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Journal of Luminescence

Frequency-domain gratings by simultaneous absorption of two photons

Aleksander K. Rebane, Mikhail A. Drobizhev, Aliaksandr Karotki

Published Jul 1, 2002• 11 citations
Publisher
DOI
10.1016/s0022-2313(02)00289-2

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Summary from only given. We have shown recently that spectral gratings can be created upon simultaneous two-photon absorption (TPA) from a pair of femtosecond pulses. In this paper we study, for the first time to our knowledge, the dependence of the frequency-domain grating on the shape of homogeneous absorption spectrum of two-photon transition. We take advantage of the complete absence of Rayleigh scattering at twice the excitation frequency, which allows us to measure resonance fluorescence spectrum as a function of temperature.
For the first time a frequency-domain grating is observed in the visible region as a result of coherence excited by two-photon absorption of time-delayed near-IR femtosecond pulses in an inhomogeneously broadened organic solid-state system. The grating appears in chlorin (2,3-dihydroporphyrin)-doped polymer film at low temperature and is detected in two different ways. First, modulation is observed in the pure electronic fluorescence band upon 'resonant' two-photon excitation with laser carrier frequency equal to one-half of the fluorescence band maximum. Second, upon long exposure time at half of the transition frequency, a persistent spectral hole with periodic structure is observed. The two-photon absorption spectrum of the chlorin molecule in the spectral range 1130–1310nm is also presented for the first time.