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In the optical Bloch limit, lifetime (7"i) and dephasing time (7~2) have the following relation: 7/2.ab~' = '/2(7"i.a~' 4- 7"i.t,~'), where 7"2.ab is a dephasing time between the states |a) and |b). T\3 and TU, are the lifetimes of the states. For example, assuming that T\ is 330 fs for both excited vibrational levels, it leads to a 7/2 of 330 fs when both a and b are excited vibrational levels, while 7~2 is 460 fs when one of the states is the vibrational ground state (7~i = 800 fs). '
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78
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84975603474
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Weiner, A. M.; Silvestri, S. D.; Ippen, E. P. J. Opt. Soc. Am. B 1985, 2, 654.
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J. Opt. Soc. Am. B
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Weiner, A.M.1
Silvestri, S.D.2
Ippen, E.P.3
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79
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33751137002
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note
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Within the optical Bloch limit, 2PE (and 3PE) signal decays as exp(-4r/7"2) when the absorption line is inhomogeneously broadened. For a homogeneously broadened line, the 2PE signal decays as exp(-liITi). In between the two limits, the echo signal interpolates in a nonmonotonic way. See ref 50 for. details.
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-
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80
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0001323210
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Nibbering, E. T. J.; Wiersma, D. A.; Duppen, K. Phys. Rev. Lett. 1991, 66, 2464.
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(1991)
Phys. Rev. Lett.
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Nibbering, E.T.J.1
Wiersma, D.A.2
Duppen, K.3
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81
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33750113793
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Vöhringer, P.; Arnett, D. C.; Westervelt, R. A.; Feldstein, M. J.; Scherer, N. F. J. Chem. Phys. 1995, 702, 4027.
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(1995)
J. Chem. Phys.
, vol.702
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Vöhringer, P.1
Arnett, D.C.2
Westervelt, R.A.3
Feldstein, M.J.4
Scherer, N.F.5
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82
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0000393089
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Becker, P. C.; Fragnito, H. L.; Bigot, J. Y.; Brito Cruz, C. H.; Fork, R. L.; Shank, C. V. Phys. Rev. Lett. 1989, 63, 505.
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(1989)
Phys. Rev. Lett.
, vol.63
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Becker, P.C.1
Fragnito, H.L.2
Bigot, J.Y.3
Brito Cruz, C.H.4
Fork, R.L.5
Shank, C.V.6
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83
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0000406731
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Fourkas, J. T.; Brewer, T. R.; Kim, H.;Fayer, M. D. J. Chem. Phys. 1991, 95, 5775.
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J. Chem. Phys.
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Fourkas, J.T.1
Brewer, T.R.2
Kim, H.3
Fayer, M.D.4
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85
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33751123194
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note
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Consider a hole burning experiment applied to an absorption band which has a ~90 fs time constant in M(l). A spectral hole cannot be observed unless the hole-burning experiment has a time resolution better than ~90 fs. In this case, however, the spectrum of the pump (burn) pulse is spectrally wide, and a hole cannot be burnt. In this sense the 90 fs process can be regarded as "homogeneous".
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86
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33751147216
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note
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Actually, both TA and TG are slightly sensitive to the spectral diffusion processes. This sensitivity to spectral diffusion processes arises from the finite pulse duration. When the pulses have finite duration, both R(r>0) and R(r<0) in eq 5 will contribute to the signal via the convolution in eq 6. The rephasing term, 7?(r>0), will be sensitive to T and cause the TA or TG signal to decay, even when the population within the band does not change. This decay due to spectral diffusion (or solvation) in the TA and TG signals, however, is only a small contribution to the signal, and they decay mostly by the population relaxation time. See ref 59 for details.
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87
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0022452961
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(a) Breton, J.; Martin, J.-L.; Migus, A.; Antonetti, A.; Orszag, A. Proc. Nail. Acad. Sci. U.SA. 1986, 83, 5121.
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Proc. Nail. Acad. Sci. U.SA.
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Breton, J.1
Martin, J.-L.2
Migus, A.3
Antonetti, A.4
Orszag, A.5
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88
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0000531711
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(b) Breton, J.; Martin, J.-L.; Fleming, G. R.; Lambry, J.-C. Biochemistry 1988, 27, 8276.
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Biochemistry
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Breton, J.1
Martin, J.-L.2
Fleming, G.R.3
Lambry, J.-C.4
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90
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33845279458
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Creighton, S.; Hwang, J. K.; Warshel, A.; Parson, W. W.; Noms, J. Biochemistry 1988, 27, 774.
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Biochemistry
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Creighton, S.1
Hwang, J.K.2
Warshel, A.3
Parson, W.W.4
Noms, J.5
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91
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0028208909
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Gehlen, J. N.; Marchi, M.; Chandler, D. Science 1994, 263, 499.
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Science
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Gehlen, J.N.1
Marchi, M.2
Chandler, D.3
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