Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations
Abstract
In this study, stacked monolayers of two-dimensional (2D) materials present a new class of hybrid materials with tunable optoelectronic properties determined by their stacking orientation, order, and atomic registry. Atomic-resolution Z-contrast scanning transmission electron microscopy (AR-Z-STEM) and electron energy loss spectroscopy (EELS) can be used to determine the exact atomic registration between different layers, in few-layer 2D stacks, however fast optical characterization techniques are essential for rapid development of the field. Here, using two- and three-layer MoSe2 and WSe2 crystals synthesized by chemical vapor deposition we show that the generally unexplored low frequency (LF) Raman modes (< 50 cm-1) that originate from interlayer vibrations can serve as fingerprints to characterize not only the number of layers, but also their stacking configurations. Ab initio calculations and group theory analysis corroborate the experimental assignments determined by AR-Z-STEM and show that the calculated LF mode fingerprints are related to the 2D crystal symmetries.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Rensselaer Polytechnic Institute, Troy, NY (United States)
- Escuela Politecnica Nacional, Quito (Ecuador)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1193188
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; two-dimensional materials; transition metal dichalcogenides; low-frequency Raman spectroscopy; stacking configurations; first-principles calculations
Citation Formats
Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Wang, Kai, Mahjouri-Samani, Masoud, Basile, Leonardo, Idrobo, Juan Carlos, Sumpter, Bobby G., Meunier, Vincent, and Geohegan, David B. Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations. United States: N. p., 2015.
Web. doi:10.1021/acsnano.5b01884.
Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Wang, Kai, Mahjouri-Samani, Masoud, Basile, Leonardo, Idrobo, Juan Carlos, Sumpter, Bobby G., Meunier, Vincent, & Geohegan, David B. Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations. United States. https://doi.org/10.1021/acsnano.5b01884
Puretzky, Alexander A., Liang, Liangbo, Li, Xufan, Xiao, Kai, Wang, Kai, Mahjouri-Samani, Masoud, Basile, Leonardo, Idrobo, Juan Carlos, Sumpter, Bobby G., Meunier, Vincent, and Geohegan, David B. Tue .
"Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations". United States. https://doi.org/10.1021/acsnano.5b01884. https://www.osti.gov/servlets/purl/1193188.
@article{osti_1193188,
title = {Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations},
author = {Puretzky, Alexander A. and Liang, Liangbo and Li, Xufan and Xiao, Kai and Wang, Kai and Mahjouri-Samani, Masoud and Basile, Leonardo and Idrobo, Juan Carlos and Sumpter, Bobby G. and Meunier, Vincent and Geohegan, David B.},
abstractNote = {In this study, stacked monolayers of two-dimensional (2D) materials present a new class of hybrid materials with tunable optoelectronic properties determined by their stacking orientation, order, and atomic registry. Atomic-resolution Z-contrast scanning transmission electron microscopy (AR-Z-STEM) and electron energy loss spectroscopy (EELS) can be used to determine the exact atomic registration between different layers, in few-layer 2D stacks, however fast optical characterization techniques are essential for rapid development of the field. Here, using two- and three-layer MoSe2 and WSe2 crystals synthesized by chemical vapor deposition we show that the generally unexplored low frequency (LF) Raman modes (< 50 cm-1) that originate from interlayer vibrations can serve as fingerprints to characterize not only the number of layers, but also their stacking configurations. Ab initio calculations and group theory analysis corroborate the experimental assignments determined by AR-Z-STEM and show that the calculated LF mode fingerprints are related to the 2D crystal symmetries.},
doi = {10.1021/acsnano.5b01884},
journal = {ACS Nano},
number = 6,
volume = 9,
place = {United States},
year = {Tue May 12 00:00:00 EDT 2015},
month = {Tue May 12 00:00:00 EDT 2015}
}
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