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Title: Reverse-engineering of graphene on metal surfaces: a case study of embedded ruthenium

Abstract

Using scanning tunneling microscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy, we show that Ru forms metallic nanoislands on graphite, covered by a graphene monolayer. These islands are air-stable, contain 2-4 layers of Ru, and have diameters on the order of 10 nm. To produce these nanoislands two conditions must be met during synthesis. The graphite surface must be ion-bombarded, and subsequently held at elevated temperature (1000-1180 K) during Ru deposition. A coincidence lattice forms between the graphene overlayer and the Ru island top. Its characteristics – coincidence lattice constant, corrugation amplitude, and variation of carbon lattice appearance within the unit cell – closely resemble the well-established characteristics of single-layer graphene on the (0001) surface of bulk Ru. Quantitative analysis of the graphene lattice in relation to the coincidence lattice on the island tops shows that the twodimensional lattice constant of the underlying metal equals that of bulk Ru(0001), within experimental error. The embedded Ru islands are energetically favored over on-top (adsorbed) islands, based on density-functional-theory calculations for Ru films with 1-3 Ru layers. We propose a formation mechanism in which Ru atoms intercalate via defects that act as entry portals to the carbon galleries, followed by nucleation and growthmore » in the galleries. In this model, high deposition temperature is necessary to prevent blockage of entry portals.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [1];  [1];  [1];  [1];  [1];  [3]; ORCiD logo [1]
  1. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
  2. Ames Lab., Ames, IA (United States)
  3. Hong Kong Univ. of Science and Technology (China)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1477243
Report Number(s):
IS-J-9745
Journal ID: ISSN 0957-4484
Grant/Contract Number:  
AC02-05CH11231; AC02-06CH11357; AC02-07CH11358; ACI-1548562
Resource Type:
Accepted Manuscript
Journal Name:
Nanotechnology
Additional Journal Information:
Journal Volume: 29; Journal Issue: 50; Journal ID: ISSN 0957-4484
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Lii-Rosales, Ann, Han, Yong, Yu, Ka Man, Jing, Dapeng, Anderson, Nathaniel, Vaknin, David, Tringides, Michael C., Evans, James W., Altman, Michael S., and Thiel, Patricia A. Reverse-engineering of graphene on metal surfaces: a case study of embedded ruthenium. United States: N. p., 2018. Web. doi:10.1088/1361-6528/aae1e3.
Lii-Rosales, Ann, Han, Yong, Yu, Ka Man, Jing, Dapeng, Anderson, Nathaniel, Vaknin, David, Tringides, Michael C., Evans, James W., Altman, Michael S., & Thiel, Patricia A. Reverse-engineering of graphene on metal surfaces: a case study of embedded ruthenium. United States. https://doi.org/10.1088/1361-6528/aae1e3
Lii-Rosales, Ann, Han, Yong, Yu, Ka Man, Jing, Dapeng, Anderson, Nathaniel, Vaknin, David, Tringides, Michael C., Evans, James W., Altman, Michael S., and Thiel, Patricia A. Tue . "Reverse-engineering of graphene on metal surfaces: a case study of embedded ruthenium". United States. https://doi.org/10.1088/1361-6528/aae1e3. https://www.osti.gov/servlets/purl/1477243.
@article{osti_1477243,
title = {Reverse-engineering of graphene on metal surfaces: a case study of embedded ruthenium},
author = {Lii-Rosales, Ann and Han, Yong and Yu, Ka Man and Jing, Dapeng and Anderson, Nathaniel and Vaknin, David and Tringides, Michael C. and Evans, James W. and Altman, Michael S. and Thiel, Patricia A.},
abstractNote = {Using scanning tunneling microscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy, we show that Ru forms metallic nanoislands on graphite, covered by a graphene monolayer. These islands are air-stable, contain 2-4 layers of Ru, and have diameters on the order of 10 nm. To produce these nanoislands two conditions must be met during synthesis. The graphite surface must be ion-bombarded, and subsequently held at elevated temperature (1000-1180 K) during Ru deposition. A coincidence lattice forms between the graphene overlayer and the Ru island top. Its characteristics – coincidence lattice constant, corrugation amplitude, and variation of carbon lattice appearance within the unit cell – closely resemble the well-established characteristics of single-layer graphene on the (0001) surface of bulk Ru. Quantitative analysis of the graphene lattice in relation to the coincidence lattice on the island tops shows that the twodimensional lattice constant of the underlying metal equals that of bulk Ru(0001), within experimental error. The embedded Ru islands are energetically favored over on-top (adsorbed) islands, based on density-functional-theory calculations for Ru films with 1-3 Ru layers. We propose a formation mechanism in which Ru atoms intercalate via defects that act as entry portals to the carbon galleries, followed by nucleation and growth in the galleries. In this model, high deposition temperature is necessary to prevent blockage of entry portals.},
doi = {10.1088/1361-6528/aae1e3},
journal = {Nanotechnology},
number = 50,
volume = 29,
place = {United States},
year = {Tue Oct 09 00:00:00 EDT 2018},
month = {Tue Oct 09 00:00:00 EDT 2018}
}

Journal Article:
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Cited by: 19 works
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Figures / Tables:

Figure 1 Figure 1: Representative topographic STM images, and corresponding line profiles, after five separate depositions of Ru on $i$-graphite at (a-c) 300 K, (d-f) 900 K, (g-i) 1000 K, (j-l) 1050 K, and (m-o) 1180 K. In (h), two examples of short features are marked by arrows. In (n), all islandsmore » are short, illustrating the progression from predominantly tall to short features. Tunneling conditions are: (a,b) +4.8 V, 0.27 nA; (d,e) +4.5 V, 0.25 nA; (g) +1.0 V, 0.26 nA; (h) +1.2 V, 0.27 nA; (j,k) +1.1 V, 0.26 nA; (m) +1.2 V, 0.27 nA; and (n) +1.6 V, 0.27 nA.« less

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