English

Coherent two-dimensional spectroscopy of a Fano model

Chemical Physics 2017-09-06 v4 Atomic Physics Quantum Physics

Abstract

The Fano lineshape arises from the interference of two excitation pathways to reach a continuum. Its generality has resulted in a tremendous success in explaining the lineshapes of many one-dimensional spectroscopies - absorption, emission, scattering, conductance, photofragmentation - applied to very varied systems - atoms, molecules, semiconductors and metals. Unravelling a spectroscopy into a second dimension reveals the relationship between states in addition to decongesting the spectra. Femtosecond-resolved two-dimensional electronic spectroscopy (2DES) is a four-wave mixing technique that measures the time-evolution of the populations, and coherences of excited states. It has been applied extensively to the dynamics of photosynthetic units, and more recently to materials with extended band-structures. In this letter, we solve the full time-dependent third-order response, measured in 2DES, of a Fano model and give the new system parameters that become accessible.

Keywords

Cite

@article{arxiv.1605.08572,
  title  = {Coherent two-dimensional spectroscopy of a Fano model},
  author = {Daniel Finkelstein-Shapiro and Felipe Poulsen and Tõnu Pullerits and Thorsten Hansen},
  journal= {arXiv preprint arXiv:1605.08572},
  year   = {2017}
}