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Title: Revealing excitonic processes and chemical bonding in Mo S 2 by x-ray spectroscopy

Abstract

Electron core-hole processes at absorption edges sport several signatures, primarily in the form of bound states and/or excitonic enhancement. Here, through analysis of the resonant-Raman Auger effect for the two-dimensional transition-metal dichalcogenide MoS 2, we demonstrate that these effects have significant manifestations at the S K edge. We characterize two asymmetric excitonically enhanced edges: one at the fundamental band edge and one several electron volts above it following a second band gap that lies entirely within the unoccupied states, with the latter revealing an anomalous postcollision interaction effect. In conclusion, our interpretation is supported by comparison of both the photoemission valence-band spectrum and the S K-edge x-ray-absorption spectrum with electronic structure calculations and an ab initio solution of the Bethe-Salpeter equation that accurately accounts for the electron-core-hole interaction.

Authors:
 [1];  [1];  [2];  [3];  [1];  [4];  [5]
  1. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Materials Measurement Science Division, Material Measurement Laboratory
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Materials Characterization Department
  4. Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin (France)
  5. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Sensor Science Division, Physical Measurement Laboratory
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1481401
Report Number(s):
BNL-209423-2018-JAAM
Journal ID: ISSN 2469-9950; PRBMDO
Grant/Contract Number:  
SC0012704; AC02-98CH10886
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 98; Journal Issue: 11; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 47 OTHER INSTRUMENTATION

Citation Formats

Woicik, J. C., Weiland, C., Rumaiz, A. K., Brumbach, M., Quackenbush, N. F., Ablett, J. M., and Shirley, E. L. Revealing excitonic processes and chemical bonding in MoS2 by x-ray spectroscopy. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.98.115149.
Woicik, J. C., Weiland, C., Rumaiz, A. K., Brumbach, M., Quackenbush, N. F., Ablett, J. M., & Shirley, E. L. Revealing excitonic processes and chemical bonding in MoS2 by x-ray spectroscopy. United States. doi:10.1103/PhysRevB.98.115149.
Woicik, J. C., Weiland, C., Rumaiz, A. K., Brumbach, M., Quackenbush, N. F., Ablett, J. M., and Shirley, E. L. Tue . "Revealing excitonic processes and chemical bonding in MoS2 by x-ray spectroscopy". United States. doi:10.1103/PhysRevB.98.115149. https://www.osti.gov/servlets/purl/1481401.
@article{osti_1481401,
title = {Revealing excitonic processes and chemical bonding in MoS2 by x-ray spectroscopy},
author = {Woicik, J. C. and Weiland, C. and Rumaiz, A. K. and Brumbach, M. and Quackenbush, N. F. and Ablett, J. M. and Shirley, E. L.},
abstractNote = {Electron core-hole processes at absorption edges sport several signatures, primarily in the form of bound states and/or excitonic enhancement. Here, through analysis of the resonant-Raman Auger effect for the two-dimensional transition-metal dichalcogenide MoS2, we demonstrate that these effects have significant manifestations at the S K edge. We characterize two asymmetric excitonically enhanced edges: one at the fundamental band edge and one several electron volts above it following a second band gap that lies entirely within the unoccupied states, with the latter revealing an anomalous postcollision interaction effect. In conclusion, our interpretation is supported by comparison of both the photoemission valence-band spectrum and the S K-edge x-ray-absorption spectrum with electronic structure calculations and an ab initio solution of the Bethe-Salpeter equation that accurately accounts for the electron-core-hole interaction.},
doi = {10.1103/PhysRevB.98.115149},
journal = {Physical Review B},
issn = {2469-9950},
number = 11,
volume = 98,
place = {United States},
year = {2018},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: a) S $K$ x-ray absorption near-edge spectra for MoS2. Theory (top). Experiment (bottom). b) Theoretical S $K$ x-ray absorption near-edge spectra for MoS2 calculated with (top) and without (bottom) the electron-core-hole interaction. The orientation of the polarization vector $ε$ of the synchrotron radiation relative to the MoS2 $c$more » direction is indicated.« less

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