Tracing the steps of photoinduced chemical reactions in organic molecules by coherent two-dimensional electronic spectroscopy using triggered exchange.

Tracing the steps of photoinduced chemical reactions in organic molecules by coherent two-dimensional electronic spectroscopy using triggered exchange.
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利用触发交换相干二维电子光谱追踪有机分子中光诱导化学反应的步骤

DOI:
10.1103/physrevlett.110.148305
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发表时间:
2013
影响因子:
8.6
通讯作者:
T. Brixner
T. Brixner
中科院分区:
物理与天体物理1区
文献类型:
--
作者:
S. Ruetzel;M. Kullmann;J. Buback;P. Nuernberger;T. Brixner

文献摘要

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我们建立了相干触发交换二维(TE 2D)电子光谱作为泵浦-再泵浦-探测瞬态吸收光谱的扩展,并独特地阐明了高躺电子态在超快光化学中的作用。作为一个例子,这是证明存在于两个开环构象的分子开关。观察到一个新物种-自由基阳离子的形成,并通过TE 2D确定其前体状态。
We establish coherent triggered-exchange two-dimensional (TE2D) electronic spectroscopy as an expansion of pump-repump-probe transient absorption spectroscopy and uniquely elucidate the role of higher-lying electronic states in ultrafast photochemistry. As an example, this is demonstrated for a molecular switch present in two ring-open conformations. The formation of a new species—the radical cation—is observed and its precursor state is identified via TE2D.