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Proc Natl Acad Sci U S A. 2011 Oct 25;108(43):17615-20. doi: 10.1073/pnas.1110642108. Epub 2011 Oct 12.

Quantum state and process tomography of energy transfer systems via ultrafast spectroscopy.

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1
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA.

Abstract

The description of excited state dynamics in energy transfer systems constitutes a theoretical and experimental challenge in modern chemical physics. A spectroscopic protocol that systematically characterizes both coherent and dissipative processes of the probed chromophores is desired. Here, we show that a set of two-color photon-echo experiments performs quantum state tomography (QST) of the one-exciton manifold of a dimer by reconstructing its density matrix in real time. This possibility in turn allows for a complete description of excited state dynamics via quantum process tomography (QPT). Simulations of a noisy QPT experiment for an inhomogeneously broadened ensemble of model excitonic dimers show that the protocol distills rich information about dissipative excitonic dynamics, which appears nontrivially hidden in the signal monitored in single realizations of four-wave mixing experiments.

PMID:
21997214
PMCID:
PMC3203777
DOI:
10.1073/pnas.1110642108
[Indexed for MEDLINE]
Free PMC Article
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