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Title: Anomalous interlayer vibrations in strongly coupled layered PdSe 2

Abstract

In this work, we show unusual effects of strong interlayer coupling on low-frequency (LF) Raman scattering in exfoliated PdSe 2 crystals with different number of layers. Unlike many other layered materials, it is found that the measured frequencies of the breathing modes cannot be simply described by a conventional linear chain model (LCM) that treats each layer as a single rigid object. By using first-principles calculations, we show that strong deviations from layer rigidity can occur for the LF breathing vibrations of PdSe 2, which accounts for the observed disagreement with the conventional LCM. The layer non-rigidity and strong interlayer coupling could also explain the unusual strong intensities of the LF breathing modes that are comparable with those of the high-frequency Raman modes. These strong intensities allowed us to use a set of the measured LF Raman lines as unique fingerprints for a precise assignment of the layer numbers. The assignment of the layer numbers was further confirmed using second harmonic generation that appeared only in the noncentrosymmetric even-layer PdSe 2 crystals. In conclusion, this work thus demonstrates a simple and fast approach for the determination of the number of layers in 2D materials with strong interlayer coupling and non-rigidmore » interlayer vibrations.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [3]; ORCiD logo [1];  [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1437902
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
2D Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 3; Journal ID: ISSN 2053-1583
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 2D materials; PdSe2; low-frequency Raman; strong interlayer coupling; linear chain model; layer partial-rigidity

Citation Formats

Puretzky, Alexander A., Oyedele, Akinola D., Xiao, Kai, Haglund, Amanda V., Sumpter, Bobby G., Mandrus, David, Geohegan, David B., and Liang, Liangbo. Anomalous interlayer vibrations in strongly coupled layered PdSe2. United States: N. p., 2018. Web. doi:10.1088/2053-1583/aabe4d.
Puretzky, Alexander A., Oyedele, Akinola D., Xiao, Kai, Haglund, Amanda V., Sumpter, Bobby G., Mandrus, David, Geohegan, David B., & Liang, Liangbo. Anomalous interlayer vibrations in strongly coupled layered PdSe2. United States. doi:10.1088/2053-1583/aabe4d.
Puretzky, Alexander A., Oyedele, Akinola D., Xiao, Kai, Haglund, Amanda V., Sumpter, Bobby G., Mandrus, David, Geohegan, David B., and Liang, Liangbo. Fri . "Anomalous interlayer vibrations in strongly coupled layered PdSe2". United States. doi:10.1088/2053-1583/aabe4d. https://www.osti.gov/servlets/purl/1437902.
@article{osti_1437902,
title = {Anomalous interlayer vibrations in strongly coupled layered PdSe2},
author = {Puretzky, Alexander A. and Oyedele, Akinola D. and Xiao, Kai and Haglund, Amanda V. and Sumpter, Bobby G. and Mandrus, David and Geohegan, David B. and Liang, Liangbo},
abstractNote = {In this work, we show unusual effects of strong interlayer coupling on low-frequency (LF) Raman scattering in exfoliated PdSe2 crystals with different number of layers. Unlike many other layered materials, it is found that the measured frequencies of the breathing modes cannot be simply described by a conventional linear chain model (LCM) that treats each layer as a single rigid object. By using first-principles calculations, we show that strong deviations from layer rigidity can occur for the LF breathing vibrations of PdSe2, which accounts for the observed disagreement with the conventional LCM. The layer non-rigidity and strong interlayer coupling could also explain the unusual strong intensities of the LF breathing modes that are comparable with those of the high-frequency Raman modes. These strong intensities allowed us to use a set of the measured LF Raman lines as unique fingerprints for a precise assignment of the layer numbers. The assignment of the layer numbers was further confirmed using second harmonic generation that appeared only in the noncentrosymmetric even-layer PdSe2 crystals. In conclusion, this work thus demonstrates a simple and fast approach for the determination of the number of layers in 2D materials with strong interlayer coupling and non-rigid interlayer vibrations.},
doi = {10.1088/2053-1583/aabe4d},
journal = {2D Materials},
number = 3,
volume = 5,
place = {United States},
year = {2018},
month = {5}
}

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    Works referencing / citing this record:

    Ferroelastic lattice rotation and band-gap engineering in quasi 2D layered-structure PdSe 2 under uniaxial stress
    journal, January 2019


    Ferroelastic lattice rotation and band-gap engineering in quasi 2D layered-structure PdSe 2 under uniaxial stress
    journal, January 2019