Physics – Quantum Physics
Scientific paper
2010-06-24
Proceedings of the National Academy of Sciences of the United States of America, 2011 108 (43) 17615-17620
Physics
Quantum Physics
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Scientific paper
10.1073/pnas.1110642108
The description of excited state dynamics in multichromophoric systems constitutes both a theoretical and experimental challenge in modern physical chemistry. An experimental protocol which can systematically characterize both coherent and dissipative processes at the level of the evolving quantum state of the chromophores is desired. In this article, we show that a carefully chosen set of polarization controlled two-color heterodyned photon-echo experiments can be used to reconstruct the time-evolving density matrix of the one-exciton manifold of a heterodimer. This possibility in turn allows for a complete description of the excited state dynamics via quantum process tomography (QPT). Calculations on the dimer show that QPT can reveal rich information about system-bath interactions, which otherwise appear nontrivially hidden in the polarization monitored in standard four-wave mixing experiments. Our study presents a novel method for analyzing condensed phase experiments with a quantum information processing perspective.
Aspuru-Guzik Alan
Krich Jacob J.
Mohseni Masoud
Yuen-Zhou Joel
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