Atomically resolved single-molecule triplet quenching
Atomically resolved single-molecule triplet quenching
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DOI：
10.1126/science.abh1155
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发表时间：
2021-07-23
期刊：
影响因子：
56.9
通讯作者：
Repp, Jascha
中科院分区：
文献类型：
--
作者：
Peng, Jinbo;Sokolov, Sophia;Repp, Jascha
分子的非平衡三重态在光催化、有机光伏和光动力治疗中发挥着重要作用。我们报告了通过在原子力显微镜中引入电子泵浦探针方法，以原子分辨率直接测量绝缘表面上单个并五苯分子的三重态寿命。如果氧分子紧密共吸附，就会观察到三线态寿命的强烈猝灭。通过单分子操纵技术，创建了氧分子的不同排列并以原子精度表征，从而使分子排列与猝灭三重态的寿命直接相关。这种对单分子的长寿命三联体的电寻址与原子尺度的操纵相结合，为控制和研究局部自旋-自旋相互作用提供了以前未探索过的途径。
The nonequilibrium triplet state of molecules plays an important role in photocatalysis, organic photovoltaics, and photodynamic therapy. We report the direct measurement of the triplet lifetime of an individual pentacene molecule on an insulating surface with atomic resolution by introducing an electronic pumpprobe method in atomic force microscopy. Strong quenching of the triplet lifetime is observed if oxygen molecules are coadsorbed in close proximity. By means of single-molecule manipulation techniques, different arrangements with oxygen molecules were created and characterized with atomic precision, allowing for the direct correlation of molecular arrangements with the lifetime of the quenched triplet. Such electrical addressing of long-lived triplets of single molecules, combined with atomic-scale manipulation, offers previously unexplored routes to control and study local spin-spin interactions.