Bredenbeck Jens, Helbing Jan, Hamm Peter
Physikalisch-Chemisches Institut, Universität Zürich, Winterthurerstr. 190, CH-8057 Zürich, Switzerland.
Phys Rev Lett. 2005 Aug 19;95(8):083201. doi: 10.1103/PhysRevLett.95.083201. Epub 2005 Aug 18.
Transient two-dimensional infrared spectroscopy (2D-IR) on a charge transfer model system is used as a nonlinear probe of solvation dynamics. Unlike what is expected in the linear response case, nonequilibrium relaxation and equilibrium spectral diffusion occur on different time scales. Transient 2D-IR spectroscopy is shown to be sensitive to higher order frequency fluctuation correlation functions, and provides evidence for a coupling between commonly observed fast and slow solvation processes.
在一个电荷转移模型系统上进行的瞬态二维红外光谱(2D-IR)被用作溶剂化动力学的非线性探针。与线性响应情况下的预期不同,非平衡弛豫和平衡光谱扩散发生在不同的时间尺度上。瞬态二维红外光谱对高阶频率涨落相关函数敏感,并为常见的快速和慢速溶剂化过程之间的耦合提供了证据。