Effects of the sol-gel solution host on the chemical and optical properties of PbS quantum dots

PbS nanoparticles were prepared via a colloidal route using an organic capping agent, and were incorporated in both a silica and a titania sol-gel solution with a concentration of 10 mol%. The stability of the particles embedded in the sols was lengthened from 2 h to several days and their growth was considerably slowed down. The kinetics of the optical absorption allowed us to quantify the growth rate of the particles. Analysis of the optical emission in the three solutions (colloid, SiO2/PbS and TiO2/PbS) showed that the PbS nanocrystals are partially passivated by the silica chains and completely by the titania chains in the sols. Conjoint study of the optical absorption and emission measurements revealed a correlation between the presence of a structured exciton peak in the absorption spectra and the absence of shallow surface states.

[1]  F. Wise,et al.  Electronic structure and optical properties of PbS and PbSe quantum dots , 1997 .

[2]  J. L. Marín,et al.  Confinement of excitons in spherical quantum dots , 1998 .

[3]  R. Kane,et al.  Theoretical Study of the Electronic Structure of PbS Nanoclusters , 1996 .

[4]  S. Risbud,et al.  Synthesis, Optical Spectroscopy and Ultrafast Electron Dynamics of PbS Nanoparticles with Different Surface Capping , 2000 .

[5]  J. Simmons,et al.  Absorption and Raman scattering spectroscopies from semiconductor–glass composites , 2000 .

[6]  J. Devreese,et al.  Multiphonon photoluminescence and Raman scattering in semiconductor quantum dots , 1998 .

[7]  J. Mugnier,et al.  Up-conversion fluorescence spectroscopy in Er3+: TiO2 planar waveguides prepared by a sol-gel process , 1996 .

[8]  H. Schmidt,et al.  Synthesis and Characterization of PbS Nanoparticles in Ethanolic Solution Stabilized by Hydroxypropyl Cellulose , 1998 .

[9]  E. Lifshitz,et al.  Properties of PbS nanocrystals embedded in zirconia sol–gel film , 2002 .

[10]  F. Wise,et al.  Lead salt quantum dots: the limit of strong quantum confinement. , 2000, Accounts of chemical research.

[11]  A. Arora,et al.  Inhomogeneous broadening in the photoluminescence spectrum of CdS nanoparticles , 1999 .

[12]  L. Langof,et al.  Synthesis and characterization of PbSe and PbSe/PbS core–shell colloidal nanocrystals , 2002 .

[13]  A D Yoffe,et al.  Semiconductor quantum dots and related systems: Electronic, optical, luminescence and related properties of low dimensional systems , 2001 .

[14]  Vittorio Degiorgio,et al.  Nonlinear optical properties of semiconductor nanocrystals , 1998 .

[15]  A. D. Yoffe,et al.  Low-dimensional systems: Quantum size effects and electronic properties of semiconductor microcrystallites (zero-dimensional systems) and some quasi-two-dimensional systems , 1993 .

[16]  S. Turrell,et al.  Spectroscopic investigations of CdS nanoparticles in sol-gel derived polymeric thin films and bulk silica matrices , 2001 .

[17]  V. D. Petrikov,et al.  Photoluminescence Stokes shift and exciton fine structure in CdTe nanocrystals , 2001 .

[18]  K. Misawa,et al.  Quenching of the superradiative decay by confined acoustic-phonons in CdS microcrystallites , 1991 .

[19]  Ghassan E. Jabbour,et al.  PbS quantum-dot doped glasses as saturable absorbers for mode locking of a Cr:forsterite laser , 1997 .

[20]  Transient optical properties of novel PbS nanoparticles coated with 2,6-O-diallyl-β-CD , 1999 .

[21]  Alessandro Martucci,et al.  Microstructural and nonlinear optical properties of silica–titania sol-gel film doped with PbS quantum dots , 1999 .

[22]  B. G. Potter,et al.  Quantum confinement effects on the photoluminescence spectra of CdTe nanocrystallites , 1996 .

[23]  John D. Mackenzie,et al.  Zirconia-ormosil films doped with PbS quantum dots , 1999 .

[24]  Frank W. Wise,et al.  Synthesis and characterization of PbSe quantum dots in phosphate glass , 1997 .

[25]  J. Boilot,et al.  Metal, semiconductor and magnetic nanoparticle inclusions in gels , 1994 .

[26]  B. Ridley Quantum Processes in Semiconductors , 1982 .