Three-pulse photon echo peak shift

Figure 18. The normalized electronic transition frequency correlation function M(t) 1= S(i)] obtained from the experimental three-pulse photon echo peak shifts and transient grating data for IR144 in ethanol (—) total W(t) ( ) ultrafast Gaussian component in M(t) ( ) oscillatory component that arises from intramolecular vibrational motion.

Fig. 11.12 Dependence of three-pulse photon-echo peak shift on delay time t2, calculated as in Eig. 11.11 using the Kubo relaxation function (Eq. 10.69) with -r = 10, 20 or 40 time units as indicated and a = 0.05 (A) or 0.1 (B) reciprocal time units...

Nagasawa, Y., Watanabe, Y., Takikawa, H., Okada, T. Solute dependence of three pulse photon echo peak shift measurements in methanol solution. J. Phys. Chem. A 107, 632-641 (2003)... 

More reeently, higher-order nonlinear optical measurements such as three-pulse photon eeho peak shift measurements have been carried out to study the SD. Fleming and co-workers studied such three-pulse photon echo from the dye molecule eosin in water. They found that a substantial amplitude (about 60%) of aqueous solvation oecurs within 30 fs. A three-exponential fit (up to 100 ps) to the data of eosin in water yields time eonstants of 17 fs (73%), 330 fs (15%), and 3 ps (12%). Analysis... 

Shortly thereafter came reports of integrated three-pulse photon echoes, especially using the echo peak shift to provide information about spectral diffusion [21, 23]. In one experiment [10, 23] the peak shift shows an intriguing oscillation at short times with a period of about 180 fs, followed by a slower relaxation with a decay time of 1.4 ps. The three-pulse echo amplitude can also be heterodyned, leading to 2DIR experiments [24 26]. The latter experiments provide a wealth of information, and there are several ways to extract the desired spectral diffusion dynamics [149]. 

Figure B2.1.10 Stimulated photon-echo peak-shift (3PEPS) signals. Top pulse sequence and interpulse delays t and T. Bottom echo signals scanned as a function of delay t at three different population periods T, obtained with samples of a tetrapyrrole-containing light-harvesting protein subunit, the a subunit of C-phycocyanin.

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