Towards the Reconstruction of Time-dependent Vibronic States from Nonlinear Wavepacket Interferometry Signals

We present one-color nonlinear wavepacket interferometry (WPI) signal calculations for a system of two electronic levels and one vibrational degree of freedom. We consider two cases, a displaced harmonic oscillator system, which can be treated analytically, and a model photodissociative system, whose WPI signal must be calculated by numerical wavepacket propagation. We show how signals obtained with different combinations of intrapulse-pair phase shifts can be combined to isolate the complex-valued overlap between a given one-pulse target wavepacket and a variable three-pulse reference wavepacket. We demonstrate that with a range of inter- and intrapulse-pair delays the complex overlaps and variable reference states can be used to reconstruct the target wavepacket. We compare our results with previous methods for vibronic state reconstruction based on linear WPI and discuss further generalizations of our method.