Ultrafast exciton transfers in DNA and its nonlinear optical spectroscopy

Kim Hyeon-Deuk, Yoshitaka Tanimura, Minhaeng Cho

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

We have calculated the nonlinear response function of a DNA duplex helix including the contributions from the exciton population and coherence transfers by developing an appropriate exciton theory as well as by utilizing a projector operator technique. As a representative example of DNA double helices, the B -form (dA)10 - (dT)10 is considered in detail. The Green functions of the exciton population and coherence transfer processes were obtained by developing the DNA exciton Hamiltonian. This enables us to study the dynamic properties of the solvent relaxation and exciton transfers. The spectral density describing the DNA base-solvent interactions was obtained by adjusting the solvent reorganization energy to reproduce the absorption and steady-state fluorescence spectra. The time-dependent fluorescence shift of the model DNA system is found to be ultrafast and it is largely determined by the exciton population transfer processes. It is further shown that the nonlinear optical spectroscopic techniques such as photon echo peak shift and two-dimensional photon echo can provide important information on the exciton dynamics of the DNA double helix. We have found that the exciton-exciton coherence transfer plays critical roles in the peculiar energy transfer and ultrafast memory loss of the initially created excitonic state in the DNA duplex helix.

Original languageEnglish
Article number135102
JournalJournal of Chemical Physics
Volume128
Issue number13
DOIs
Publication statusPublished - 2008 Apr 14

Fingerprint

deoxyribonucleic acid
excitons
DNA
spectroscopy
helices
echoes
Photons
Fluorescence
LDS 751
Optical spectroscopy
Hamiltonians
fluorescence
Spectral density
shift
photons
projectors
Green's function
Energy transfer
dynamic characteristics
Green's functions

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

Ultrafast exciton transfers in DNA and its nonlinear optical spectroscopy. / Hyeon-Deuk, Kim; Tanimura, Yoshitaka; Cho, Minhaeng.

In: Journal of Chemical Physics, Vol. 128, No. 13, 135102, 14.04.2008.

Research output: Contribution to journalArticle

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