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Recently Christensson (Ref.) have reported the TG signals and photon-echo peak shifts of two carotenoids: astaxanthin and lycopene. The experimental results are analyzed based on the model proposed by Brixner (Ref.), which is more rigorous than the model used in this study. The intermediate state Sx is not included in their model calculation, which appears to contradict with our results. The most important aspect of the present study is that the minimum around 50 fs shown in Fig. 3 is reproduced better only when an intermediate state between S2 and S1 is introduced (see Fig. 9).
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When we assume that the coherence is conserved in the S2 → Sx process and then lost subsequently in the Sx → S1 process, the TG signals should be the same as those shown in Fig. 6, but this does not reproduce the experimental results.
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When we assume that the coherence is conserved in the S2 → Sx process and then lost subsequently in the Sx → S1 process, the TG signals should be the same as those shown in Fig. 6, but this does not reproduce the experimental results.
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