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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, K American Chemical Society 2016 Nano letters Vol.16 No.8
<P>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. Here, we demonstrate the growth of MoSe2-x single crystals with selenium (Se) vacancies far beyond intrinsic levels, up to similar 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 similar to 250 cm(-1) appears, and the A(1g) Raman characteristic mode at 240 cm(-1) softens toward similar to 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 (p)roperties of the pristine crystals. First-principles calculations reveal the underlying mechanisms for the corresponding vacancy induced electrical and optical transitions.</P>