Ultrabroadband two-dimensional electronic spectroscopy in the pump–probe geometry using conventional optics

We report ultrabroadband two-dimensional electronic spectroscopy (2D ES) measurements obtained in the pump–probe geometry using conventional optics. A phase-stabilized Michelson interferometer provides the pump-pulse delay interval, τ₁, necessary to obtain the excitation-frequency dimension. Spectral resolution of the probe beam provides the detection-frequency dimension, ω₃. The interferometer incorporates active phase stabilization via a piezo stage and feedback from interference of a continuous-wave reference laser detected in quadrature. To demonstrate the method, we measured a well-characterized laser dye sample and obtained the known peak structure. The vibronic peaks are modulated as a function of the waiting time, τ₂, by vibrational wave packets. The interferometer simplifies ultrabroadband 2D ES measurements and analysis.