At 20 K, optically excited excitons in monolayer WS2 are predicted to exhibit transient negative diffusion, with their spatial distribution narrowing for tens of picoseconds due to intervalley exciton-phonon scattering.
Exciton propagation and halo formation in two-dimensional materials
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abstract
The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.
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cond-mat.mes-hall 1years
2019 1verdicts
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Negative excitonic diffusion in transition metal dichalcogenides
At 20 K, optically excited excitons in monolayer WS2 are predicted to exhibit transient negative diffusion, with their spatial distribution narrowing for tens of picoseconds due to intervalley exciton-phonon scattering.