Suppression of Defects and Deep Levels Using Isoelectronic Tungsten Substitution in Monolayer MoSe2

Li, Xufan; Puretzky, Alexander A.; Sang, Xiahan; KC, Santosh; Tian, Mengkun; Ceballos, Frank; Mahjouri-Samani, Masoud; Wang, Kai; Unocic, Raymond R.; Zhao, Hui; Duscher, Gerd; Cooper, Valentino R.; Rouleau, Christopher M.; Geohegan, David B.; Xiao, Kai

doi:10.1002/adfm.201603850

Suppression of Defects and Deep Levels Using Isoelectronic Tungsten Substitution in Monolayer MoSe₂

Journal Article · Thu May 18 00:00:00 EDT 2017 · Advanced Functional Materials (Online)

DOI:https://doi.org/10.1002/adfm.201603850· OSTI ID:1360047

Li, Xufan ^[1]; Puretzky, Alexander A. ^[1]; Sang, Xiahan ^[1]; KC, Santosh ^[1]; Tian, Mengkun ^[1]; Ceballos, Frank ^[2]; Mahjouri-Samani, Masoud ^[1]; Wang, Kai ^[1]; Unocic, Raymond R. ^[1]; Zhao, Hui ^[2]; Duscher, Gerd ^[3]; Cooper, Valentino R. ^[1]; Rouleau, Christopher M. ^[1]; Geohegan, David B. ^[1]; Xiao, Kai ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Kansas, Lawrence, KS (United States)
Univ. of Tennessee, Knoxville, TN (United States)

Chemical vapor deposition (CVD) is one of the most promising, scalable synthetic techniques to enable large-area synthesis of two-dimensional (2D) transition metal dichalcogenides (TMDs) for the realization of next generation optoelectronic devices. However, defects formed during the CVD growth process currently limit the quality and electronic properties of 2D TMDs. Effective synthesis and processing strategies to suppress defects and enhance the quality of 2D TMDs are urgently needed. In this work, isoelectrnic doping to produce stable alloy is presented as a new strategy to suppress defects and enhance photoluminescence (PL) in CVD-grown TMD monolayers. The random, isoelectronic substitution of W atoms for Mo atoms in CVD-grown monolayers of Mo_1-xW_xSe₂ (02 monolayers. The resultant decrease in defect-medicated non-radiative recombination in the Mo_0.82W_0.18Se₂ monolayers yielded ~10 times more intense PL and extended the carrier lifetime by a factor of 3 compared to pristine CVD-grown MoSe₂ monolayers grown under similar conditions. Low temperatures (4 125 K) PL from defect-related localized states confirms theoretical predictions that isoelectronic W alloying should suppress deep levels in MoSe₂, showing that the defect levels in Mo_1-xW_xSe₂ monolayers are higher in energy and quenched more quickly than in MoSe₂. Isoelectronic substitution therefore appears to be a promising synthetic method to control the heterogeneity of 2D TMDs to realize the scalable production of high performance optoelectronic and electronic devices.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1360047

Journal Information:: Advanced Functional Materials (Online), Journal Name: Advanced Functional Materials (Online) Journal Issue: 19 Vol. 27; ISSN 1616-3028

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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