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Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe2 with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.

Funder: European Commission, When a twist angle is applied between two layered materials (LMs), the registry of the layers and the associated change in their functional properties are spatially modulated, and a moiré superlattice arises. Several works explored the optical, electric, and electromechanical moiré-dependent properties of such twisted LMs but, to the best of our knowledge, no direct visualization and quantification of van der Waals (vdW) interlayer interactions has been presented, so far. Here, we use tapping mode atomic force microscopy phase-imaging to probe the spatial modulation of the vdW potential in twisted hexagonal boron nitride. We find a moiré superlattice in the phase channel only when noncontact (long-range) forces are probed, revealing the modulation of the vdW potential at the sample surface, following AB and BA stacking domains. The creation of scalable electrostatic domains, modulating the vdW potential at the interface with the environment by means of layer twisting, could be used for local adhesion engineering and surface functionalization by affecting the deposition of molecules or nanoparticles.