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 pump-probe 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.

分子的非平衡三重态在光催化、有机光伏和光动力治疗中起着重要作用。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。如果氧分子在附近共吸附，则观察到三重态寿命的强烈猝灭。通过单分子操作技术，氧分子的不同排列被创造出来，并以原子精度表征，允许分子排列与淬火三重态的寿命直接相关。这种长寿命的单分子三联体的电寻址，结合原子尺度的操作，