Finite size effect of proton-conductivity of amorphous silicate thin films based on mesoscopic fluctuation of glass network

Yoshitaka Aoki, Hiroki Habazaki, Shinji Nagata, Aiko Nakao, Toyoki Kunitake, Shu Yamaguchi

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

The finite size effect of proton conductivity of amorphous silicate thin films, a-M0.1Si0.9Ox (M = Al, Ga, Hf, Ti, Ta, and La), was investigated. The proton conductivity across films, σ, was measured in dry air by changing the thickness in the range of 10-1000 nm. σ of the films with M = Al, Ga, and Ta was elevated in a power law by decreasing thickness into less than a few hundred nanometers, and the increment was saturated at a thickness of several 10's of nanometers. On the other hand, σ of the films with M = Hf, Ti, and La was not related to the decrease of the thickness in the range of >10 nm. Thickness-dependent conductivity of the former could be numerically simulated by a percolative resistor network model that involves the randomly distributed array of two kinds of resistors R 1 and R2 (R1 > R2) in the form of a simple cubic-type lattice. High-resolution TEM clarified that a-M 0.1Si0.9Ox films involved heterogeneous microstructures made of the condensed domain and the surrounding uncondensed matrix due to the fluctuation of glass networks on the nanometer scale. The condensed domain had a wormlike shape with an average length of several 10's of nanometers and performed the role of the proton conduction pathway penetrating through the poorly conducting matrix. It was concluded that the thickness-dependent conductivity could be identical to finite-size scaling of the percolative network of the interconnected domains in the nanometer range.

Original languageEnglish
Pages (from-to)3471-3479
Number of pages9
JournalJournal of the American Chemical Society
Volume133
Issue number10
DOIs
Publication statusPublished - Mar 16 2011
Externally publishedYes

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Silicates
Proton conductivity
Glass
Protons
Thin films
Resistors
Air
Transmission electron microscopy
Microstructure

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Finite size effect of proton-conductivity of amorphous silicate thin films based on mesoscopic fluctuation of glass network. / Aoki, Yoshitaka; Habazaki, Hiroki; Nagata, Shinji; Nakao, Aiko; Kunitake, Toyoki; Yamaguchi, Shu.

In: Journal of the American Chemical Society, Vol. 133, No. 10, 16.03.2011, p. 3471-3479.

Research output: Contribution to journalArticle

Aoki, Yoshitaka ; Habazaki, Hiroki ; Nagata, Shinji ; Nakao, Aiko ; Kunitake, Toyoki ; Yamaguchi, Shu. / Finite size effect of proton-conductivity of amorphous silicate thin films based on mesoscopic fluctuation of glass network. In: Journal of the American Chemical Society. 2011 ; Vol. 133, No. 10. pp. 3471-3479.
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abstract = "The finite size effect of proton conductivity of amorphous silicate thin films, a-M0.1Si0.9Ox (M = Al, Ga, Hf, Ti, Ta, and La), was investigated. The proton conductivity across films, σ, was measured in dry air by changing the thickness in the range of 10-1000 nm. σ of the films with M = Al, Ga, and Ta was elevated in a power law by decreasing thickness into less than a few hundred nanometers, and the increment was saturated at a thickness of several 10's of nanometers. On the other hand, σ of the films with M = Hf, Ti, and La was not related to the decrease of the thickness in the range of >10 nm. Thickness-dependent conductivity of the former could be numerically simulated by a percolative resistor network model that involves the randomly distributed array of two kinds of resistors R 1 and R2 (R1 > R2) in the form of a simple cubic-type lattice. High-resolution TEM clarified that a-M 0.1Si0.9Ox films involved heterogeneous microstructures made of the condensed domain and the surrounding uncondensed matrix due to the fluctuation of glass networks on the nanometer scale. The condensed domain had a wormlike shape with an average length of several 10's of nanometers and performed the role of the proton conduction pathway penetrating through the poorly conducting matrix. It was concluded that the thickness-dependent conductivity could be identical to finite-size scaling of the percolative network of the interconnected domains in the nanometer range.",
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