Excited and ground state vibrational dynamics revealed by two-dimensional electronic spectroscopy

39Citations
Citations of this article
81Readers
Mendeley users who have this article in their library.
Get full text

Abstract

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. © 2012 American Institute of Physics.

Cite

CITATION STYLE

APA

Caram, J. R., Fidler, A. F., & Engel, G. S. (2012). Excited and ground state vibrational dynamics revealed by two-dimensional electronic spectroscopy. Journal of Chemical Physics, 137(2). https://doi.org/10.1063/1.4733710

Register to see more suggestions

Mendeley helps you to discover research relevant for your work.

Already have an account?

Save time finding and organizing research with Mendeley

Sign up for free