通过超快光谱学对能量转移系统的量子态和过程层析成像。
Quantum state and process tomography of energy transfer systems via ultrafast spectroscopy.
机构信息
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA.
出版信息
Proc Natl Acad Sci U S A. 2011 Oct 25;108(43):17615-20. doi: 10.1073/pnas.1110642108. Epub 2011 Oct 12.
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.
摘要
在能量转移系统中，激发态动力学的描述是现代化学物理学的一个理论和实验挑战。人们希望有一种光谱学协议，可以系统地表征被探测发色团的相干和耗散过程。在这里，我们展示了一组双色光子回波实验通过实时重构其密度矩阵来对二聚体的单激子态进行量子态层析（QST）。这种可能性反过来又允许通过量子过程层析（QPT）对激发态动力学进行完整描述。对非均匀展宽的模型激子二聚体集合进行的噪声 QPT 实验的模拟表明，该协议可以提取有关耗散激子动力学的丰富信息，这些信息在单四波混频实验的信号中不易察觉。
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