21 research outputs found
Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide.
Excitation of ionic solids with extreme ultraviolet pulses creates localized core-level excitons, which in some cases couple strongly to the lattice. Here, core-level-exciton states of magnesium oxide are studied in the time domain at the Mg L_{2,3} edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near-infrared pulses. Combined with a few-state theoretical model, this reveals that the infrared pulse shifts the energy of bright (dipole-allowed) core-level-exciton states as well as induces features arising from dark core-level excitons. We report coherence lifetimes for the two lowest core-level excitons of 2.3±0.2 and 1.6±0.5 fs and show that these are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process
Ultrafast Hidden Spin Polarization Dynamics of Bright and Dark Excitons in 2H-WSe
We performed spin-, time- and angle-resolved extreme ultraviolet
photoemission spectroscopy (STARPES) of excitons prepared by photoexcitation of
inversion-symmetric 2H-WSe with circularly polarized light. The very short
probing depth of XUV photoemission permits selective measurement of
photoelectrons originating from the top-most WSe layer, allowing for direct
measurement of hidden spin polarization of bright and momentum-forbidden dark
excitons. Our results reveal efficient chiroptical control of bright excitons'
hidden spin polarization. Following optical photoexcitation, intervalley
scattering between nonequivalent K-K' valleys leads to a decay of bright
excitons' hidden spin polarization. Conversely, the ultrafast formation of
momentum-forbidden dark excitons acts as a local spin polarization reservoir,
which could be used for spin injection in van der Waals heterostructures
involving multilayer transition metal dichalcogenides
Source noise suppression in attosecond transient absorption spectroscopy by edge-pixel referencing.
Femtosecond Pulse Shaping and Characterization: From Simulation to Experimental Pulse Retrieval Using a Python-Based User Friendly Interface
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Source noise suppression in attosecond transient absorption spectroscopy by edge-pixel referencing.
Attosecond transient absorption spectroscopy (ATAS) is used to observe photoexcited dynamics with outstanding time resolution. The main experimental challenge of this technique is that high-harmonic generation sources show significant instabilities, resulting in sub-par sensitivity when compared to other techniques. This paper proposes edge-pixel referencing as a means to suppress this noise. Two approaches are introduced: the first is deterministic and uses a correlation analysis, while the second relies on singular value decomposition. Each method is demonstrated and quantified on a noisy measurement taken on WS2 and results in a fivefold increase in sensitivity. The combination of the two methods ensures the fidelity of the procedure and can be implemented on live data collection but also on existing datasets. The results show that edge-referencing methods bring the sensitivity of ATAS near the detector noise floor. An implementation of the post-processing code is provided to the reader