Phase cycling schemes for two-dimensional optical spectroscopy with a pump-probe beam geometry

We present phase cycling schemes for two-dimensional (2D) optical spectroscopy with a pump-probe beam geometry. We detail the theoretical derivation on how the phase cycling schemes measure a pure absorptive 2D spectrum. The 'rotating frame' is inherent in such phase locked phase cycling experiments, and can increase the efficiency of the experiment by reducing the number of data points needed to be collected. 2D optical spectra are simulated for the phase cycling pump-probe experiment by solving the Liouville equation that describes the system-field interaction using a non-perturbative method.