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Optomechanical Tuning of Second Harmonic Generation Anisotropy in Janus MoSSe/MoS2 Heterostructures

Journal Article · · ACS Nano
 [1];  [2];  [3];  [4];  [2];  [5];  [4];  [6];  [7]
  1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Tohoku Univ., Sendai (Japan); National Taiwan Univ., Taipei (Taiwan)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Tohoku Univ., Sendai (Japan); National Taiwan Normal University, Taipei (Taiwan)
  6. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; Kavli Energy NanoScience Institute, Berkeley, CA (United States); University of California, Berkeley, CA (United States)
  7. Rice Univ., Houston, TX (United States)
+ Show Author Affiliations
Symmetry breaking in van der Waals materials enables the realization of quantum states and advanced device functionalities. Janus transition-metal dichalcogenides (TMDs) exhibit distinctive nonlinear optical properties due to their broken out-of-plane mirror symmetry. However, the dynamic control of second harmonic generation (SHG) anisotropy and resonance behavior via optical excitation remains elusive. Here, in this work, we investigate the SHG response of Janus MoSSe/MoS2 heterostructures with 2H and 3R stackings. We can tune the SHG response by varying the incident photon wavelength from 800 to 1000 nm, which shows a resonance-dependent enhancement in intensity and a deviation from 6-fold symmetry, indicating wavelength-dependent anisotropy. The ratio between maximum and minimum intensity in the armchair directions, associated with the SHG anisotropy, reaches a value of 1.73 at the excitation wavelength of 1000 nm. Group theory analysis and first-principles calculations reveal that the observed anisotropy arises from optically induced strain. Our findings highlight the role of symmetry breaking and optical resonance contributing to the optomechanical tuning of SHG anisotropy, offering opportunities for developing Janus TMD-based photonic devices for frequency conversion, light generation, and optical switching.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Organization:
National Science Foundation (NSF); Robert A. Welch Foundation; US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; SC0020042
Other Award/Contract Number:
C-2144
FA2386-24-1-4049
FA9550-22-1-0408
ECCS-1943895
ECCS-2246564
OSTI ID:
3012725
Alternate ID(s):
OSTI ID: 3013950
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 44 Vol. 19; ISSN 1936-086X; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Journal Article · Mon Jul 31 20:00:00 EDT 2023 · Advanced Optical Materials · OSTI ID:1993522

Related Subjects

Janus transition metal dichalcogenides
interlayer coupling
optical resonance
optostriction
second harmonic generation
strain