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Title: Effects of Vanadium Doping on the Optical Response and Electronic Structure of WS 2 Monolayers
Abstract 2D dilute magnetic semiconductors have been recently reported in transition metal dichalcogenides doped with spin‐polarized transition metal atoms, for example vanadium‐doped WS2monolayers, which exhibit room‐temperature ferromagnetic ordering. However, a broadband characterization of the electronic band structure of these doped WS2monolayers and its dependence on vanadium concentration is still lacking. Therefore, power‐dependent photoluminescence, resonant four‐wave mixing, and differential reflectance spectroscopies are performed here to study optical transitions close to the A exciton energy of vanadium‐doped WS2monolayers at three different doping levels. Instead of a single A exciton peak, vanadium‐doped samples exhibit two photoluminescence peaks associated with transitions from a donor‐like level and the conduction band minima. Moreover, resonant Raman and second‐harmonic generation experiments reveal a blueshift in the B exciton energy but no energy change in the C exciton after vanadium doping. Density functional theory calculations show that the band structure is sensitive to the HubbardUcorrection for vanadium, and several scenarios are proposed to explain the two photoluminescence peaks around the A exciton energy region. This work provides the first broadband optical characterization of these 2D dilute magnetic semiconductors, shedding light on the novel and tunable electronic features of V‐doped WS2 monolayers.  more » « less
Award ID(s):
2039351
PAR ID:
10584861
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
Wiley-VCH GmbH
Date Published:
Journal Name:
Advanced Optical Materials
Volume:
12
Issue:
19
ISSN:
2195-1071
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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