Single particle versus ensemble average: from power-law intermittency of a single quantum dot to quasistretched exponential fluorescence decay of an ensemble.
Light-induced diffusion-controlled electron transfer is proposed as an underlying mechanism for the intermittency (power law and breakdown) of a single quantum dot and ensemble-averaged fluorescence decay. The intensity decay can be approximated to a stretched exponential expression. The physical links to the free energy gap, reorganization energy, electronic coupling, and diffusion correlation times are discussed. A procedure is described for extracting these molecular-based parameters from experiments and is demonstrated with examples using existing data.
Tang
Jau
J
Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena, CA 91125, USA. jautang@caltech.edu
Marcus
R A
RA