Significant enhancement of the quantum yield of CdTe nanocrystals synthesized in aqueous phase by controlling the pH and concentrations of precursor solutions

Abstract In this paper, we systematically investigated the aqueous synthesis conditions of CdTe nanocrystals (QDs), and found that the pH value and the concentrations of precursors significantly affected the photoluminescence quantum yield (QY) of CdTe QDs. When the concentration of precursors (Cd) was 1.25 mM, and the pH of Cd precursors solution was about 8.0, CdTe QDs with high QY up to 40–67% were successfully prepared in aqueous phase. Moreover, these high luminescent QDs showed excellent stabilities in aqueous phases, and their luminescence was nearly independent of the pH of the colloid solution. The XPS and XRD characterizations implied that the high luminescence of the QDs synthesized at lower pH was possibly attributed to the formation of the thicker shell (cadmium–3–mercaptopropionic acid complexes) on particles surface, which not only decreased the traps on QDs surface, but also acted as a steric barrier to control the kinetics of QDs growth and led to the formation of a better surface structure. Our modification of conventional aqueous synthesis dramatically improved the QY of the prepared CdTe QDs, and it will become an attractive alternative to the synthesis of QDs in organic phase.

[1]  D. Balding,et al.  HLA Sequence Polymorphism and the Origin of Humans , 2006 .

[2]  A. Rogach Nanocrystalline CdTe and CdTe(S) particles: wet chemical preparation, size-dependent optical properties and perspectives of optoelectronic applications , 2000 .

[3]  A. Rogach,et al.  A Novel Organometallic Synthesis of Highly Luminescent CdTe Nanocrystals , 2001 .

[4]  Nikolai Gaponik,et al.  THIOL-CAPPING OF CDTE NANOCRYSTALS: AN ALTERNATIVE TO ORGANOMETALLIC SYNTHETIC ROUTES , 2002 .

[5]  Hao Zhang,et al.  Studies on quantum dots synthesized in aqueous solution for biological labeling via electrostatic interaction. , 2003, Analytical biochemistry.

[6]  Shuming Nie,et al.  Alloyed semiconductor quantum dots: tuning the optical properties without changing the particle size. , 2003, Journal of the American Chemical Society.

[7]  Horst Weller,et al.  Biofunctionalization of Silica-Coated CdTe and Gold Nanocrystals , 2002 .

[8]  W. Webb,et al.  Water-Soluble Quantum Dots for Multiphoton Fluorescence Imaging in Vivo , 2003, Science.

[9]  Wei Chen,et al.  Antigen/Antibody Immunocomplex from CdTe Nanoparticle Bioconjugates , 2002 .

[10]  Mingyuan Gao,et al.  From Water‐Soluble CdTe Nanocrystals to Fluorescent Nanocrystal–Polymer Transparent Composites Using Polymerizable Surfactants , 2003 .

[11]  J. Demas,et al.  Measurement of photoluminescence quantum yields. Review , 1971 .

[12]  Vicki L. Colvin,et al.  X-ray Photoelectron Spectroscopy of CdSe Nanocrystals with Applications to Studies of the Nanocrystal Surface , 1994 .

[13]  S. Nie,et al.  Quantum dot bioconjugates for ultrasensitive nonisotopic detection. , 1998, Science.

[14]  D. L. Klayman,et al.  Reaction of selenium with sodium borohydride in protic solvents. A Facile Method for the introduction of selenium into organic molecules , 1973 .

[15]  A Paul Alivisatos,et al.  Sorting fluorescent nanocrystals with DNA. , 2002, Journal of the American Chemical Society.

[16]  Alexander Eychmüller,et al.  Strongly Photoluminescent CdTe Nanocrystals by Proper Surface Modification , 1998 .

[17]  Xiaogang Peng,et al.  Formation of high-quality CdTe, CdSe, and CdS nanocrystals using CdO as precursor. , 2001, Journal of the American Chemical Society.

[18]  Xiaogang Peng,et al.  Formation and stability of size-, shape-, and structure-controlled CdTe nanocrystals: Ligand effects on monomers and nanocrystals , 2003 .

[19]  M. Bruchez,et al.  Immunofluorescent labeling of cancer marker Her2 and other cellular targets with semiconductor quantum dots , 2003, Nature Biotechnology.

[20]  Vincent Noireaux,et al.  In Vivo Imaging of Quantum Dots Encapsulated in Phospholipid Micelles , 2002, Science.

[21]  Mingyuan Gao,et al.  The Influence of Carboxyl Groups on the Photoluminescence of Mercaptocarboxylic Acid-Stabilized CdTe Nanoparticles , 2003 .

[22]  A. L. Rogach,et al.  Semiconductor Quantum Dot-Labeled Microsphere Bioconjugates Prepared by Stepwise Self-Assembly , 2002 .

[23]  P. Guyot-Sionnest,et al.  Synthesis and Characterization of Strongly Luminescing ZnS-Capped CdSe Nanocrystals , 1996 .

[24]  A. Rogach,et al.  Synthesis and surface modification of amino-stabilized CdSe, CdTe and InP nanocrystals , 2002 .

[25]  Xiaogang Peng,et al.  Control of photoluminescence properties of CdSe nanocrystals in growth. , 2002, Journal of the American Chemical Society.

[26]  M. Bawendi,et al.  Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites , 1993 .

[27]  J. Matthew Mauro,et al.  Long-term multiple color imaging of live cells using quantum dot bioconjugates , 2003, Nature Biotechnology.

[28]  Xiaogang Peng,et al.  Epitaxial Growth of Highly Luminescent CdSe/CdS Core/Shell Nanocrystals with Photostability and Electronic Accessibility , 1997 .

[29]  A. Rogach,et al.  Synthesis and characterization of thiol-stabilized CdTe nanocrystals , 1996 .

[30]  Xiaogang Peng,et al.  Alternative Routes toward High Quality CdSe Nanocrystals , 2001 .

[31]  ller,et al.  Relations between the Photoluminescence Efficiency of CdTe Nanocrystals and Their Surface Properties Revealed by Synchrotron XPS , 2003 .

[32]  J. Matthew Mauro,et al.  Self-Assembly of CdSe−ZnS Quantum Dot Bioconjugates Using an Engineered Recombinant Protein , 2000 .

[33]  M. Bawendi,et al.  (CdSe)ZnS Core-Shell Quantum Dots - Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites , 1997 .

[34]  G. Sukhorukov,et al.  Toward Encoding Combinatorial Libraries: Charge‐Driven Microencapsulation of Semiconductor Nanocrystals Luminescing in the Visible and Near IR , 2002 .

[35]  Zhiyong Tang,et al.  Spontaneous Organization of Single CdTe Nanoparticles into Luminescent Nanowires , 2002, Science.