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Chemical Stabilization of 1T ' Phase Transition Metal Dichalcogenides with Giant Optical Kerr Nonlinearity

TitleChemical Stabilization of 1T ' Phase Transition Metal Dichalcogenides with Giant Optical Kerr Nonlinearity
Publication TypeJournal Article
Year of Publication2017
AuthorsTan, Sherman J. R., Abdelwahab Ibrahim, Ding Zijing, Zhao Xiaoxu, Yang Tieshan, Loke Gabriel Z. J., Lin Han, Verzhbitskiy Ivan, Poh Sock Mui, Xu Hai, Nai Chang Tai, Zhou Wu, Eda Goki, Jia Baohua, and Loh Kian Ping
JournalJ. Am. Chem. Soc.
Volume139
Pagination2504–2511
Date Published02/2017
ISSN0002-7863
Keywordsatomic mechanism, contacts, intercalation chemistry, lattice-dynamics, molybdenum-disulfide, mos2 monolayer, mote2, ws2
Abstract

The 2H-to-1T' phase transition in transition metal dichalcogenides (TMDs) has been exploited to phase engineer TMDs for applications in which the metallicity of the 1T' phase is beneficial. However, phase-engineered 1T'-TMDs are metastable; thus, Stabilization of the 1T' phase remains an important challenge to overcome before its properties can be exploited. Herein, we performed a systematic study of the 2H-to-IT' phase evolution by lithiation in ultrahigh vacuum. We discovered that:by hydrogenating the intercalated Li to form lithium hydride (LiH), unprecedented longterm ({\textgreater}3 months) air stability of the 1T1 phase can be achieved. Most importantly, this passivation method has wide applicability for other alkali: metalS and TMDs. Density functional theory calculations' reveal that LiH is a good electron donor and stabilizes the IT' phase against 2H conversion, aided by the formation of a greatly enhanced interlayer dipole dipole interaction. Nonlinear optical studies reveal that air-stable 1T'-TMDs exhibit much stronger optical Kerr nonlinearity and higher optical transparency than the 2H phase, which is prornising for nonlinear photonic applications.

DOI10.1021/jacs.6b13238

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