Efficient orbital imaging based on ultrafast momentum microscopy and sparsity-driven phase retrieval

Abstract

We present energy-resolved photoelectron momentum maps for orbital tomography that have been collected with a novel and efficient time-of-flight momentum microscopy setup. This setup is combined with a 0.5 MHz table-top femtosecond extreme-ultraviolet light source, which enables unprecedented speed in data collection and paves the way towards time-resolved orbital imaging experiments in the future. Moreover, we take a significant step forward in the data analysis procedure for orbital imaging, and present a sparsity-driven approach to the required phase retrieval problem, which uses only the number of non-zero pixels in the orbital. Here, no knowledge of the object support is required, and the sparsity number can easily be determined from the measured data. Used in the relaxed averaged alternating reflections algorithm, this sparsity constraint enables fast and reliable phase retrieval for our experimental as well as noise-free and noisy simulated photoelectron momentum map data.