Imaging theory of structured pump-probe microscopy

Abstract

With sub-micron spatial resolution and femtosecond temporal resolution, pump probe microscopy provides a powerful spectroscopic probe of complex electronic environments in bulk and nanoscale materials. However, the electronic structure of many materials systems are governed by compositional and morphological heterogeneities on length scales that lie below the diffraction limit. We have recently demonstrated Structured Pump Probe Microscopy (SPPM), which employs a patterned pump excitation field to provide spectroscopic interrogation of sub-diffraction limited sample volumes. Herein, we develop the imaging theory of SPPM in two dimensions to accompany the previously published experimental methodology. We show that regardless of pump and probe wavelengths, a nearly two-fold reduction in spectroscopic probe volume can be achieved. We also examine the limitations of the approach, with a detailed discussion of ringing in the point spread function that can reduce imaging performance.