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

Fowlkes, J. D.; Geier, B.; Lewis, B. B.; Rack, P. D.; Stanford, M. G.; Winkler, R.; Plank, H.

doi:10.1039/C5CP01196E

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

Journal Article · Mon Jun 01 00:00:00 EDT 2015 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C5CP01196E· OSTI ID:1209204

Fowlkes, J. D. ^[1]; Geier, B. ^[2]; Lewis, B. B. ^[3]; Rack, P. D. ^[1]; Stanford, M. G. ^[3]; Winkler, R. ^[4]; Plank, H. ^[5]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Graz Centre for Electron Microscopy, Graz (Austria)
Univ. of Tennessee, Knoxville, TN (United States)
Graz Centre for Electron Microscopy. Graz (Austria)
Graz Centre for Electron Microscopy. Graz (Austria); Univ. of Technology, Graz (Austria)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1209204

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 28 Vol. 17; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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