Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe 2-x Crystals

Mahjouri-Samani, Masoud; Liang, Liangbo; Oyedele, Akinola; Kim, Yong-Sung; Tian, Mengkun; Cross, Nicholas; Wang, Kai; Lin, Ming-Wei; Boulesbaa, Abdelaziz; Rouleau, Christopher M.; Puretzky, Alexander A.; Xiao, Kai; Yoon, Mina; Eres, Gyula; Duscher, Gerd; Sumpter, Bobby G.; Geohegan, David B.

doi:10.1021/acs.nanolett.6b02263

Title: Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe _2-x Crystals

Journal Article · Fri Jan 01 00:00:00 EST 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.6b02263· OSTI ID:1324108

Mahjouri-Samani, Masoud ^[1]; Liang, Liangbo ^[1]; Oyedele, Akinola ^[2]; Kim, Yong-Sung ^[3]; Tian, Mengkun ^[4]; Cross, Nicholas ^[4]; Wang, Kai ^[1]; Lin, Ming-Wei ^[1]; Boulesbaa, Abdelaziz ^[1]; Rouleau, Christopher M. ^[1]; Puretzky, Alexander A. ^[1]; Xiao, Kai ^[1]; Yoon, Mina ^[1]; Eres, Gyula ^[5]; Duscher, Gerd ^[6]; Sumpter, Bobby G. ^[1]; Geohegan, David B. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Korea Research Institute of Standards and Science, Daejeon (Korea); Korea University of Science and Technology, Daejeon (Korea)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Defect engineering has been a critical step in controlling the transport characteristics of electronic devices, and the ability to create, tune, and annihilate defects is essential to enable the range of next-generation devices. Whereas defect formation has been well-demonstrated in three-dimensional semiconductors, similar exploration of the heterogeneity in atomically thin two-dimensional semiconductors and the link between their atomic structures, defects, and properties has not yet been extensively studied. In this paper, we demonstrate the growth of MoSe_2–x single crystals with selenium (Se) vacancies far beyond intrinsic levels, up to ~20%, that exhibit a remarkable transition in electrical transport properties from n- to p-type character with increasing Se vacancy concentration. A new defect-activated phonon band at ~250 cm^-1 appears, and the A_1g Raman characteristic mode at 240 cm^-1 softens toward ~230 cm^-1 which serves as a fingerprint of vacancy concentration in the crystals. We show that post-selenization using pulsed laser evaporated Se atoms can repair Se-vacant sites to nearly recover the properties of the pristine crystals. Finally, first-principles calculations reveal the underlying mechanisms for the corresponding vacancy-induced electrical and optical transitions.

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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), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1324108

Journal Information:: Nano Letters, Vol. 16, Issue 8; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 109 works

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Title: Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe _2-x Crystals