2 ABSTRACT: Dominant recombination pathways in monolayer transition metal dichalcogenides (TMDCs) depend primarily on background carrier concentration, generation rate and applied strain. Charged excitons formed in the presence of background carriers mainly recombine nonradiatively. Neutral excitons recombine completely radiatively at low generation rates, but experience nonradiative exciton-exciton annihilation (EEA) at high generation rates. Strain can suppress EEA resulting in near-unity photoluminescence quantum yield (PL QY) at all exciton densities. Although exciton diffusion is the primary channel of energy transport in excitonic materials and a critical optoelectronic design consideration, the combined effects of these factors on exciton diffusion are not clearly understood. In this work, we decouple the diffusion of neutral and charged excitons with chemical counterdoping and explore the effect of strain and generation rate on exciton diffusion. According to the standard semiconductor paradigm a shorter carrier recombination lifetime should lead to a smaller diffusion length. Surprisingly, we find that increasing generation rate shortens the exciton lifetime but increases the diffusion length in unstrained monolayers of TMDCs. When we suppress EEA by strain, both lifetime and diffusion length becomes independent of generation rate. During EEA one exciton nonradiatively recombines and kinetically energizes another exciton, which then diffuses fast. Our results probe concentration dependent diffusion of pure neutral exciton by counterdoping and elucidate how strain controls exciton transport and many-body interactions in TMDC monolayers.
KEYWORDS: WS2, exciton, trion, diffusion, transport, quantum yield, strain
April 25, 2022
Uddin, Shiekh Zia; Higashitarumizu, Naoki; Kim, Hyungjin; Yi, Jun; Zhang, Xiang; Chrzan, Daryl; et al. (1753): Enhanced Neutral Exciton Diffusion in Monolayer WS2 by Exciton–Exciton Annihilation. ACS Publications. Collection. https://doi.org/10.1021/acsnano.2c00956