Fifth-Order Three-Dimensional Electronic Spectroscopy Using a Pump–Probe Configuration

• Main Authors: Zhang, Zhengyang, Wells, Kym L., Seidel, Marco T., Tan, Howe-Siang
• Other Authors: School of Physical and Mathematical Sciences
• Format: Article
• Language: English
• Published: 2016
• Subjects: Chemistry and Biological Chemistry
• Online Access: https://hdl.handle.net/10356/82240; http://hdl.handle.net/10220/39845
• Institution: Nanyang Technological University

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.