Raman detection of hidden phonons assisted by atomic point defects in a two-dimensional semimetal

Hui Yuan, Xieyu Zhou, Yan Cao, Qi Bian, Zongyuan Zhang, Haigen Sun, Shaojian Li, Zhibin Shao, Jin Hu, Yanglin Zhu, Zhiqiang Mao, Wei Ji, Minghu Pan

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Defects usually have an important role in tailoring various properties of two-dimensional (2D) materials. However, optical detection of defects, especially single-atom point defects, is very challenging in 2D layers. Here, we report our systematic studies on the Raman-activated defect vibrational modes in 2D semimetallic material by combining Raman spectroscopy, density functional theory (DFT) calculation and scanning tunneling microscopy (STM). We observed three common Raman-active vibrational modes located at 95 (A1g2), 228 (A1g1), and 304 cm−1 (B1g1) in ZrSiTe few-layers, consistent with our theoretical calculations. Moreover, a pronounced mode sitting at 131.7 cm−1 was found in the ZrSiTe monolayer. This mode fades out quickly in the bilayer (2L) and eventually disappears in 4L. The high-resolution STM images and DFT calculations suggest this mode to be an intralayer shear mode at the Brillouin zone boundary which is activated by atomic point defects, and STM-based inelastic tunneling spectrum further confirms the existence of such a defect mode. The appearance of such ‘forbidden’ modes in Raman spectra may pave an avenue for the optical characterization of single-atom point defects in metallic 2D layers.

Original languageEnglish (US)
Article number12
Journalnpj 2D Materials and Applications
Volume3
Issue number1
DOIs
StatePublished - Dec 1 2019

Fingerprint

Metalloids
metalloids
Point defects
Phonons
point defects
phonons
Scanning tunneling microscopy
Defects
Density functional theory
scanning tunneling microscopy
defects
Atoms
vibration mode
density functional theory
Raman spectroscopy
Raman scattering
Monolayers
Brillouin zones
atoms
Raman spectra

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Mechanical Engineering
  • Mechanics of Materials
  • Condensed Matter Physics
  • Chemistry(all)

Cite this

Yuan, Hui ; Zhou, Xieyu ; Cao, Yan ; Bian, Qi ; Zhang, Zongyuan ; Sun, Haigen ; Li, Shaojian ; Shao, Zhibin ; Hu, Jin ; Zhu, Yanglin ; Mao, Zhiqiang ; Ji, Wei ; Pan, Minghu. / Raman detection of hidden phonons assisted by atomic point defects in a two-dimensional semimetal. In: npj 2D Materials and Applications. 2019 ; Vol. 3, No. 1.
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abstract = "Defects usually have an important role in tailoring various properties of two-dimensional (2D) materials. However, optical detection of defects, especially single-atom point defects, is very challenging in 2D layers. Here, we report our systematic studies on the Raman-activated defect vibrational modes in 2D semimetallic material by combining Raman spectroscopy, density functional theory (DFT) calculation and scanning tunneling microscopy (STM). We observed three common Raman-active vibrational modes located at 95 (A1g2), 228 (A1g1), and 304 cm−1 (B1g1) in ZrSiTe few-layers, consistent with our theoretical calculations. Moreover, a pronounced mode sitting at 131.7 cm−1 was found in the ZrSiTe monolayer. This mode fades out quickly in the bilayer (2L) and eventually disappears in 4L. The high-resolution STM images and DFT calculations suggest this mode to be an intralayer shear mode at the Brillouin zone boundary which is activated by atomic point defects, and STM-based inelastic tunneling spectrum further confirms the existence of such a defect mode. The appearance of such ‘forbidden’ modes in Raman spectra may pave an avenue for the optical characterization of single-atom point defects in metallic 2D layers.",
author = "Hui Yuan and Xieyu Zhou and Yan Cao and Qi Bian and Zongyuan Zhang and Haigen Sun and Shaojian Li and Zhibin Shao and Jin Hu and Yanglin Zhu and Zhiqiang Mao and Wei Ji and Minghu Pan",
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Yuan, H, Zhou, X, Cao, Y, Bian, Q, Zhang, Z, Sun, H, Li, S, Shao, Z, Hu, J, Zhu, Y, Mao, Z, Ji, W & Pan, M 2019, 'Raman detection of hidden phonons assisted by atomic point defects in a two-dimensional semimetal', npj 2D Materials and Applications, vol. 3, no. 1, 12. https://doi.org/10.1038/s41699-019-0093-7

Raman detection of hidden phonons assisted by atomic point defects in a two-dimensional semimetal. / Yuan, Hui; Zhou, Xieyu; Cao, Yan; Bian, Qi; Zhang, Zongyuan; Sun, Haigen; Li, Shaojian; Shao, Zhibin; Hu, Jin; Zhu, Yanglin; Mao, Zhiqiang; Ji, Wei; Pan, Minghu.

In: npj 2D Materials and Applications, Vol. 3, No. 1, 12, 01.12.2019.

Research output: Contribution to journalArticle

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AU - Yuan, Hui

AU - Zhou, Xieyu

AU - Cao, Yan

AU - Bian, Qi

AU - Zhang, Zongyuan

AU - Sun, Haigen

AU - Li, Shaojian

AU - Shao, Zhibin

AU - Hu, Jin

AU - Zhu, Yanglin

AU - Mao, Zhiqiang

AU - Ji, Wei

AU - Pan, Minghu

PY - 2019/12/1

Y1 - 2019/12/1

N2 - Defects usually have an important role in tailoring various properties of two-dimensional (2D) materials. However, optical detection of defects, especially single-atom point defects, is very challenging in 2D layers. Here, we report our systematic studies on the Raman-activated defect vibrational modes in 2D semimetallic material by combining Raman spectroscopy, density functional theory (DFT) calculation and scanning tunneling microscopy (STM). We observed three common Raman-active vibrational modes located at 95 (A1g2), 228 (A1g1), and 304 cm−1 (B1g1) in ZrSiTe few-layers, consistent with our theoretical calculations. Moreover, a pronounced mode sitting at 131.7 cm−1 was found in the ZrSiTe monolayer. This mode fades out quickly in the bilayer (2L) and eventually disappears in 4L. The high-resolution STM images and DFT calculations suggest this mode to be an intralayer shear mode at the Brillouin zone boundary which is activated by atomic point defects, and STM-based inelastic tunneling spectrum further confirms the existence of such a defect mode. The appearance of such ‘forbidden’ modes in Raman spectra may pave an avenue for the optical characterization of single-atom point defects in metallic 2D layers.

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