Coherent Exciton Dynamics in Supramolecular Light-Harvesting Nanotubes Revealed by Ultrafast Quantum Process Tomography
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Bawendi_Coherent exciton.pdf
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Author(s)
Arias, Dylan H.
Eisele, Dorthe M.
Krich, Jacob J.
Bawendi, Moungi G.
Yuen, Joel
Steiner, Colby Peyton
Nelson, Keith Adam
Aspuru-Guzik, Alan
Date Issued
April 2014
Journal
ACS Nano
Publisher
American Chemical Society (ACS)
Citation
Yuen-Zhou, Joel, Dylan H. Arias, Dorthe M. Eisele, Colby P. Steiner, Jacob J. Krich, Moungi G. Bawendi, Keith A. Nelson, and Alan Aspuru-Guzik. “Coherent Exciton Dynamics in Supramolecular Light-Harvesting Nanotubes Revealed by Ultrafast Quantum Process Tomography.” ACS Nano 8, no. 6 (June 24, 2014): 5527–5534.
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Original manuscript
Abstract
Long-lived exciton coherences have been recently observed in photosynthetic complexes via ultrafast spectroscopy, opening exciting possibilities for the study and design of coherent exciton transport. Yet, ambiguity in the spectroscopic signals has led to arguments against interpreting them in terms of exciton dynamics, demanding more stringent tests. We propose a novel strategy, quantum process tomography (QPT), for ultrafast spectroscopy and apply it to reconstruct the evolving quantum state of excitons in double-walled supramolecular light-harvesting nanotubes at room temperature from eight narrowband transient grating experiments. Our analysis reveals the absence of nonsecular processes, unidirectional energy transfer from the outer to the inner wall exciton states, and coherence between those states lasting about 150 fs, indicating weak electronic coupling between the walls. Our work constitutes the first experimental QPT in a “warm” and complex system and provides an elegant scheme to maximize information from ultrafast spectroscopy experiments.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Research Laboratory of Electronics
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DOI of Published Version
https://doi.org/10.1021/nn406107q
