Atypical Exciton-Phonon Interactions in WS2 and WSe2 Monolayers Revealed by Resonance Raman Spectroscopy

E. Del Corro, A. Botello-Méndez, Y. Gillet, Ana Laura Elias Arriaga, H. Terrones, S. Feng, C. Fantini, Daniel Rhodes, N. Pradhan, L. Balicas, X. Gonze, J. C. Charlier, Mauricio Terrones Maldonado, M. A. Pimenta

Research output: Contribution to journalArticle

46 Citations (Scopus)

Abstract

Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS2 and WSe2 using more than 25 laser lines. The Raman excitation profiles of both materials show unexpected differences. All Raman features of WS2 monolayers are enhanced by the first-optical excitations (with an asymmetric response for the spin-orbit related XA and XB excitons), whereas Raman bands of WSe2 are not enhanced at XA/B energies. Such an intriguing phenomenon is addressed by DFT calculations and by solving the Bethe-Salpeter equation. These two materials are very similar. They prefer the same crystal arrangement, and their electronic structure is akin, with comparable spin-orbit coupling. However, we reveal that WS2 and WSe2 exhibit quite different exciton-phonon interactions. In this sense, we demonstrate that the interaction between XC and XA excitons with phonons explains the different Raman responses of WS2 and WSe2, and the absence of Raman enhancement for the WSe2 modes at XA/B energies. These results reveal unusual exciton-phonon interactions and open new avenues for understanding the two-dimensional materials physics, where weak interactions play a key role coupling different degrees of freedom (spin, optic, and electronic).

Original languageEnglish (US)
Pages (from-to)2363-2368
Number of pages6
JournalNano letters
Volume16
Issue number4
DOIs
StatePublished - Apr 13 2016

Fingerprint

Excitons
Raman spectroscopy
Monolayers
excitons
interactions
Orbits
orbits
Bethe-Salpeter equation
Photoexcitation
Phonons
Discrete Fourier transforms
excitation
Electronic structure
LDS 751
Optics
phonons
Physics
degrees of freedom
optics
electronic structure

All Science Journal Classification (ASJC) codes

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

Cite this

Del Corro, E. ; Botello-Méndez, A. ; Gillet, Y. ; Elias Arriaga, Ana Laura ; Terrones, H. ; Feng, S. ; Fantini, C. ; Rhodes, Daniel ; Pradhan, N. ; Balicas, L. ; Gonze, X. ; Charlier, J. C. ; Terrones Maldonado, Mauricio ; Pimenta, M. A. / Atypical Exciton-Phonon Interactions in WS2 and WSe2 Monolayers Revealed by Resonance Raman Spectroscopy. In: Nano letters. 2016 ; Vol. 16, No. 4. pp. 2363-2368.
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abstract = "Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS2 and WSe2 using more than 25 laser lines. The Raman excitation profiles of both materials show unexpected differences. All Raman features of WS2 monolayers are enhanced by the first-optical excitations (with an asymmetric response for the spin-orbit related XA and XB excitons), whereas Raman bands of WSe2 are not enhanced at XA/B energies. Such an intriguing phenomenon is addressed by DFT calculations and by solving the Bethe-Salpeter equation. These two materials are very similar. They prefer the same crystal arrangement, and their electronic structure is akin, with comparable spin-orbit coupling. However, we reveal that WS2 and WSe2 exhibit quite different exciton-phonon interactions. In this sense, we demonstrate that the interaction between XC and XA excitons with phonons explains the different Raman responses of WS2 and WSe2, and the absence of Raman enhancement for the WSe2 modes at XA/B energies. These results reveal unusual exciton-phonon interactions and open new avenues for understanding the two-dimensional materials physics, where weak interactions play a key role coupling different degrees of freedom (spin, optic, and electronic).",
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Del Corro, E, Botello-Méndez, A, Gillet, Y, Elias Arriaga, AL, Terrones, H, Feng, S, Fantini, C, Rhodes, D, Pradhan, N, Balicas, L, Gonze, X, Charlier, JC, Terrones Maldonado, M & Pimenta, MA 2016, 'Atypical Exciton-Phonon Interactions in WS2 and WSe2 Monolayers Revealed by Resonance Raman Spectroscopy', Nano letters, vol. 16, no. 4, pp. 2363-2368. https://doi.org/10.1021/acs.nanolett.5b05096

