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Title: Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights

Abstract

Here in this paper, we present an extensive experimental study of the conditions under which Cu forms encapsulated islands under the top surface layers of graphite, as a result of physical vapor deposition of Cu on argon-ion-bombarded graphite. When the substrate is held at 800 K during deposition, conditions are optimal for formation of encapsulated multilayer Cu islands. Deposition temperatures below 600 K favor adsorbed Cu clusters, while deposition temperatures above 800 K favor a different type of feature that is probably a single-layer intercalated Cu island. The multilayer Cu islands are characterized with respect to size and shape, thickness and continuity of the graphitic overlayer, relationship to graphite steps, and stability in air. The experimental techniques are scanning tunneling microscopy and X-ray photoelectron spectroscopy. We also present an extensive study using density functional theory to compare stabilities of a wide variety of configurations of Cu atoms, Cu clusters, and Cu layers on/under the graphite surface. The only configuration that is significantly more stable under the graphite surface than on top of it, is a single Cu atom. This analysis leads us to conclude that formation of encapsulated Cu islands is kinetically driven, rather than thermodynamically driven.

Authors:
 [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [2]; ORCiD logo [4]; ORCiD logo [5]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry
  2. Ames Lab., Ames, IA (United States)
  3. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy, and Dept. of Mathematics
  4. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy
  5. Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry and Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1422772
Report Number(s):
IS-J-9545
Journal ID: ISSN 1932-7447; TRN: US1801660
Grant/Contract Number:  
AC02-07CH11358; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 8; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Lii-Rosales, Ann, Han, Yong, Evans, James W., Jing, Dapeng, Zhou, Yinghui, Tringides, Michael C., Kim, Minsung, Wang, Cai-Zhuang, and Thiel, Patricia A. Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.7b12533.
Lii-Rosales, Ann, Han, Yong, Evans, James W., Jing, Dapeng, Zhou, Yinghui, Tringides, Michael C., Kim, Minsung, Wang, Cai-Zhuang, & Thiel, Patricia A. Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights. United States. https://doi.org/10.1021/acs.jpcc.7b12533
Lii-Rosales, Ann, Han, Yong, Evans, James W., Jing, Dapeng, Zhou, Yinghui, Tringides, Michael C., Kim, Minsung, Wang, Cai-Zhuang, and Thiel, Patricia A. Tue . "Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights". United States. https://doi.org/10.1021/acs.jpcc.7b12533. https://www.osti.gov/servlets/purl/1422772.
@article{osti_1422772,
title = {Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights},
author = {Lii-Rosales, Ann and Han, Yong and Evans, James W. and Jing, Dapeng and Zhou, Yinghui and Tringides, Michael C. and Kim, Minsung and Wang, Cai-Zhuang and Thiel, Patricia A.},
abstractNote = {Here in this paper, we present an extensive experimental study of the conditions under which Cu forms encapsulated islands under the top surface layers of graphite, as a result of physical vapor deposition of Cu on argon-ion-bombarded graphite. When the substrate is held at 800 K during deposition, conditions are optimal for formation of encapsulated multilayer Cu islands. Deposition temperatures below 600 K favor adsorbed Cu clusters, while deposition temperatures above 800 K favor a different type of feature that is probably a single-layer intercalated Cu island. The multilayer Cu islands are characterized with respect to size and shape, thickness and continuity of the graphitic overlayer, relationship to graphite steps, and stability in air. The experimental techniques are scanning tunneling microscopy and X-ray photoelectron spectroscopy. We also present an extensive study using density functional theory to compare stabilities of a wide variety of configurations of Cu atoms, Cu clusters, and Cu layers on/under the graphite surface. The only configuration that is significantly more stable under the graphite surface than on top of it, is a single Cu atom. This analysis leads us to conclude that formation of encapsulated Cu islands is kinetically driven, rather than thermodynamically driven.},
doi = {10.1021/acs.jpcc.7b12533},
journal = {Journal of Physical Chemistry. C},
number = 8,
volume = 122,
place = {United States},
year = {2018},
month = {2}
}

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