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Volumn 118, Issue 1, 2003, Pages 46-61

Wave packet interferometry for short-time electronic energy transfer: Multidimensional optical spectroscopy in the time domain

Author keywords

[No Author keywords available]

Indexed keywords

DIMERS; ELECTRIC FIELDS; ELECTRON ENERGY LEVELS; ELECTRON SPECTROSCOPY; HAMILTONIANS; MOLECULAR DYNAMICS; MOLECULAR VIBRATIONS; PERTURBATION TECHNIQUES; PHASE SPACE METHODS; POTENTIAL ENERGY; PROBABILITY DENSITY FUNCTION; TIME DOMAIN ANALYSIS;

EID: 0037255309     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.1519259     Document Type: Article
Times cited : (28)

References (109)
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    • For a recent relaxation-theory study of vibrational effects in electronic energy transfer see, M. Yang and G. R. Fleming, Chem. Phys. 275, 355 (2002)
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    • John Jean investigated the short-pulse-driven dynamics of a similar system in contact with a thermal reservoir in a ground-breaking study of the competition between coherence and relaxation in wave packet surface crossing: J. M. Jean, J. Phys. Chem. A 102, 7549 (1998)
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    • For plots of the adiabatic potential energy surfaces of this model under strong and weak couplng, see Fig. 2 of Förster's article (Ref. 35)
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    • FC, the acceptor surface passes through the donor minimum; for continuous spectra this would be the case of maximal "Förster overlap" between donor emission and acceptor absorption. A further redshift in the acceptor absorption spectrum would lead to an inverted regime of decreasing energy-transfer efficiency
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    • note
    • The lower-case subscripts designate "preparation," "waiting," and "delay
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    • Experiments on fluorescence detection of femtosecond accumulated photon echoes have measured a similar quantity that is quadrilinear in the field amplitudes of phase-related continuous wave beams. The time resolution in those experiments was set by the field correlation time of a continuous-wave laser rather than the pulse duration. K. Uchikawa, H. Ohsawa, T. Suga, and S. Saikan, Opt. Lett. 16, 13 (1991)
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    • note
    • We set ℏ = 1 throughout this paper
  • 82
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    • note
    • nO
  • 83
    • 85008331825 scopus 로고    scopus 로고
    • note
    • † = - I
  • 84
    • 85008385628 scopus 로고    scopus 로고
    • note
    • I+H.c
  • 85
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    • note
    • 0>
  • 86
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    • note
    • uπ/2 associated with the energy-transfer process, which our amplitude-sensitive measurements will be able to detect
  • 87
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    • note
    • An experimental strategy for isolating the interference contribution to the population of a given electronic state with beam choppers and lock-in amplifiers was demonstrated in Refs. 1 and 2
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    • note
    • We use notation in which a bra retains the name of the ket to which it is dual:
  • 89
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    • note
    • I
  • 91
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    • note
    • w allows us to regard the interpulse-pair phase shifts as random variables. For a detailed discussion of the relationship between phase shifts and time delays, see Ref. 3
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    • note
    • A rudimentary example of phase-cycling in linear ultrafast spectroscopy can be found in Ref. 2. There it was shown that in-phase and in-quadrature interferograms could be combined to yield the resonant part of the time-dependent linear dipole susceptibility
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    • note
    • x polarization (see Appendix A) is observation-time independent. For both polarization combinations, however, it may be desirable in cases of relatively strong energy-transfer coupling to time gate the measurement of acceptor-state population - on about a picosecond time scale - in order to ensure that the portion linear in J dominates the acceptor-state population
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    • 85008350579 scopus 로고    scopus 로고
    • note
    • d interval of (backwards) motion in state 2. This interesting elementary feature of the transferred amplitude's motion in an energy-transfer system does not seem to have been noted previously
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    • 85008404719 scopus 로고    scopus 로고
    • note
    • vib/2
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    • 85008407595 scopus 로고    scopus 로고
    • note
    • 6. The interference signals presented here supersede the preliminary calculations of D. Kilin and J. A. Cina, Ultrafast Phenomena (Springer, Berlin, in press), Vol. 13, conference proceedings. The latter calculations were performed less accurately, by numerical diagonalization of the one-exciton subspace in the presence of a small specified value for J
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    • note
    • There does not appear to be any fundamental reason why fluorescence-detected wave packet interferometry signals could not be measured on single molecules; in which case the issue of inhomogeneous broadening would be moot if the site energies were stable for the duration of data acquisition
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    • note
    • See Chap. 10 of Shaul Mukamel's book, cited in Ref. 13
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    • note
    • 2 due to electronic energy transfer. The corresponding quadrilinear signal should be resistant to degradation by orientational disorder, and even provide useful amplitude-level information from a randomly oriented sample
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    • note
    • w. It is worth noting that the C and D terms can more generally be separated from each other by phase cycling, which isolates A + D and B + C. See Ref. 26


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