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Title: Gold Dispersion and Activation on the Basal Plane of Single-Layer MoS2

Abstract

Gold islands are typically associated with high binding affinity to adsorbates and catalytic activity. In this paper, we present the growth of dispersed nanoscale gold islands on single layer MoS2, prepared on an inert SiO2/Si support by chemical vapor deposition. This study offers a combination of growth process development, optical characterization, photoelectron spectroscopy at submicron spatial resolution, and advanced density functional theory modeling for detailed insight into the electronic interaction between gold and single-layer MoS2. In particular, we find the gold density of states in Au/MoS2/SiO2/Si to be far less well-defined than Au islands on other 2-dimensional materials such as graphene, for which we also provide data. We attribute this effect to the presence of heterogeneous Au adatom/MoS2-support interactions within the nanometer-scale gold cluster. Theory predicts that CO will exhibit adsorption energies in excess of 1 eV at the Au cluster edges, where the local density of states is dominated by Au 5dz2 symmetry.

Authors:
 [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [2];  [1];  [4];  [4];  [5];  [6];  [1];  [1];  [1];  [1];  [1];  [4];  [2]; ORCiD logo [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of California, Riverside, CA (United States). Dept. of Chemistry, and Materials Science & Engineering Program
  2. Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
  3. Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy
  4. Elettra-Sincrotrone Trieste (Italy)
  5. Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
  6. King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE
OSTI Identifier:
1483381
Grant/Contract Number:  
FG02-07ER15842
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 1; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Merida, Cindy S., Le, Duy, Echeverria, Elena M., Nguyen, Ariana E., Rawal, Takat B., Naghibi Alvillar, Sahar, Kandyba, Viktor, Al-Mahboob, Abdullah, Losovyj, Yaroslav, Katsiev, Khabiboulakh, Valentin, Michael D., Huang, Chun-Yu, Gomez, Michael J., Lu, I-Hsi, Guan, Alison, Barinov, Alexei, Rahman, Talat S., Dowben, Peter A., and Bartels, Ludwig. Gold Dispersion and Activation on the Basal Plane of Single-Layer MoS2. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b07632.
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Merida, Cindy S., Le, Duy, Echeverria, Elena M., Nguyen, Ariana E., Rawal, Takat B., Naghibi Alvillar, Sahar, Kandyba, Viktor, Al-Mahboob, Abdullah, Losovyj, Yaroslav, Katsiev, Khabiboulakh, Valentin, Michael D., Huang, Chun-Yu, Gomez, Michael J., Lu, I-Hsi, Guan, Alison, Barinov, Alexei, Rahman, Talat S., Dowben, Peter A., & Bartels, Ludwig. Gold Dispersion and Activation on the Basal Plane of Single-Layer MoS2. United States. https://doi.org/10.1021/acs.jpcc.7b07632
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Merida, Cindy S., Le, Duy, Echeverria, Elena M., Nguyen, Ariana E., Rawal, Takat B., Naghibi Alvillar, Sahar, Kandyba, Viktor, Al-Mahboob, Abdullah, Losovyj, Yaroslav, Katsiev, Khabiboulakh, Valentin, Michael D., Huang, Chun-Yu, Gomez, Michael J., Lu, I-Hsi, Guan, Alison, Barinov, Alexei, Rahman, Talat S., Dowben, Peter A., and Bartels, Ludwig. Sat . "Gold Dispersion and Activation on the Basal Plane of Single-Layer MoS2". United States. https://doi.org/10.1021/acs.jpcc.7b07632. https://www.osti.gov/servlets/purl/1483381.
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@article{osti_1483381,
title = {Gold Dispersion and Activation on the Basal Plane of Single-Layer MoS2},
author = {Merida, Cindy S. and Le, Duy and Echeverria, Elena M. and Nguyen, Ariana E. and Rawal, Takat B. and Naghibi Alvillar, Sahar and Kandyba, Viktor and Al-Mahboob, Abdullah and Losovyj, Yaroslav and Katsiev, Khabiboulakh and Valentin, Michael D. and Huang, Chun-Yu and Gomez, Michael J. and Lu, I-Hsi and Guan, Alison and Barinov, Alexei and Rahman, Talat S. and Dowben, Peter A. and Bartels, Ludwig},
abstractNote = {Gold islands are typically associated with high binding affinity to adsorbates and catalytic activity. In this paper, we present the growth of dispersed nanoscale gold islands on single layer MoS2, prepared on an inert SiO2/Si support by chemical vapor deposition. This study offers a combination of growth process development, optical characterization, photoelectron spectroscopy at submicron spatial resolution, and advanced density functional theory modeling for detailed insight into the electronic interaction between gold and single-layer MoS2. In particular, we find the gold density of states in Au/MoS2/SiO2/Si to be far less well-defined than Au islands on other 2-dimensional materials such as graphene, for which we also provide data. We attribute this effect to the presence of heterogeneous Au adatom/MoS2-support interactions within the nanometer-scale gold cluster. Theory predicts that CO will exhibit adsorption energies in excess of 1 eV at the Au cluster edges, where the local density of states is dominated by Au 5dz2 symmetry.},
doi = {10.1021/acs.jpcc.7b07632},
journal = {Journal of Physical Chemistry. C},
number = 1,
volume = 122,
place = {United States},
year = {Sat Dec 09 00:00:00 EST 2017},
month = {Sat Dec 09 00:00:00 EST 2017}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpcc.7b07632
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Citation Metrics:
Cited by: 14 works
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Figures / Tables:

Figure 1 Figure 1: a) Schematic representation of the experiment and results: as the Au coverage on single-layer MoS2 islands increases from isolated atoms to single- an bi-layer islands, strong Au-MoS2 interaction at isolated atoms, island edges and the bottom layer modify the Au 5d density of states. The layer thickness/island densitymore » is for illustrative purpose and does not reflect the experimental values quantiatively; b) Photoluminescence (PL) spectroscopy shows bright signal at the optical bandgap of MoS2 prior to gold deposition and complete quenching following deposition of 4Å of gold; c) Raman spectroscopy reveals surface enhanced MoS2 E2g and A1g signal once the gold is deposited (at unchanged position) as well as attenuation of the Si substrate peak; d) map of the lateral variation of the photoelectron yield reveals the size and location of the single-layer single-crystalline MoS2 islands used in this study.« less
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