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Optics Communications

Changes in fluorescence lifetimes induced by variation of of the radiating molecules' optical environment

W. Lukosz, Ralf Kunz

Published Oct 1, 1979• 24 citations
Publisher
DOI
10.1016/0030-4018(79)90240-2

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We report the measured dressed lifetimes of fourth-order fluorescence and spontaneous parametric four-wave mixing signals by the perturbation chain method in a two-level and heteronuclear-like molecule system of Pr3+:YSO both in theory and experiment. The lifetime of the fourth-order fluorescence depends on the nonlinear processes in the perturbation chain, and can be modulated by the dark state due to the dressing effect and the induced dipole–dipole interaction by changing the frequency detuning and power of the controlling field. Such results can find potential applications in all-optical communication and optical information processing on photonic chips.
Light–matter coupling-induced hybrid states provide the potential to tune the emission dynamics of molecular chromophores having multilevel systems. We demonstrate the alteration of delayed fluorescence dynamics by hybrid states formation through the interaction of light with a thermally activated delayed fluorescence molecule embedded in a conventional Fabry–Pérot cavity. The proximity of cavity resonance with the excited state absorption is modified by manipulating the incident angles (with sample) instead of varying the active layer thickness. The coupling-induced hybrid states are observed by angle-dependent emission spectroscopy and lifetime measurements. The variation in average emission lifetime with respect to incident angle is over 10 μs and is accompanied by significant changes in the full width at half maxima (factor of three). The control of emission via a barrier-free route or reverse intersystem crossing transition is demonstrated from these measurements. These findings suggest the possibility of tailoring intermediate states for lasing, where exciton density inversion can enhance spontaneous emission.
We have observed optically induced birefringence1 in Ti:AI2O3 at signal wavelengths of 632.8 and 790.7 nm during the course of small-signal gain measurements2 on a Ti:AI2O3 amplifier pumped with 532-nm radiation from a frequency-doubled Q-switched (10-ns pulse) Nd:YAG laser. The changes in intensity of the signal beam due to induced birefringence were found to decay with a time constant characteristic of the fluorescence lifetime of Ti3+ ions. We, therefore, attribute the induced birefringence to the Ti3+ excited-state (2Eg) population.