Nonlinear Optical Responses of Janus MoSSe/MoS2 Heterobilayers Optimized by Stacking Order and Strain
Journal
ACS Nano
Journal Volume
17
Journal Issue
20
Start Page
19877
End Page
19886
ISSN
19360851
1936086X
Date Issued
2023
Author(s)
Zhang, Kunyan
van Thanh, Vuong
Guo, Yunfan
Puretzky, Alexander A.
Geohegan, David B.
Kong, Jing
Huang, Shengxi
Saito, Riichiro
Abstract
Nonlinear optical responses in second harmonic generation (SHG) of van der Waals heterobilayers, Janus MoSSe/MoS2, are theoretically optimized as a function of strain and stacking order by adopting an exchange-correlation hybrid functional and a real-time approach in first-principles calculation. We find that the calculated nonlinear susceptibility, χ(2), in AA stacking (550 pm/V) becomes three times as large as AB stacking (170 pm/V) due to the broken inversion symmetry in the AA stacking. The present theoretical prediction is compared with the observed SHG spectra of Janus MoSSe/MoS2 heterobilayers, in which the peak SHG intensity of AA stacking becomes four times as large as AB stacking. Furthermore, a relatively large, two-dimensional strain (4%) that breaks the C3v point group symmetry of the MoSSe/MoS2, enhances calculated χ(2) values for both AA (900 pm/V) and AB (300 pm/V) stackings 1.6 times as large as that without strain.
Subjects
2d Janus Heterobilayers
First-principles Calculations
Second-harmonic Generation
Stacking Effect
Strain Engineering
Time-dependent Density-functional Theory
Density Functional Theory
Nonlinear Optics
Optical Correlation
Van Der Waals Forces
2d Janus Heterobilayer
Exchange Correlations
First Principle Calculations
Nonlinear Optical Response
Stacking Effect
Stacking Order
Stackings
Strain Engineering
Time Dependent Density Functional Theory
Van Der Waal
Harmonic Generation
Article
Density Functional Theory
Prediction
Publisher
American Chemical Society
Type
journal article