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

Prokhorenko, V., Halpin, A., & Miller, R. J. D. (2011). Coherently-controlled two-dimensional spectroscopy: Evidence for phase induced long-lived memory effects. Faraday Discussions, 153, 27-39. doi:10.1039/C1FD00095K.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-1F7C-1 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-1F7D-0
Genre: Journal Article

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http://dx.doi.org/10.1039/C1FD00095K (Publisher version)
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 Creators:
Prokhorenko, Valentyn1, 2, Author              
Halpin, Alexei3, Author
Miller, R. J. Dwayne1, 2, 3, Author              
Affiliations:
1Atomically Resolved Structural Dynamics Division, Max Planck Research Department for Structural Dynamics, Department of Physics, University of Hamburg, External Organizations, ou_2173636              
2Center of Free Electron Laser Science, Notkestr. 85, Hamburg, Germany , ou_persistent22              
3University of Toronto, The Departments of Chemistry and Physics, 80 St. George St., Toronto, Canada , ou_persistent22              

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Free keywords: Coherence and Control in Chemistry
 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 ωt 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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Language(s): eng - English
 Dates: 2011-05-232011-05-252011-09-092011-10-25
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1039/C1FD00095K
 Degree: -

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Title: Faraday Discussions
  Abbreviation : Faraday Discuss.
Source Genre: Journal
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Publ. Info: London : Royal Society of Chemistry
Pages: - Volume / Issue: 153 Sequence Number: - Start / End Page: 27 - 39 Identifier: ISSN: 1359-6640
CoNE: /journals/resource/954925269326