Journal of Physical Chemistry

Optical probing of single molecules of terrylene in a Shpol'skii matrix: A two-state single-molecule switch

View publication


We report fluorescence excitation spectra of individual impurity molecules in a new system: terrylene in a Shpol'skii matrix of hexadecane. Studies of optical incoherent saturation, fluorescence microscope images, and resonance frequency changes are reported for the 0-0 electronic transition at 1.7 K. For four stable molecules, the low-power optical line width at 1.7 K is 40 ± 2 MHz full width at half-maximum, the saturation intensity is near 1 W/cm2, and the peak detected count rate can reach 11 000 counts per second. Most single molecules either are stable or require many minutes of irradiation before the resonance frequency changes suddenly, but some show spectral changes on a time scale of seconds. Since higher laser power increases the average rate of frequency shifts, this effect represents a light-driven change in the local environment analogous to nonphotochemical hole-burning in large ensembles. Several two-state molecules have been observed, and a preliminary characterization of this light-driven "molecular switch" has been completed. Multistate behavior also occurs. This work demonstrates that Shpol'skii matrices should provide fertile ground for the generation of a large number of new materials in which single-molecule spectra can be obtained. © 1994 American Chemical Society.