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Activation of the dimers and tetramers of metal amidinate atomic layer deposition precursors upon adsorption on silicon oxide surfaces

  • Bo Chen
  • , Yichen Duan
  • , Yunxi Yao
  • , Qiang Ma
  • , Jason P. Coyle
  • , Seán T. Barry
  • , Andrew V. Teplyakov
  • , Francisco Zaera
  • University of Delaware
  • University of California at Riverside
  • Carleton University

Research output: Contribution to journalArticlepeer-review

14 Scopus citations

Abstract

The gas-phase structure of three copper amidinate compounds, copper(I)-N,N′-di-sec-butyl-acetamidinate (1), copper(I)-N-sec-butyl-2-iminopyrrolidinate (2), and copper(I)-N-tert-butyl-5,5-dimethyl-2-iminopyrrolidinate (3), and their initial adsorption on silicon oxide surfaces, were characterized by a combination of experimental measurements and density-functional theory (DFT) calculations. These compounds have previously been shown to crystallize in dimeric or tetrameric form, and liquid-injection field desorption ionization mass spectrometry data proved that such structures are retained upon vaporization into the gas phase (dimers for the first and third compounds, a tetramer for the second). Results from DFT calculations of the relative energies of formation of the monomers, dimers, and tetramers confirmed the experimental results. Adsorption on the surface of silicon oxide films was determined, based on additional DFT calculations, to lead to the binding of the copper amidinates preferentially as dimers; although the monomers form stronger bonds to the silicon surface because they bind directly through their copper atom, this cannot fully compensate for the large energy required to break the dimers apart. N 1s x-ray photoelectron spectroscopy data were used to corroborate both the presence of the dimers on the surface with the second (2) precursor and the threshold for their surface decomposition around room temperature. The behavior of the third compound is somewhat more complex, with some decomposition possibly happening immediately upon adsorption at 100 K.

Original languageEnglish
Article number01B124
JournalJournal of Vacuum Science and Technology A: Vacuum, Surfaces and Films
Volume35
Issue number1
DOIs
StatePublished - Jan 1 2017

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