Abstract

With high-efficiency fluorescence excitation techniques optical spectra of single impurity molecules of perylene in a polyethylene matrix can be obtained at 1.5 K. Analysis of such spectra shows a variety of spectral diffusion effects, including fast (<2 s) resonance frequency changes on the 1–100-MHz scale, which lead to a range of apparent linewidths, as well as discontinuous jumps in the resonance frequency of 10–1000 MHz on a longer time scale. In addition, light-induced changes in the resonance frequency of a single molecule (persistent spectral hole burning) have been conclusively observed by showing that the burning time decreases with increased laser power. Surprisingly, hole-burned single molecules often spontaneously return to the original frequency in 1–100 s. Measurements of the burning time for a large number of hole-burning events for the same single molecule yield an exponential burn-time distribution, which is the first direct measurement to our knowledge of the stochastic kinetics of a single molecule. Analysis of the signal-to-noise function appropriate to these experiments gives the conditions under which other systems may permit single-molecule detection: strong absorption, high fluorescence yield, weak bottlenecks in the optical pumping process, and low hole-burning quantum efficiency.

© 1992 Optical Society of America

Full Article  |  PDF Article
More Like This
Fluorescence excitation of single molecules

H. Talon, L. Fleury, J. Bernard, and M. Orrit
J. Opt. Soc. Am. B 9(5) 825-828 (1992)

Persistent infrared spectral hole burning of the fundamental stretching mode of SH in alkali halides

C. E. Mungan and A. J. Sievers
J. Opt. Soc. Am. B 9(5) 746-752 (1992)

References

You do not have subscription access to this journal. Citation lists with outbound citation links are available to subscribers only. You may subscribe either as an Optica member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Login to access Optica Member Subscription

Cited By

You do not have subscription access to this journal. Cited by links are available to subscribers only. You may subscribe either as an Optica member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Login to access Optica Member Subscription

Figures (9)

You do not have subscription access to this journal. Figure files are available to subscribers only. You may subscribe either as an Optica member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Login to access Optica Member Subscription

Equations (2)

You do not have subscription access to this journal. Equations are available to subscribers only. You may subscribe either as an Optica member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Login to access Optica Member Subscription

Metrics

You do not have subscription access to this journal. Article level metrics are available to subscribers only. You may subscribe either as an Optica member, or as an authorized user of your institution.

Contact your librarian or system administrator
or
Login to access Optica Member Subscription