Exciton trapping is responsible for the long apparent lifetime in acid-treated MoS2

Goodman, A. J.; Willard, A. P.; Tisdale, W. A.

doi:10.1103/physrevb.96.121404

Title: Exciton trapping is responsible for the long apparent lifetime in acid-treated MoS₂

Journal Article · Thu Sep 14 00:00:00 EDT 2017 · Physical Review B

DOI:https://doi.org/10.1103/physrevb.96.121404· OSTI ID:1470496

Goodman, A. J. ^[1]; Willard, A. P. ^[1]; Tisdale, W. A. ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Here, we show that deep trapped “dark” exciton states are responsible for the surprisingly long lifetime of band-edge photoluminescence in acid-treated single-layer MoS₂. Temperature-dependent transient photoluminescence spectroscopy reveals an exponential tail of long-lived states extending hundreds of meV into the band gap. These subband states, which are characterized by a 4 μs radiative lifetime, quickly capture and store photogenerated excitons before subsequent thermalization up to the band edge where fast radiative recombination occurs. By intentionally saturating these trap states, we are able to measure the “true” 150 ps radiative lifetime of the band-edge exciton at 77 K, which extrapolates to ~ 600 ps at room temperature. These experiments reveal the dominant role of dark exciton states in acid-treated MoS₂, and suggest that excitons spend >95 % of their lifetime at room temperature in trap states below the band edge. In this work, we hypothesize that these states are associated with native structural defects, which are not introduced by the superacid treatment; rather, the superacid treatment dramatically reduces nonradiative recombination through these states, extending the exciton lifetime and increasing the likelihood of eventual radiative recombination.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0001088; 1122374

OSTI ID:: 1470496

Alternate ID(s):: OSTI ID: 1390364

Journal Information:: Physical Review B, Vol. 96, Issue 12; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 49 works

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Title: Exciton trapping is responsible for the long apparent lifetime in acid-treated MoS2

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Title: Exciton trapping is responsible for the long apparent lifetime in acid-treated MoS₂