Time-Resolved Photoemission Electron Microscopy: Development and Applications

Abstract: Time-resolved photoemission electron microscopy (TR-PEEM) belongs to a class of experimental techniquescombining the spatial resolution of electron-based microscopy with the time resolution of ultrafast opticalspectroscopy. This combination provides insight into fundamental processes on the nanometer spatial andfemto/picosecond time scale, such as charge carrier transport in semiconductors or collective excitations ofconduction band electrons at metal surfaces. The high spatiotemporal resolution also offers a detailed view of therelationship between local structure and ultrafast photoexcitation dynamics in nanostructures and nanostructuredmaterials, which is beneficial in exploring new materials and applications in opto-electronics and nano-optics.This thesis describes the investigation of ultrafast photoexcitation dynamics in metal- and III-V semiconductornanostructures using TR-PEEM. We investigate hot carrier cooling in individual InAs nanowires where we findevidence that electron-hole scattering strongly contributes to the intra-band energy relaxation of photoexcitedelectrons on a sub-picosecond time scale and we observe ultrafast hot electron transport towards the nanowiresurface due to an in-built electric field. We demonstrate the combination of TR-PEEM with optical time-domainspectroscopy to enable time- and excitation frequency-resolved PEEM imaging. The technique is applied to GaAssubstrates and nanowires. TR-PEEM is further used to investigate localized and propagating surface plasmonpolaritons. We explore the optical properties of disordered, porous gold nano-particles (nanosponges). Using TRPEEM,we can resolve several plasmonic hotspots with different resonance frequencies and lifetimes within singlenanosponges. We also explore excitation and temporal control of surface plasmon polaritons by means of singlelayeredcrystals of the transition metal dichalcogenide WSe2.In addition, this thesis includes developments in ultrafast optics, aiming to expand the capabilities of the TR-PEEMsetup. We present a setup for generating tunable broadband ultraviolet (UV) laser pulses via achromatic secondharmonic generation. The setup is suitable for operation at high repetition rates and low pulse energies due to its highconversion efficiency. Further, we describe a transmission grating-based interferometer for the generation of stable,phase-locked pulse pairs. Pulse shaping based on liquid crystal technology allows accurate control over the temporalshape of femtosecond laser pulses. We characterize Fabry-Perot interferences affecting the accuracy of such pulseshapers, and we demonstrate a calibration scheme to compensate for these interference effects.