The low photon energy of driving fields in the multi-terahertz (multi-THz) spectral window has proven particularly suitable to
Searching for quantum functionalities requires access to the electronic structure, constituting the foundation of exquisite spin-valley–electronic, topological, and many-body effects. All-optical band-structure reconstruction could directly connect electronic structure with the coveted quantum phenomena if strong lightwaves transported localized electrons within preselected bands. Here, we demonstrate that harmonic sideband (HSB) generation in monolayer tungsten diselenide creates distinct electronic interference combs in momentum space. Locating these momentum combs in spectroscopy enables super-resolution tomography of key band-structure details in situ. We experimentally tuned the optical-driver frequency by a full octave and show that the predicted super-resolution manifests in a critical intensity and frequency dependence of HSBs. Our concept offers a practical, all-optical, fully three-dimensional tomography of electronic structure even in microscopically small quantum materials, band by band.
Spectroscopic measurements of the hydroxyl (OH) airglow emissions are often used to infer neutral temperatures near the mesopause. Correct Einstein coefficients for the various transitions in the OH airglow are needed to calculate accurate temperatures. However, studies from some studys showed experimentally and theoretically that the most commonly used Einstein spontaneous emission transition probabilities for the Q-branch of the OH Meinel (6,2) transition are overestimated. Extending their work to several Δv = 2 and 3 transitions from v′ = 3 to 9, we have determined Einstein coefficients for the first four Q-branch rotational lines. These have been derived from high resolution, high signal to noise spectroscopic observations of the OH airglow in the night sky from the Nordic Optical Telescope. The Q-branch Einstein coefficients calculated from these spectra show that values currently tabulated in the HITRAN database overestimate many of the Q-branch transition probabilities. The implications for atmospheric temperatures derived from OH Q-branch measurements are discussed.
Ultrafast charge separation after photoexcitation is a common phenomenon in various van-der-Waals (vdW) heterostructures with great relevance for future applications in light harvesting and detection. Theoretical understanding of this phenomenon converges towards a coherent mechanism through charge transfer states accompanied by energy dissipation into strongly coupled phonons. The detailed microscopic pathways are material specific as they sensitively depend on the band structures of the individual layers, the relative band alignment in the heterostructure, the twist angle between the layers, and interlayer interactions resulting in hybridization. We used time- and angle-resolved photoemission spectroscopy combined with tight binding and density functional theory electronic structure calculations to investigate ultrafast charge separation and recombination in WS2-graphene vdW heterostructures. We identify several avoided crossings in the band structure and discuss their relevance for ultrafast charge transfer. We relate our own observations to existing theoretical models and propose a unified picture for ultrafast charge transfer in vdW heterostructures where band alignment and twist angle emerge as the most important control parameters.
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