Atypical Exciton-Phonon Interactions in WS2 and WSe2 Monolayers Revealed by Resonance Raman Spectroscopy. / Del Corro, E.; Botello-Méndez, A.; Gillet, Y.; Elias Arriaga, Ana Laura; Terrones, H.; Feng, S.; Fantini, C.; Rhodes, Daniel; Pradhan, N.; Balicas, L.; Gonze, X.; Charlier, J. C.; Terrones Maldonado, Mauricio; Pimenta, M. A.

In: Nano letters, Vol. 16, No. 4, 13.04.2016, p. 2363-2368.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Atypical Exciton-Phonon Interactions in WS2 and WSe2 Monolayers Revealed by Resonance Raman Spectroscopy

AU - Del Corro, E.

AU - Botello-Méndez, A.

AU - Gillet, Y.

AU - Elias Arriaga, Ana Laura

AU - Terrones, H.

AU - Feng, S.

AU - Fantini, C.

AU - Rhodes, Daniel

AU - Pradhan, N.

AU - Balicas, L.

AU - Gonze, X.

AU - Charlier, J. C.

AU - Terrones Maldonado, Mauricio

AU - Pimenta, M. A.

PY - 2016/4/13

Y1 - 2016/4/13

N2 - Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS2 and WSe2 using more than 25 laser lines. The Raman excitation profiles of both materials show unexpected differences. All Raman features of WS2 monolayers are enhanced by the first-optical excitations (with an asymmetric response for the spin-orbit related XA and XB excitons), whereas Raman bands of WSe2 are not enhanced at XA/B energies. Such an intriguing phenomenon is addressed by DFT calculations and by solving the Bethe-Salpeter equation. These two materials are very similar. They prefer the same crystal arrangement, and their electronic structure is akin, with comparable spin-orbit coupling. However, we reveal that WS2 and WSe2 exhibit quite different exciton-phonon interactions. In this sense, we demonstrate that the interaction between XC and XA excitons with phonons explains the different Raman responses of WS2 and WSe2, and the absence of Raman enhancement for the WSe2 modes at XA/B energies. These results reveal unusual exciton-phonon interactions and open new avenues for understanding the two-dimensional materials physics, where weak interactions play a key role coupling different degrees of freedom (spin, optic, and electronic).

AB - Resonant Raman spectroscopy is a powerful tool for providing information about excitons and exciton-phonon coupling in two-dimensional materials. We present here resonant Raman experiments of single-layered WS2 and WSe2 using more than 25 laser lines. The Raman excitation profiles of both materials show unexpected differences. All Raman features of WS2 monolayers are enhanced by the first-optical excitations (with an asymmetric response for the spin-orbit related XA and XB excitons), whereas Raman bands of WSe2 are not enhanced at XA/B energies. Such an intriguing phenomenon is addressed by DFT calculations and by solving the Bethe-Salpeter equation. These two materials are very similar. They prefer the same crystal arrangement, and their electronic structure is akin, with comparable spin-orbit coupling. However, we reveal that WS2 and WSe2 exhibit quite different exciton-phonon interactions. In this sense, we demonstrate that the interaction between XC and XA excitons with phonons explains the different Raman responses of WS2 and WSe2, and the absence of Raman enhancement for the WSe2 modes at XA/B energies. These results reveal unusual exciton-phonon interactions and open new avenues for understanding the two-dimensional materials physics, where weak interactions play a key role coupling different degrees of freedom (spin, optic, and electronic).

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JF - Nano Letters

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