Fifth-Order Three-Dimensional Electronic Spectroscopy Using a Pump–Probe Configuration
Wells, Kym L.
Seidel, Marco T.
Date of Issue2013-06-28
School of Physical and Mathematical Sciences
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.
Chemistry and Biological Chemistry
The Journal of Physical Chemistry B
© 2013 American Chemical Society. This is the author created version of a work that has been peer reviewed and accepted for publication by The Journal of Physical Chemistry B, American Chemical Society. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1021/jp4046403].