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Volume 153, 2011
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Coherently-controlled two-dimensional spectroscopy: Evidence for phase induced long-lived memory effects

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Abstract

Using low-intensity phase-shaped excitation pulses we used two-dimensional (2D) electronic spectroscopy to follow the time dependence of the coherent correlations imposed on a solvated organic dye (Rhodamine 101 in methanol) at room temperature. Shaping of the excitation pulses strongly affects both the real and imaginary parts of the 2D-spectra, especially at small waiting times. In particular, the periodic phase modulation of the excitation pulses appears as a two-dimensional grid-like modulation in the correlation spectrum corresponding to the waiting time T = 0. By increasing the waiting time, this modulation quickly disappears in ωt space. However, it is still present in ωτ space even at very long waiting times (≥80 ps) where the inhomogeneous broadening is significantly reduced, and reaches its stationary value of ∼16%. The resonant nature of this induced modulation at long waiting time allows us to conclude that phase shaping of the excitation induces a long-lived memory in solvated organic dyes that is associated with coherent population transfer.

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Article information


Submitted
23 May 2011
Accepted
25 May 2011
First published
09 Sep 2011

Faraday Discuss., 2011,153, 27-39
Article type
Paper

Coherently-controlled two-dimensional spectroscopy: Evidence for phase induced long-lived memory effects

V. I. Prokhorenko, A. Halpin and R. J. D. Miller, Faraday Discuss., 2011, 153, 27
DOI: 10.1039/C1FD00095K

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