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Title: Isotope Effect in Bilayer WSe2

Journal Article · · Nano Letters
 [1];  [2];  [3]; ORCiD logo [4]
  1. Univ. of Connecticut, Storrs, CT (United States). Dept. of Mechanical Engineering, and Inst. of Materials Science
  2. Univ. of Connecticut, Storrs, CT (United States).Inst. of Materials Science
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Univ. of Connecticut, Storrs, CT (United States). Dept. of Mechanical Engineering, and Inst. of Materials Science; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Isotopes of an element have the same electron number but differ in neutron number and atomic mass. However, due to the thickness-dependent properties in MX2 (M = Mo, W; X = S, Se, Te) transition metal dichalcogenides (TMDs), the isotopic effect in atomically thin TMDs still remains unclear especially for phonon-assisted indirect excitonic transitions. Here, we report the first observation of the isotope effect on the electronic and vibrational properties of a TMD material, using naturally abundant NAWNASe2 and isotopically pure 186W80Se2 bilayer single crystals over a temperature range of 4.4–300 K. We demonstrate a higher optical band gap energy in 186W80Se2 than in NAWNASe2 (3.9 ± 0.7 meV from 4.41 to 300 K), which is surprising as isotopes are neutral impurities. Phonon energies decrease in the isotopically pure crystal due to the atomic mass dependence of harmonic oscillations, with correspondingly longer E2g and A21g phonon lifetimes than in the naturally abundant sample. Finally, the change in electronic band gap renormalization energy is postulated as being the dominant mechanism responsible for the change in optical emission spectra.

Research Organization:
Los Alamos National Laboratory (LANL)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC)
Grant/Contract Number:
89233218CNA000001
OSTI ID:
1499358
Report Number(s):
LA-UR-18-29405
Journal Information:
Nano Letters, Journal Name: Nano Letters Journal Issue: 3 Vol. 19; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (3)

Tunable thermal transport in a WS 2 monolayer with isotopic doping and fractal structure journal January 2019
Locally defined quantum emission from epitaxial few-layer tungsten diselenide journal May 2019
Phonon-polaritonics: enabling powerful capabilities for infrared photonics journal October 2019