Fluorescence intermittency in single cadmium selenide nanocrystals

SEMICONDUCTOR nanocrystals offer the opportunity to study the evolution of bulk materials properties as the size of a system increases from the molecular scale1,2. In addition, their strongly size-dependent optical properties render them attractive candidates as tunable light absorbers and emitters in optoelectronic devices such as light-emitting diodes3,4 and quantum-dot lasers5,6, and as optical probes of biological systems7. Here we show that light emission from single fluorescing nanocrystals of cadmium selenide under continuous excitation turns on and off intermittently with a characteristic timescale of about 0.5 seconds. This intermittency is not apparent from ensemble measurements on many nanocrystals. The dependence on excitation intensity and the change in on/off times when a passivating, high-bandgap shell of zinc sulphide encapsulates the nanocrystal8,9 suggests that the abrupt turning off of luminescence is caused by photo-ionization of the nanocrystal. Thus spectroscopic measurements on single nanocrystals can reveal hitherto unknown aspects of their photophysics.

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

[2]  R. Griffin,et al.  Investigation of the surface morphology of capped CdSe nanocrystallites by 31P nuclear magnetic resonance , 1994 .

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

[4]  M. Orrit,et al.  Photon bunching in the fluorescence from single molecules: A probe for intersystem crossing , 1993 .

[5]  M. Bawendi,et al.  Electroluminescence from CdSe quantum‐dot/polymer composites , 1995 .

[6]  C. Weisbuch Recent progress in III–V quantum optoelectronic devices , 1994 .

[7]  C. Bräuchle,et al.  Direct spectroscopic observation of quantum jumps of a single molecule , 1995, Nature.

[8]  P. Roussignol,et al.  New results on optical phase conjugation in semiconductor-doped glasses , 1987 .

[9]  Louis E. Brus,et al.  Nucleation and Growth of CdSe on ZnS Quantum Crystallite Seeds and Vice Versa, in Inverse Micelle Media , 1990 .

[10]  Norris,et al.  Measurement and assignment of the size-dependent optical spectrum in CdSe quantum dots. , 1996, Physical review. B, Condensed matter.

[11]  A. Alivisatos Semiconductor Clusters, Nanocrystals, and Quantum Dots , 1996, Science.

[12]  M. G. Ivanov,et al.  Auger ionization of semiconductor quantum drops in a glass matrix , 1990 .

[13]  L. Brus,et al.  Quantum crystallites and nonlinear optics , 1991 .

[14]  A. Alivisatos,et al.  Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer , 1994, Nature.

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

[16]  W. P. Ambrose,et al.  Detection and spectroscopy of single pentacene molecules in a p‐terphenyl crystal by means of fluorescence excitation , 1991 .

[17]  D. Ledbetter,et al.  Multicolor Spectral Karyotyping of Human Chromosomes , 1996, Science.

[18]  Louis E. Brus,et al.  Imaging and Time-Resolved Spectroscopy of Single Molecules at an Interface , 1996, Science.

[19]  Cook,et al.  Possibility of direct observation of quantum jumps. , 1985, Physical review letters.