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Vertically stacked van der Waals (vdW) heterostructures exhibit unique electronic, optical, and thermal properties that can be manipulated by twist-angle engineering. However, the weak phononic coupling at a bilayer interface imposes a fundamental thermal bottleneck for future two-dimensional devices. Using ultrafast electron diffraction, we directly investigated photoinduced nonequilibrium phonon dynamics in MoS2/WS2at 4° twist angle and WSe2/MoSe2heterobilayers with twist angles of 7°, 16°, and 25°. We identified an interlayer heat transfer channel with a characteristic timescale of ~20 picoseconds, about one order of magnitude faster than molecular dynamics simulations assuming initial intralayer thermalization. Atomistic calculations involving phonon-phonon scattering suggest that this process originates from the nonthermal phonon population following the initial interlayer charge transfer and scattering. Our findings present an avenue for thermal management in vdW heterostructures by tailoring nonequilibrium phonon populations.
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Determining the twist angle of stacked MoS 2 layers using machine learning‐assisted low‐frequency interlayer Raman fingerprints
Abstract The investigation of twisted stacked few‐layer MoS2has revealed novel electronic, optical, and vibrational properties over an extended period. For the successful integration of twisted stacked few‐layer MoS2into a wide range of applications, it is crucial to employ a noninvasive, versatile technique for characterizing the layered architecture of these complex structures. In this work, we introduce a machine learning‐assisted low‐frequency Raman spectroscopy method to characterize the twist angle of few‐layer stacked MoS2samples. A feedforward neural network (FNN) is utilized to analyze the low‐frequency breathing mode as a function of the twist angle. Moreover, using finite difference method (FDM) and density functional theory (DFT) calculations, we show that the low‐frequency Raman spectra of MoS2are mainly influenced by the effect of the nearest and second nearest layers. A new improved linear chain model (TA‐LCM) with taking the twist angle into the consideration is developed to understand the interlayer breathing modes of stacked few‐layer MoS2. This approach can be extended to other 2D materials systems and provides an intelligent way to investigate naturally stacked and twisted interlayer interactions.
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- Award ID(s):
- 1945364
- PAR ID:
- 10441883
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Journal of Raman Spectroscopy
- Volume:
- 54
- Issue:
- 9
- ISSN:
- 0377-0486
- Format(s):
- Medium: X Size: p. 1021-1029
- Size(s):
- p. 1021-1029
- Sponsoring Org:
- National Science Foundation
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