Direct growth of graphene-like (GL) films (nano-crystalline graphite films) on single crystal quartz substrates by chemical vapor deposition (CVD) from methane and molecular beam growth (MBG) is reported. The GL films have been characterized by means of Raman spectroscopy, atomic force microscopy and electrical measurements. Raman spectroscopy reveals nanocrystalline structure of the films grown at different conditions. The thinnest CVD grown GL films obtained so far have a thickness of 1.5 nm, a relatively rough surface structure and electrical conductivity in the range of 20 kΩ/square. Low temperature Hall-effect measurements performed on these films have revealed that the major charge carriers are holes with mobility of 40 cm2/Vs at room temperature. While inferior to graphene in terms of electronic properties, the graphene-like films possess very high chemical sensitivity. Study of MBG grown films revealed formation of a non-conductive carbon layer of low crystallinity on the initial stage of the growth process.
In order to study the influence of the quartz substrate on the film formation process we performed ab initio simulation of the MBG process. For this simulation we used an atom-by-atom approach, which, we believe, is a closer approximation to the real molecular beam deposition process reported so far. The simulation showed that the initial formation of the film follows the atomic structure of the substrate. This leads to a high content of sp3 hybridized atoms at the initial stage of growth and explains formation of a non-conductive film. Additionally, we demonstrated how a non-conductive film becomes conductive with the increase of the film thickness. These results agree fairly well with the data obtained by AFM, electrical, and Raman measurements conducted on the films grown by MBG.
High chemical sensitivity of GL films has been demonstrated by measuring the change in their conductance during exposure to a NO2-containing atmosphere. Sensitivity of CVD grown GL films have been shown to be superior to that of MBG grown GL films. The stimulating action of ultraviolet light illumination on the chemical sensitivity has been found to be comparable to that of carbon nanotubes. A detection limit of 40 ppb (parts-per-billion) of NO2 diluted in an inert atmosphere has been estimated from the signal-to-noise ratio analysis. The optimal electrical conductance, high chemical sensitivity as well as the simple growth method make the CVD grown GL films promising for practical applications as a chemically sensitive material.
Results obtained during this work were presented on several conferences: Gotham-Metro Condensed Matter Meeting (New York, NY), April 2010 and November 2012; American Physical Society March Meeting (Dallas, TX), March 2011; Nanoelectronic Devices for Defense & Security (NANO-DDS) Conference (Brooklyn, NY), August 2011. Two papers (http://dx.doi.org/10.1016/j.snb.2013.02.067 and http://dx.doi.org/10.1016/j.snb.2013.06.023) were published based on the results presented in this thesis.
|Advisor:||Zaitsev, Alexander M.|
|Commitee:||Gorokhovsky, Anshel A., Kuklov, Anatoly, Lozovskyi, Oleksandr, Vitkalov, Sergey A., Zaitsev, Alexander M.|
|School:||City University of New York|
|School Location:||United States -- New York|
|Source:||DAI-B 75/03(E), Dissertation Abstracts International|
|Subjects:||Nanoscience, Molecular physics|
|Keywords:||Chemical vapor deposition, Density functional theory, Graphene, Molecular beam growth, Thin films|
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