Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials
Abstract
Ever since the isolation of single-layer graphene in 2004, two-dimensional layered structures have been among the most extensively studied classes of materials. To date, the pool of two-dimensional materials (2DMs) continues to grow at an accelerated pace and already covers an extensive range of fascinating and technologically relevant properties. An array of experimental techniques have been developed and used to fully characterize and understand these properties. In particular, Raman spectroscopy has proven to be a key experimental technique, thanks to its capability to identify minute structural and electronic effects in nondestructive measurements. While high-frequency (HF) intralayer Raman modes have been extensively employed for 2DMs, recent experimental and theoretical progress has demonstrated that low-frequency (LF) interlayer Raman modes are more effective at determining layer numbers and stacking configurations, and provide a unique opportunity to study interlayer coupling. These advantages are due to 2DMs’ unique interlayer vibration patterns where each layer behaves as an almost rigidly moving object with restoring forces corresponding to weak interlayer interactions. Compared to HF Raman modes, the relatively small attention originally devoted to LF Raman modes is largely due to their weaker signal and their proximity to the strong Rayleigh line background, which previously made their detectionmore »
- Authors:
-
[1];
[2];
[1];
[2];
[3]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
- Rensselaer Polytechnic Inst., Troy, NY (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1410198
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 12; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; interlayer bond polarizability model; interlayer coupling; interlayer vibrations; linear chain model; low-frequency phonons; Raman scattering; stacking fingerprints; thickness fingerprints; two-dimensional materials
Citation Formats
Liang, Liangbo, Zhang, Jun, Sumpter, Bobby G., Tan, Qing -Hai, Tan, Ping -Heng, and Meunier, Vincent. Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials. United States: N. p., 2017.
Web. doi:10.1021/acsnano.7b06551.
Liang, Liangbo, Zhang, Jun, Sumpter, Bobby G., Tan, Qing -Hai, Tan, Ping -Heng, & Meunier, Vincent. Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials. United States. https://doi.org/10.1021/acsnano.7b06551
Liang, Liangbo, Zhang, Jun, Sumpter, Bobby G., Tan, Qing -Hai, Tan, Ping -Heng, and Meunier, Vincent. Fri .
"Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials". United States. https://doi.org/10.1021/acsnano.7b06551. https://www.osti.gov/servlets/purl/1410198.
@article{osti_1410198,
title = {Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials},
author = {Liang, Liangbo and Zhang, Jun and Sumpter, Bobby G. and Tan, Qing -Hai and Tan, Ping -Heng and Meunier, Vincent},
abstractNote = {Ever since the isolation of single-layer graphene in 2004, two-dimensional layered structures have been among the most extensively studied classes of materials. To date, the pool of two-dimensional materials (2DMs) continues to grow at an accelerated pace and already covers an extensive range of fascinating and technologically relevant properties. An array of experimental techniques have been developed and used to fully characterize and understand these properties. In particular, Raman spectroscopy has proven to be a key experimental technique, thanks to its capability to identify minute structural and electronic effects in nondestructive measurements. While high-frequency (HF) intralayer Raman modes have been extensively employed for 2DMs, recent experimental and theoretical progress has demonstrated that low-frequency (LF) interlayer Raman modes are more effective at determining layer numbers and stacking configurations, and provide a unique opportunity to study interlayer coupling. These advantages are due to 2DMs’ unique interlayer vibration patterns where each layer behaves as an almost rigidly moving object with restoring forces corresponding to weak interlayer interactions. Compared to HF Raman modes, the relatively small attention originally devoted to LF Raman modes is largely due to their weaker signal and their proximity to the strong Rayleigh line background, which previously made their detection challenging. Recent progress in Raman spectroscopy with technical and hardware upgrades now makes it possible to probe LF modes with a standard single-stage Raman system and has proven crucial to characterize and understand properties of 2DMs. Here, we present a comprehensive and forward-looking review on the current status of exploiting LF Raman modes of 2DMs from both experimental and theoretical perspectives, revealing the fundamental physics and technological significance of LF Raman modes in advancing the field of 2DMs. We review a broad array of materials, with varying thickness and stacking configurations, discuss the effect of in-plane anisotropy, and present a generalized linear chain model and interlayer bond polarizability model to rationalize the experimental findings. We also discuss the instrumental improvements of Raman spectroscopy to enhance and separate LF Raman signals from the Rayleigh line. Lastly, we highlight the opportunities and challenges ahead in this fast-developing field.},
doi = {10.1021/acsnano.7b06551},
journal = {ACS Nano},
number = 12,
volume = 11,
place = {United States},
year = {Fri Nov 03 00:00:00 EDT 2017},
month = {Fri Nov 03 00:00:00 EDT 2017}
}
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