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Direct Observation of Different One- and Two-Photon Fluorescent States in a Pyrrolo[3,2-b]pyrrole Fluorophore.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-05-22 , DOI: 10.1021/acs.jpclett.0c00669 Yangzhong Qin 1 , Christoph Schnedermann 1 , Mariusz Tasior 2 , Daniel T Gryko 2 , Daniel G Nocera 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-05-22 , DOI: 10.1021/acs.jpclett.0c00669 Yangzhong Qin 1 , Christoph Schnedermann 1 , Mariusz Tasior 2 , Daniel T Gryko 2 , Daniel G Nocera 1
Affiliation
Two-photon fluorophores are frequently employed to obtain superior spatial resolution in optical microscopy applications. To guide the rational design of these molecules, a detailed understanding of their excited-state deactivation pathways after two-photon excitation is beneficial, especially to assess the often-assumed presumption that the one- and two-photon excited-state dynamics are similar after excitation. Here, we showcase the breakdown of this assumption for one- and two-photon excitation of a centrosymmetric pyrrolo[3,2-b]pyrrole chromophore by combining time-resolved fluorescence and broadband femtosecond transient absorption spectroscopy. Compared to one-photon excitation, where radiative decay dominates the photodynamics, two-photon excitation leads to dynamics arising from increased nonradiative decay pathways. These different photodynamics are manifest to different quantum yields, thus highlighting the types of time-resolved studies described here to be valuable guideposts in the design of two-photon fluorophores for imaging applications.
中文翻译:
在吡咯并[3,2-b]吡咯荧光团中直接观察到不同的一光子和二光子荧光状态。
在光学显微镜应用中,经常使用两光子荧光团来获得优异的空间分辨率。为了指导这些分子的合理设计,对双光子激发后它们的激发态失活途径的详细了解是有益的,尤其是评估经常假定的假设,即单光子激发后和两个光子激发态动力学相似励磁。在这里,我们展示了中心对称吡咯并[3,2- b结合时间分辨荧光和宽带飞秒瞬态吸收光谱法研究]吡咯发色团。与辐射衰减主导光动力学的单光子激发相比,双光子激发导致非辐射衰减路径增加而产生的动力学。这些不同的光动力学表现为不同的量子产率,因此突出了此处描述的时间分辨研究的类型,这对于设计用于成像应用的双光子荧光团是有价值的指导。
更新日期:2020-06-18
中文翻译:
在吡咯并[3,2-b]吡咯荧光团中直接观察到不同的一光子和二光子荧光状态。
在光学显微镜应用中,经常使用两光子荧光团来获得优异的空间分辨率。为了指导这些分子的合理设计,对双光子激发后它们的激发态失活途径的详细了解是有益的,尤其是评估经常假定的假设,即单光子激发后和两个光子激发态动力学相似励磁。在这里,我们展示了中心对称吡咯并[3,2- b结合时间分辨荧光和宽带飞秒瞬态吸收光谱法研究]吡咯发色团。与辐射衰减主导光动力学的单光子激发相比,双光子激发导致非辐射衰减路径增加而产生的动力学。这些不同的光动力学表现为不同的量子产率,因此突出了此处描述的时间分辨研究的类型,这对于设计用于成像应用的双光子荧光团是有价值的指导。