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Excited States of Pt(PF3)(4) and Their Role in Focused Electron Beam Nanofabrication

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2016
Authors
Zlatar, Matija
Allan, Michael
Fedor, Juraj
Article (Published version)
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Abstract
Electron induced chemistry of metal-containing precursor molecules is central in focused electron beam induced deposition (FEBID). While some elementary processes leading to precursor decomposition were quantitatively characterized, data for neutral dissociation is missing. We provide this data for the model precursor Pt(PF3)(4) by using the available cross sections for electronic excitation and characterizing fragmentation of the excited states theoretically by TDDFT. The potential energy curves for a number of states visible in the experimental electron energy loss spectra are dissociative, either directly or via conical intersections, indicating that the quantum yield for dissociation is close to 100%. Taking into account typical electron energy distribution at the FEBID spot reveals that the importance of neutral dissociation exceeds that of dissociative electron attachment, which has been so far considered to be the dominant decomposition process. We thus established neutral disso...ciation as an important, albeit often neglected, channel for FEBID using Pt(PF3)(4). The calculations revealed a number of other phenomena that can play a role in electron induced chemistry of this compound, e.g., a considerable increase of bond dissociation energy with sequential removal of multiple ligands.

Source:
Journal of Physical Chemistry C, 2016, 120, 19, 10667-10674
Publisher:
  • Amer Chemical Soc, Washington
Projects:
  • Rational design and synthesis of biologically active and coordination compounds and functional materials, relevant for (bio)nanotechnology (RS-172035)
  • Swiss National Science Foundation - 200020-144367/1
  • COST action - CM1301 CELINA

DOI: 10.1021/acs.jpcc.6b02660

ISSN: 1932-7447

WoS: 000376417500060

Scopus: 2-s2.0-84971318229
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URI
http://cer.ihtm.bg.ac.rs/handle/123456789/2022
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