Time-dependent theory of three-step absorption of three light pulses; pp. 54–63Full article in PDF format
The time-dependent theory of the three-step absorption of three different light pulses in the electronic four-level systems is considered using the time-dependent perturbation theory. The first, the second, and the third pulse are in resonance with transitions from level 0 to level 1, from level 1 to level 2, and from level 2 to level 3, respectively. The spectral and temporal behaviour of the probability that the fourth level is excited at the moment of time t depends on the energy relaxation constants of the excited electronic levels, the frequencies of the maxima, the spectral widths (and so the durations) of the light pulses, and the time delays between the pulses. To conclude, there are 12 parameters that affect the spectra in the simple model used. We calculate and analyse the case where the frequencies of the maxima of the first and the second pulse are fixed and the frequency of the maximum of the third pulse varies. On the whole, three lines may exist, one of which corresponds to the coherent contribution and the others do not.
1. Yan, Yi J. and Mukamel, S. Femtosecond pump-probe spectroscopy of polyatomic molecules in condensed phases. Phys. Rev. A, 1990, 41, 6485–6504.
2. Yan, Yi J., Fried, L. E., and Mukamel, S. Ultrafast pump-probe spectroscopy: femtosecond dynamics in Liouville space.
J. Phys. Chem., 1989, 93, 8149–8162.
3. Dobryakov, A. L., Perez Lustres, J. L., Kovalenko, S. A., and Ernsting, N. P. Femtosecond transient absorption with chirped pump and supercontinuum probe: perturbative calculation of transient spectra with general lineshape functions, and simplifications. Chem. Phys., 2008, 347, 127–138.
4. Dobryakov, A. L., Kovalenko, S. A., and Ernsting, N. P. Coherent and sequential contributions to femtosecond transient absorption spectra of a rhodamine dye in solution. J. Chem. Phys., 2005, 123, 044502.
5. Tanasittikosol, M., Carr, C., Adams, C. S., and Wetherill, K. J. Subnatural linewidths in two-photon excited-state spectroscopy. Phys. Rev. A, 2012, 85, 033830.
6. Rebane, I. Time dependent theory of two-step absorption of two pulses. Phys. Lett. A, 2015, 379, 2135–2139.
7. Hizhnyakov, V. and Tehver, I. Theory of resonant secondary radiation due to impurity centres in crystals. Phys. Stat. Sol
., 1967, 21
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