Molecular Coherent Three-Quantum Two-Dimensional Fluorescence Spectroscopy.,The Journal of Physical Chemistry Letters

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Molecular Coherent Three-Quantum Two-Dimensional Fluorescence Spectroscopy.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-06-09 , DOI: 10.1021/acs.jpclett.0c00987
Stefan Mueller ₁ , Tobias Brixner _{1,

2}

Affiliation

We introduce molecular coherent three-quantum (3Q) two-dimensional (2D) fluorescence spectroscopy with phase cycling via shot-to-shot pulse shaping at a 1 kHz repetition rate. This allows us to acquire simultaneously, within a single scan, three fourth-order and six sixth-order signals correlating various one-quantum, two-quantum, and 3Q coherences. We demonstrate the approach on the dye molecule rhodamine 700 and reproduce all nine 2D data sets, including their absolute signal strengths, with simulations using a single, consistent set of model parameters. We observe a linear concentration dependence of all nonlinear signals, evidencing the absence of cascades and many-particle signals of noninteracting molecules. The single-beam, background-free implementation allows direct comparability between various nonlinear signal types and provides information about multiple excited states. Apart from molecules, the method is expected to be applicable to supramolecular systems, polymers, and solid-state materials with the prospect of revealing signatures of bi- and triexcitonic states.

中文翻译：

分子相干三量子二维荧光光谱。

我们介绍了分子相干三量子（3Q）二维（2D）荧光光谱，通过以1 kHz重复频率的逐脉冲成形来实现相位循环。这使我们能够在单次扫描中同时获取三个与各种一量子，二量子和3Q相干性相关的四阶和六阶信号。我们使用染料分子若丹明700演示了该方法，并使用单个一致的模型参数集进行仿真，再现了所有九个2D数据集，包括其绝对信号强度。我们观察到所有非线性信号的线性浓度依赖性，证明不存在级联和非相互作用分子的多粒子信号。单光束无背景实现可实现各种非线性信号类型之间的直接可比性，并提供有关多个激发态的信息。除了分子之外，该方法有望应用于超分子体系，聚合物和固态材料，并有望揭示出双和三正激基态的特征。

更新日期：2020-07-02

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