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Quantum process tomography by 2D fluorescence spectroscopy

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4919954· OSTI ID:1370896
 [1];  [2];  [3]
  1. Univ. de Antioquia UdeA, Medellín, (Colombia) Grupo de Física Atómica y Molecular, Inst. de Física, Facultad de Ciencias Exactas y Naturales; Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology
  2. Univ. of Oregon, Eugene, OR (United States). Dept. of Chemistry and Biochemistry, Oregon Center for Optics, and Inst. of Molecular Biology
  3. Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry and Chemical Biology

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. Finally, applications to foundational and applied problems, as well as further extensions, are discussed.

Research Organization:
Energy Frontier Research Centers (EFRC), Washington D.C. (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0001088
OSTI ID:
1370896
Alternate ID(s):
OSTI ID: 1228176
OSTI ID: 22415910
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 142; ISSN JCPSA6; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods book June 2018
Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods journal June 2018
Interplay between structural hierarchy and exciton diffusion in artificial light harvesting journal October 2019
Quantum coherences reveal excited-state dynamics in biophysical systems journal June 2019
Towards a spectroscopic protocol for unambiguous detection of quantum coherence in excitonic energy transport journal January 2020
Secular versus nonsecular Redfield dynamics and Fano coherences in incoherent excitation: An experimental proposal journal January 2018
Quantum process tomography via completely positive and trace-preserving projection journal December 2018
Single-scan acquisition of multiple multidimensional spectra journal January 2019
Secular vs. Non-secular Redfield Dynamics and Fano Coherences in Incoherent Excitation: An Experimental Proposal text January 2017

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