Journal
NANO LETTERS
Volume 19, Issue 10, Pages 7317-7323Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b02948
Keywords
exciton diffusion; halos; Auger scattering; hot phonons
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Funding
- Swedish Research Council (VR) [2018-00734]
- European Union's Horizon 2020 research and innovation program [785219]
- Chalmers' Excellence Initiative Nano under its Excellence PhD program
- DFG via Emmy Noether Grant [CH 1672/1-1]
- DFG via Collaborative Research Center [SFB 1277]
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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 nonequilibrium 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. On the basis of 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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