RESUMEN
When electronically excited CO(a(3)Π) collides with a Au(111) surface, electron emission can be observed with a quantum efficiency of 0.13. We have studied the influence of Ar, Kr and Xe adsorption on the electron emission efficiency resulting from CO(a(3)Π) quenching. Surprisingly, a single monolayer (ML) of rare gas dramatically enhances electron emission. For Ar and Kr bilayers, emission efficiency is further enhanced and approaches unity. The quenching mechanism involves electron transfer from the metal to the CO(a(3)Π) molecule followed by electron emission from the molecule. The enhanced emission efficiency is due to the long range nature of the initial electron transfer process and the rare gas adlayer's ability to reflect the electron emitted by the transient CO anion. This work shows that CO(a(3)Π) quenching is a useful model system for investigating the fate of electronically excited molecules at surfaces.
RESUMEN
High harmonic generation (HHG) makes it possible to measure spin and charge dynamics in materials on femtosecond to attosecond timescales. However, the extreme nonlinear nature of the high harmonic process means that intensity fluctuations can limit measurement sensitivity. Here we present a noise-canceled, tabletop high harmonic beamline for time-resolved reflection mode spectroscopy of magnetic materials. We use a reference spectrometer to independently normalize the intensity fluctuations of each harmonic order and eliminate long term drift, allowing us to make spectroscopic measurements near the shot noise limit. These improvements allow us to significantly reduce the integration time required for high signal-to-noise (SNR) measurements of element-specific spin dynamics. Looking forward, improvements in the HHG flux, optical coatings, and grating design can further reduce the acquisition time for high SNR measurements by 1-2 orders of magnitude, enabling dramatically improved sensitivity to spin, charge, and phonon dynamics in magnetic materials.
RESUMEN
The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds.