Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University , 21 Nanyang Link, Singapore 637371.
J Phys Chem B. 2013 Dec 12;117(49):15369-85. doi: 10.1021/jp4046403. Epub 2013 Jul 25.
We present the theoretical details and experimental demonstration of fifth-order three-dimensional (3D) electronic spectroscopy using a pump-probe beam geometry. This is achieved using a pulse shaper and appropriate phase cycling schemes. We show how 8-step and 27-step phase cycling schemes can measure purely absorptive 3D spectra as well as 3D spectra for the individual fifth-order processes that contribute to the purely absorptive spectrum. 3D spectra as a function of two separate controllable waiting time periods can be obtained. The peak shapes and positions of the peaks in the experimental measurement correspond well to theory.
我们提出了使用泵浦-探测光束几何结构的五阶三维（3D）电子光谱的理论细节和实验演示。这是通过脉冲整形器和适当的相位循环方案实现的。我们展示了 8 步和 27 步相位循环方案如何测量纯吸收 3D 光谱以及对纯吸收光谱有贡献的各个五阶过程的 3D 光谱。可以获得两个单独可控等待时间周期的 3D 光谱。实验测量中峰的形状和位置与理论很好地对应。
