Reconstruction of the dynamics (quantum process tomography) of the single-exciton manifold in energy transfer systems is proposed here on the basis of two-dimensional fluorescence spectroscopy (2D-FS) with phase-modulation. The quantum-process-tomography protocol introduced here benefits from, e.g., the sensitivity enhancement ascribed to 2D-FS. Although the isotropically averaged spectroscopic signals depend on the quantum yield parameter Γ of the doubly-excited-exciton manifold, it is shown that the reconstruction of the dynamics is insensitive to this parameter. Applications to foundational and applied problems, as well as further extensions, are discussed.
@article{arxiv.1502.02363,
title = {Quantum Process Tomography by 2D Fluorescence Spectroscopy},
author = {Leonardo A. Pachon and Andrew H. Marcus and Alan Aspuru-Guzik},
journal= {arXiv preprint arXiv:1502.02363},
year = {2015}
}