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Title: Electron nanoprobe induced oxidation: A simulation of direct-write purification

Electron beam direct-write has recently taken a large step forward with the advent of methods to purify deposits. This development has opened the door for future direct-write device prototyping and editing. In one such approach, an additional beam scanning procedure removes carbonaceous impurities via oxidation from metal–carbon deposits (e.g., PtC5) in the presence of H2O or O2 after deposition. So far, critical aspects of the oxidation reaction remain unclear; experiments reveal clearly that electron stimulated oxidation drives the process yet it is not understood why H2O purifies by a bottom-up mechanism while O2 purifies from the top-down. The simulation results presented here suggest that the chemisorption of dissolved O2 at buried Pt nanoparticle surfaces controls purification in the top-down case while both the high relative solubility coupled with weak physisorption of H2O explains the bottom-up process. Crucial too is the role that the carbonaceous contaminant itself has on the dissolution and diffusion of O2 and H2O. The results pave the way for simulation driven experiments where (1) the transient densification of the deposit can be accounted for in the initial deposit design stage and (2) the deposition and purification steps can be combined.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [3] ;  [4] ;  [5]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Graz Centre for Electron Microscopy, Graz (Austria)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Graz Centre for Electron Microscopy. Graz (Austria)
  5. Graz Centre for Electron Microscopy. Graz (Austria); Univ. of Technology, Graz (Austria)
Publication Date:
OSTI Identifier:
1209204
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 17; Journal Issue: 28; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY