Lifetime mapping using femtosecond time-resolved photoemission electron microscopy

Time-resolved photoemission electron microscopy (PEEM) has established itself as a versatile experimental technique to unravel the ultrafast electron dynamics of materials with nanometer-scale resolution. However, the approach of performing PEEM-based, pixel-by-pixel lifetime mapping has not been reported thus far. Herein, we describe in detail the data pre-processing procedure and an algorithm to perform time-trace fittings of each pixel. We impose an energy cutoff for each pixel prior to spectral integration to enhance the robustness of our approach. With the energy cutoff, the energy-integrated time traces show improved statistics and lower fitting errors, thus resulting in a more accurate determination of the fit parameters, e.g., decay time constants. Our work allows us to reliably construct PEEM-based lifetime maps, which potentially shed light on the effects of local microenvironment on the ultrafast processes of the material and allow spatial distributions of lifetimes to be correlated with observables obtained from complementary microscopic techniques, hence enabling a more comprehensive characterization of the material.