Calibration of optical parametric amplifiers for frequency-domain ultrafast coherent multidimensional spectroscopic...

Frequency-domain ultrafast coherent multidimensional spectroscopy has made possible a family of fully coherent spectroscopies that can create and interrogate characteristic superpositions of the quantum-mechanical states of a system under investigation. Typical applications include the resolution of couplings and dynamics among multiple electronic states in atoms, molecules, and materials. These methods require scanning the wavelengths of multiple, ultrafast light sources-often optical parametric amplifiers (OPAs). Spectral calibration of the OPA output (a.k.a. wavelength-tuning) involves optimizing the OPA output intensity by adjusting the angles of its component nonlinear crystals and motorized delay stages. When the spectral range addressed in the experiment is large, optimization and control of the one or more OPAs become complex. This work describes an automated calibration strategy that measures the multidimensional configuration-space of a typical 800-nm OPA over all angular and delay degrees-of-freedom in order to create a global tuning curve that spans its dynamic spectral range with optimal power and smooth interpolation. To accomplish this task, the optimization assesses the wavelength-dependent variations to the temporal and spatial characteristics of the OPA output caused by material dispersion so that compensations may be applied during a wavelength scan.