Intensity fluctuation spectroscopy of small numbers of dye molecules in a microcavity

Abstract

The spontaneous emission from a thin layer of a dilute solution of fluorescent dye molecules within an optical microcavity has been studied. Strong fluctuations in fluorescence intensity are observed when the average number of molecules in the measurement volume is small. We have performed experiments that simultaneously characterize these fluctuations over nine orders of magnitude of time, from ns to s. These measurements have identified photon antibunching characteristic of single-molecule emission, along with triplet-state shelving and diffusion driven number fluctuations. The results give fundamental information on the kinetics of dye molecules and allow one to speculate about the prospect of using single molecules as sources of single photons for quantum optics. ͓S1050-2947͑98͒00107-3͔

Single-photon emitting diode in silicon carbide

“…Such a process may involve, for example, a two-step carrier capturing process. The equation that is used to fit the PL data is a double exponential, which is commonly used for three level systems 25 . A standard analysis based on such a system yields a relatively fast excited state lifetime of t PL L ¼ 3:3 AE 0:3 ns with transitions to a dark state every 10 cycles.…”

Controlling the properties of single photon emitters via the Purcell effect

“…This expression has been first applied to dye molecules. 26 In order to account for the background emission, that gives a nonzero g (2) (0) value, we modify Eq. (2) as follows:…”

“…It has been observed in molecules 26,30 and diamond centers 9,31 as well as in semiconductor QDs. 32 It is generally attributed to part-time occupation of the exciton in a metastable, nonradiative state.…”

Observation of Nonclassical Photon Statistics due to Quantum Interference

“…Since then, such a nonclasical effect has been observed in the fluorescence in a variety of systems consisting of a small number of atoms, ions and molecules [2][3][4]. Recently, potential application in quantum cryptography has renewed the interest in producing anti-bunched photon source [5][6][7][8][9][10][11][12]. …”