Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 137, Issue 2, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4733710
Keywords
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Funding
- National Science Foundation (NSF) MRSEC [DMR 08-02054]
- (U.S.) Air Force Office of Scientific Research (USAFOSR) [FA9550-09-1-0117]
- DTRA [HDTRA1-10-1-0091 P00002]
- Defense Advanced Research Projects Agency (DARPA) QuBE [N66001-10-1-4060]
- (U.S.) Department of Energy (DOE) SCGF
- NSF GRFP
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [820054] Funding Source: National Science Foundation
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Broadband two-dimensional electronic spectroscopy (2DES) can assist in understanding complex electronic and vibrational signatures. In this paper, we use 2DES to examine the electronic structure and dynamics of a long chain cyanine dye (1,1-diethyl-4,4-dicarbocyanine iodide, or DDCI-4), a system with a vibrational progression. Using broadband pulses that span the resonant electronic transition, we measure two-dimensional spectra that show a characteristic six peak pattern from coherently excited ground and excited state vibrational modes. We model these features using a spectral density formalism and the vibronic features are assigned to Feynman pathways. We also examine the dynamics of a particular set of peaks demonstrating anticorrelated peak motion, a signature of oscillatory wavepacket dynamics on the ground and excited states. These dynamics, in concert with the general structure of vibronic two-dimensional spectra, can be used to distinguish between pure electronic and vibrational quantum coherences. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4733710]
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