Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems.
Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems.
复制标题
DOI：
10.1103/physrevlett.94.078302
复制
发表时间：
2005-02
影响因子：
8.6
通讯作者：
E. van Dijk;J. Hernando;J. Garcia-Lopez;M. Crego-calama;D. Reinhoudt;L. Kuipers;M. Garcia-Parajo;N. V. van Hulst
中科院分区：
文献类型：
--
作者：
E. van Dijk;J. Hernando;J. Garcia-Lopez;M. Crego-calama;D. Reinhoudt;L. Kuipers;M. Garcia-Parajo;N. V. van Hulst
我们报道了用一种新型的超快单分子泵-探针方法对单个分子进行飞秒时间分辨率的首次实验研究。弛豫时间范围从100到400fs不等，揭示了不同振动模式下的能量再分配以及声子与纳米环境的耦合。处理量子耦合分子，我们发现更长的衰减时间，指向由于离域激发而抑制的分子内衰减。有趣的是，每个单独的系统在飞秒响应中表现出离散的跳跃，反映了耦合超辐射状态的突然破裂。
We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.