Document Type

Article

Publication Date

11-10-2022

Department

Department of Physics

Abstract

Significant efforts developing MoS2-PbS-based heterostructure devices with several different architectures show promise for photosensor, solar cell, and chemical sensor applications. Merelaniite (Mo4Pb4VSbS15) is a newly discovered natural van der Waals heterostructure of the cylindrite type, composed predominantly of heavily modulated pseudotetragonal PbS layers and pseudohexagonal MoS2 layers with large misfit-induced anisotropy. For an incommensurate modulated structure, the refined structural model from single-crystal x-ray diffraction analysis is in reasonable agreement with the results obtained by high-resolution scanning transmission electron microscopy, especially in light of the fact that that the two isolated single-crystal domains used for the x-ray and electron diffraction experiments were extracted from two different whiskers and subjected to different sample preparation methods. The effects of the misfit-induced structural anisotropy are studied using angle-resolved polarized Raman spectroscopy. The intensities of 12 Raman modes are studied as a function of incident polarization angle relative to merelaniite's whisker axis, and show maximal intensity with the polarization direction perpendicular to the whisker axis. Polarization-dependent anisotropic third-harmonic generation from ultrathin mechanically exfoliated flakes reveals the anisotropy of the third-order nonlinear susceptibility tensor. Merelaniite demonstrates an expanded structure-chemistry space for engineering stable layered materials for potential device applications.

Publisher's Statement

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Publisher’s version of record: https://doi.org/10.1103/PhysRevMaterials.6.115202

Publication Title

Physical Review Materials

Version

Publisher's PDF

Included in

Physics Commons

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