Controlling fluorescence emission of single molecules by vibrational excitation (B03)

我们研究了单分子振动态受控激发后的荧光发射。在我们的激发方案中，荧光发射将通过振动激发来切换。使用了两种实现方式：i)振动态的非线性光学激发和ii)振动的直接红外激发。由于对称性的限制，这两种方案是互补的，并解决了不同的振动态。在任何一种情况下，对超快振动弛豫现象的时间分辨监测都是可能的。这两种方法都将在单分子的基础上用于研究聚合物薄膜的局域非均质性。

We study the fluorescence emission of single molecules after controlled excitation of their vibrational states. In our excitation scheme, fluorescence emission will be switched by vibrational excitation. Two implementations are used: i) Non-linear optical excitation of vibrational states and ii) direct infrared excitation of vibrations. Due to symmetry constraints, both schemes are complementary and address different vibrational states. In either case, time-resolved monitoring of ultrafast vibrational relaxation phenomena is possible. Both methods will be used to study local heterogenei-ties in thin polymer films on basis of single molecules.