Two-dimensional electronic spectroscopy using incoherent light

Theoretical analysis

Daniel Turner, Dylan J. Howey, Erika J. Sutor, Rebecca A. Hendrickson, M. W. Gealy, Darin J. Ulness

Research output: Contribution to journalArticle

Abstract

Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations in two-dimensional electronic spectroscopy measurements of pigment-protein complexes measured with femtosecond laser pulses. A persistent issue in the field is to reconcile the results of measurements performed using femtosecond laser pulses with physiological illumination conditions. Noisy-light spectroscopy can begin to address this question. In this work we present the theoretical analysis of incoherent two-dimensional electronic spectroscopy, I(4) 2D ES. Simulations reveal diagonal peaks, cross peaks, and coherent oscillations similar to those observed in femtosecond two-dimensional electronic spectroscopy experiments. The results also expose fundamental differences between the femtosecond-pulse and noisy-light techniques; the differences lead to new challenges and new opportunities.

Original languageEnglish (US)
Pages (from-to)5926-5954
Number of pages29
JournalJournal of Physical Chemistry A
Volume117
Issue number29
DOIs
StatePublished - Jul 25 2013

Fingerprint

Ultrashort pulses
Spectroscopy
electronics
spectroscopy
pulses
Photosynthesis
Chromophores
oscillations
Pigments
photosynthesis
Energy transfer
pigments
Lighting
chromophores
lasers
illumination
energy transfer
proteins
Proteins
Experiments

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Turner, D., Howey, D. J., Sutor, E. J., Hendrickson, R. A., Gealy, M. W., & Ulness, D. J. (2013). Two-dimensional electronic spectroscopy using incoherent light: Theoretical analysis. Journal of Physical Chemistry A, 117(29), 5926-5954. https://doi.org/10.1021/jp310477y

Two-dimensional electronic spectroscopy using incoherent light : Theoretical analysis. / Turner, Daniel; Howey, Dylan J.; Sutor, Erika J.; Hendrickson, Rebecca A.; Gealy, M. W.; Ulness, Darin J.

In: Journal of Physical Chemistry A, Vol. 117, No. 29, 25.07.2013, p. 5926-5954.

Research output: Contribution to journalArticle

Turner, D, Howey, DJ, Sutor, EJ, Hendrickson, RA, Gealy, MW & Ulness, DJ 2013, 'Two-dimensional electronic spectroscopy using incoherent light: Theoretical analysis', Journal of Physical Chemistry A, vol. 117, no. 29, pp. 5926-5954. https://doi.org/10.1021/jp310477y
Turner, Daniel ; Howey, Dylan J. ; Sutor, Erika J. ; Hendrickson, Rebecca A. ; Gealy, M. W. ; Ulness, Darin J. / Two-dimensional electronic spectroscopy using incoherent light : Theoretical analysis. In: Journal of Physical Chemistry A. 2013 ; Vol. 117, No. 29. pp. 5926-5954.
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