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Emergence of metallic conductivity in ordered one-dimensional coordination polymer thin films upon reductive doping

(2021) ACS APPLIED MATERIALS & INTERFACES. 13(8). p.10249-10256
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Abstract
The prospect of introducing tunable electric conductivity in metal-organic coordination polymers is of high interest for nanoelectronic applications. As the electronic properties of these materials are strongly dependent on their microstructure, the assembly of coordination polymers into thin films with well-controlled growth direction and thickness is crucial for practical devices. Here, we report the deposition of one-dimensional (1D) coordination polymer thin films of N,N'-dimethyl dithiooxamidato-copper by atomic/molecular layer deposition. High out-of-plane ordering is observed in the resulting thin films suggesting the formation of a well-ordered secondary structure by the parallel alignment of the 1D polymer chains. We show that the electrical conductivity of the thin films is highly dependent on their oxidation state. The as-deposited films are nearly insulating with an electrical conductivity below 10(-10) S cm(-1) with semiconductor-like temperature dependency. Partial reduction with H-2 at elevated temperature leads to an increase in the electrical conductivity by 8 orders of magnitude. In the high-conductance state, metallic behavior is observed over the temperature range of 2-300 K. Density functional theory calculations indicate that the metallic behavior originates from the formation of a half-filled energy band intersecting the Fermi level with the conduction pathway formed by the Cu-S-Cu interaction between neighboring polymer chains.
Keywords
General Materials Science, coordination polymer, thin films, atomic layer, deposition, molecular layer deposition

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MLA
Nisula, Mikko, et al. “Emergence of Metallic Conductivity in Ordered One-Dimensional Coordination Polymer Thin Films upon Reductive Doping.” ACS APPLIED MATERIALS & INTERFACES, vol. 13, no. 8, 2021, pp. 10249–56, doi:10.1021/acsami.1c01738.
APA
Nisula, M., Karttunen, A., Solano Minuesa, E., Tewari, G., Karppinen, M., Minjauw, M., … Detavernier, C. (2021). Emergence of metallic conductivity in ordered one-dimensional coordination polymer thin films upon reductive doping. ACS APPLIED MATERIALS & INTERFACES, 13(8), 10249–10256. https://doi.org/10.1021/acsami.1c01738
Chicago author-date
Nisula, Mikko, Antti. Karttunen, Eduardo Solano Minuesa, Girish Tewari, Maarit Karppinen, Matthias Minjauw, Himanshu Jena, Pascal Van Der Voort, Dirk Poelman, and Christophe Detavernier. 2021. “Emergence of Metallic Conductivity in Ordered One-Dimensional Coordination Polymer Thin Films upon Reductive Doping.” ACS APPLIED MATERIALS & INTERFACES 13 (8): 10249–56. https://doi.org/10.1021/acsami.1c01738.
Chicago author-date (all authors)
Nisula, Mikko, Antti. Karttunen, Eduardo Solano Minuesa, Girish Tewari, Maarit Karppinen, Matthias Minjauw, Himanshu Jena, Pascal Van Der Voort, Dirk Poelman, and Christophe Detavernier. 2021. “Emergence of Metallic Conductivity in Ordered One-Dimensional Coordination Polymer Thin Films upon Reductive Doping.” ACS APPLIED MATERIALS & INTERFACES 13 (8): 10249–10256. doi:10.1021/acsami.1c01738.
Vancouver
1.
Nisula M, Karttunen A, Solano Minuesa E, Tewari G, Karppinen M, Minjauw M, et al. Emergence of metallic conductivity in ordered one-dimensional coordination polymer thin films upon reductive doping. ACS APPLIED MATERIALS & INTERFACES. 2021;13(8):10249–56.
IEEE
[1]
M. Nisula et al., “Emergence of metallic conductivity in ordered one-dimensional coordination polymer thin films upon reductive doping,” ACS APPLIED MATERIALS & INTERFACES, vol. 13, no. 8, pp. 10249–10256, 2021.
@article{8695299,
  abstract     = {{The prospect of introducing tunable electric conductivity in metal-organic coordination polymers is of high interest for nanoelectronic applications. As the electronic properties of these materials are strongly dependent on their microstructure, the assembly of coordination polymers into thin films with well-controlled growth direction and thickness is crucial for practical devices. Here, we report the deposition of one-dimensional (1D) coordination polymer thin films of N,N'-dimethyl dithiooxamidato-copper by atomic/molecular layer deposition. High out-of-plane ordering is observed in the resulting thin films suggesting the formation of a well-ordered secondary structure by the parallel alignment of the 1D polymer chains. We show that the electrical conductivity of the thin films is highly dependent on their oxidation state. The as-deposited films are nearly insulating with an electrical conductivity below 10(-10) S cm(-1) with semiconductor-like temperature dependency. Partial reduction with H-2 at elevated temperature leads to an increase in the electrical conductivity by 8 orders of magnitude. In the high-conductance state, metallic behavior is observed over the temperature range of 2-300 K. Density functional theory calculations indicate that the metallic behavior originates from the formation of a half-filled energy band intersecting the Fermi level with the conduction pathway formed by the Cu-S-Cu interaction between neighboring polymer chains.}},
  author       = {{Nisula, Mikko and Karttunen, Antti. and Solano Minuesa, Eduardo and Tewari, Girish and Karppinen, Maarit and Minjauw, Matthias and Jena, Himanshu and Van Der Voort, Pascal and Poelman, Dirk and Detavernier, Christophe}},
  issn         = {{1944-8244}},
  journal      = {{ACS APPLIED MATERIALS & INTERFACES}},
  keywords     = {{General Materials Science,coordination polymer,thin films,atomic layer,deposition,molecular layer deposition}},
  language     = {{eng}},
  number       = {{8}},
  pages        = {{10249--10256}},
  title        = {{Emergence of metallic conductivity in ordered one-dimensional coordination polymer thin films upon reductive doping}},
  url          = {{http://dx.doi.org/10.1021/acsami.1c01738}},
  volume       = {{13}},
  year         = {{2021}},
}

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