dots for in vivo molecular and cellular imaging. , 2008, Advanced drug delivery reviews.

[28]  Miqin Zhang,et al.  Chitosan-based hydrogels for controlled, localized drug delivery. , 2010, Advanced drug delivery reviews.

[29]  Britton Chance,et al.  Synergistic effects of light-emitting probes and peptides for targeting and monitoring integrin expression , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[30]  Yueqing Gu,et al.  Versatile self-assembly of water-soluble thiol-capped CdTe quantum dots: external destabilization and internal stability of colloidal QDs. , 2013, Langmuir : the ACS journal of surfaces and colloids.

[31]  S. Achilefu,et al.  Highly luminescent water-soluble quaternary Zn-Ag-In-S quantum dots for tumor cell-targeted imaging. , 2013, Physical chemistry chemical physics : PCCP.

[32]  Fan Yang,et al.  A facile approach to synthesize high-quality Zn(x)Cu(y)InS(1.5+x+0.5y) nanocrystal emitters. , 2011, Chemical communications.

[33]  Haizheng Zhong,et al.  Tuning the Luminescence Properties of Colloidal I-III-VI Semiconductor Nanocrystals for Optoelectronics and Biotechnology Applications. , 2012, The journal of physical chemistry letters.

[34]  J. Willmann,et al.  Molecular imaging in drug development , 2008, Nature Reviews Drug Discovery.