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Chemical Physics Letters

Two-dimensional line-shape analysis of photon-echo signal

Ko Okumura, Andrei Tokmakoff, Yoshitaka Tanimura

Published Dec 1, 1999• 57 citations
Publisher
DOI
10.1016/s0009-2614(99)01173-2

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We report photon echoes from two-dimensional (2D) excitons in a GaAs-AlGaAs quantum well structure at 2 K. We analyze our data with a theoretical model of the generation of photon echoes by pulses of finite length which includes phase relaxation during excitation. A line shape analysis yields the phase relaxation time of 2D excitons. We find that the phase coherence near the line center decays, together with the resonant population, within 4 ps, whereas well below line center the phase coherence is conserved for times up to 20 ps.
The time-integrated three-pulse photon echo is discussed in terms of the line-shape functions which are shown to be directly related to the solvation dynamics. By using the short-time approximation to the line-shape function, an algebraic form of the three-pulse photon echo signal S PE (τ, T ) is obtained as a function of two delay times, τ and T, between pulses. On the basis of the approximate form of the photon echo signal, the echo peak shift with respect to the second delay time (population evolution period) is derived and found to be linearly proportional to the time-dependent fluorescence Stokes shift function for times greater than the bath correlation time, τ c . In the case of intermediate inhomogeneous broadening, the asymptotic echo peak shift magnitude is found to be useful in estimating the static inhomogeneous width. To illustrate the theoretical results, an analysis of the echo peak shift measurement of IR144 in a room temperature glass, PMMA, is presented.