Quantum process tomography by 2D fluorescence spectroscopy

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.,...

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Veröffentlicht in:The Journal of chemical physics 2015-06, Vol.142 (21), p.212442-212442
Hauptverfasser: Pachón, Leonardo A, Marcus, Andrew H, Aspuru-Guzik, Alán
Format: Artikel
Sprache:eng
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Zusammenfassung: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.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4919954