Imaging and time-resolved spectroscopy of single molecules at an interface
Imaging and time-resolved spectroscopy of single molecules at an interface
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DOI：
10.1126/science.272.5259.255
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发表时间：
1996-04-12
期刊：
影响因子：
56.9
通讯作者：
Brus, LE
中科院分区：
文献类型：
--
作者：
Macklin, JJ;Trautman, JK;Brus, LE
远场显微镜用于无创测量位于聚合物-空气界面上的单个染料分子的室温光学特性。由于局部变化的分子环境的扰动而引起的荧光光谱的变化以及跃迁偶极矩的方向与激发态寿命的变化相关。寿命对光谱偏移的依赖性被认为是由自发发射率的频率依赖性引起的。发现寿命对偶极子方向的依赖性是聚合物-空气界面处荧光辐射的电磁边界条件的结果。
Far-field microscopy was used to noninvasively measure the room-temperature optical properties of single dye molecules located on a polymer-air interface. Shifts in the fluorescence spectrum, due to perturbation by the locally varying molecular environment, and the orientation of the transition dipole moment were correlated to variation in the excited-state lifetime. The lifetime dependence on spectral shift is argued to result from the frequency dependence of the spontaneous emission rate; the lifetime dependence on dipole orientation was found to be a consequence of the electromagnetic boundary conditions on the fluorescent radiation at the polymer-air interface.