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Nat Mater. 2015 Sep;14(9):889-93. doi: 10.1038/nmat4356. Epub 2015 Jul 13.

Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2.

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Department of Physics, University of Regensburg, D-93040 Regensburg, Germany.
Institute of Physics, University of Münster, D-48149 Münster, Germany.


Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

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