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Title: Tunable electronic structure in gallium chalcogenide van der Waals compounds

Abstract

Transition-metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe by using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by in situ potassium deposition as well as by forming GaSxSe1-x alloy compounds. We find that potassium-dosed samples exhibit a substantial change of the dispersion around the valence-band maximum (VBM). The observed band dispersion resembles that of a single tetralayer and is consistent with a transition from the direct-gap character of the bulk to the indirect-gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to AA' stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies, which correlates with a blueshift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [4];  [3];  [3];  [3];  [5];  [3];  [6]
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  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Aarhus Univ., Aarhus (Denmark). Interdisciplinary Nanoscience Center (iNANO)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Arizona State Univ., Tempe, AZ (United States)
  5. Univ. of California, Berkeley, CA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); German Academic Exchange Service (DAAD)
OSTI Identifier:
1574341
Grant/Contract Number:  
AC02-05CH11231; DMR-1807233; 15375
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B
Additional Journal Information:
Journal Volume: 100; Journal Issue: 16; 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

Citation Formats

Shevitski, Brian, Ulstrup, Søren, Koch, Roland J., Cai, Hui, Tongay, Sefaattin, Moreschini, Luca, Jozwiak, Chris, Bostwick, Aaron, Zettl, Alex, Rotenberg, Eli, and Aloni, Shaul. Tunable electronic structure in gallium chalcogenide van der Waals compounds. United States: N. p., 2019. Web. doi:10.1103/physrevb.100.165112.
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Shevitski, Brian, Ulstrup, Søren, Koch, Roland J., Cai, Hui, Tongay, Sefaattin, Moreschini, Luca, Jozwiak, Chris, Bostwick, Aaron, Zettl, Alex, Rotenberg, Eli, & Aloni, Shaul. Tunable electronic structure in gallium chalcogenide van der Waals compounds. United States. https://doi.org/10.1103/physrevb.100.165112
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Shevitski, Brian, Ulstrup, Søren, Koch, Roland J., Cai, Hui, Tongay, Sefaattin, Moreschini, Luca, Jozwiak, Chris, Bostwick, Aaron, Zettl, Alex, Rotenberg, Eli, and Aloni, Shaul. Wed . "Tunable electronic structure in gallium chalcogenide van der Waals compounds". United States. https://doi.org/10.1103/physrevb.100.165112. https://www.osti.gov/servlets/purl/1574341.
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@article{osti_1574341,
title = {Tunable electronic structure in gallium chalcogenide van der Waals compounds},
author = {Shevitski, Brian and Ulstrup, Søren and Koch, Roland J. and Cai, Hui and Tongay, Sefaattin and Moreschini, Luca and Jozwiak, Chris and Bostwick, Aaron and Zettl, Alex and Rotenberg, Eli and Aloni, Shaul},
abstractNote = {Transition-metal monochalcogenides comprise a class of two-dimensional materials with electronic band gaps that are highly sensitive to material thickness and chemical composition. Here, we explore the tunability of the electronic excitation spectrum in GaSe by using angle-resolved photoemission spectroscopy. The electronic structure of the material is modified by in situ potassium deposition as well as by forming GaSxSe1-x alloy compounds. We find that potassium-dosed samples exhibit a substantial change of the dispersion around the valence-band maximum (VBM). The observed band dispersion resembles that of a single tetralayer and is consistent with a transition from the direct-gap character of the bulk to the indirect-gap character expected for monolayer GaSe. Upon alloying with sulfur, we observe a phase transition from AB to AA' stacking. Alloying also results in a rigid energy shift of the VBM towards higher binding energies, which correlates with a blueshift in the luminescence. The increase of the band gap upon sulfur alloying does not appear to change the dispersion or character of the VBM appreciably, implying that it is possible to engineer the gap of these materials while maintaining their salient electronic properties.},
doi = {10.1103/physrevb.100.165112},
journal = {Physical Review. B},
number = 16,
volume = 100,
place = {United States},
year = {Wed Oct 09 00:00:00 EDT 2019},
month = {Wed Oct 09 00:00:00 EDT 2019}
}
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Journal Article:
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https://doi.org/10.1103/physrevb.100.165112
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Figures / Tables:

FIG. 1 FIG. 1: Real space structure and HRSTEM images of the two most common GaSxSe1−x polytypes. Panels (a) and (b) show the crystal structure of the ε phase in the planes defined by the axes in the labels. The corresponding HRSTEM image in (c) shows a trigonal lattice, resulting from themore » projection of Bernal (AB) stacked honeycomb layers. The intensity cut in (d) was obtained from the red rectangle in (c) and shows bright atomic columns with approximately twice the intensity of dim atomic columns. Analogous images in (e)-(f) show the geometry of the β phase. The HRSTEM image in (g) shows a honeycomb mesh, with no intensity in the interstitial columns between hexagonal cells.« less
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    Visualizing Orbital Content of Electronic Bands in Anisotropic 2D Semiconducting ReSe$_{2}$
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