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Register a new userRaman micro-spectroscopy as a tool to measure the absorption coefficient and the erosion rate of hydrogenated amorphous carbon films heat-treated under hydrogen bombardment
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Cedric Pardanaud
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We present a fast and simple way to determine the erosion rate and absorption coefficient of hydrogenated amorphous carbon films exposed to a hydrogen atomic source based on ex-situ Raman micro-spectroscopy. Results are compared to ellipsometry measurement. The method is applied to films eroded at different temperatures. A maximum of the erosion rate is found at ~ 450 {degree}C in agreement with previous results. This technique is suitable for future quantitative studies on the erosion of thin carbonaceous films, especially of interest for plasma wall interactions occurring in thermonuclear fusion devices.
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We revisit here how Raman spectroscopy can be used to estimate the H content in hard hydrogenated amorphous carbon layers. The H content was varied from 2 at.% to 30 at.%, using heat treatments of a a-C:H, from room temperature to 1300 K and was determined independently using ion beam analysis. We examine the correlation of various Raman parameters and the consistency of their thermal evolution with thermo-desorption results. We identify a weak band at 860 cm-1 attributed to H bonded to C(sp2). We show that the HD/HG parameter (Height ratio between the D and G bands) is quasi-linear in the full range of H content and can thus be used to estimate the H content. Conversely, we show that the m/HG parameter (ratio between the photoluminescence background, m, and the height of the G band), often used to estimate the H content, should be used with care, first because it is sensitive to various photoluminescence quenching processes and second because it is not sensitive to H bonded to C(sp2).
We study the kinetics of the H release from plasma-deposited hydrogenated amorphous carbon films under isothermal heating at 450, 500 and 600 {degree}C for long times up to several days using in situ Raman microscopy. Four Raman parameters are analyzed. They allow the identification of different processes such as the carbon network reorganization and the H release from sp3 or sp2 carbon atoms and the corresponding timescales. Carbon reorganization with aromatization and loss of sp3 hybridization occurs first in 100 minutes at 500 {degree}C. The final organization is similar at all investigated temperatures. Full H release from sp3 carbon occurs on a longer timescale of about 10 hours while H release from sp2 carbon atoms is only partial, even after several days. All these processes occur more rapidly with higher initial H content, in agreement with what is known about the stability of these types of films. A quantitative analysis of these kinetics studies gives valuable information about the microscopic processes at the origin of the H release through the determination of activation energies.
Raman spectroscopy has been employed to distinguish between the Raman spectrum of pristine hydrogenated diamond like carbon (PHDLC) and that of electrochemically hydrogenated diamond like carbon (ECHDLC). The enhancement of the background photoluminescence (PL) in the Raman spectrum and broadening of PL spectrum of ECHDLC are identified to be due to increase of sp3 C-H density onto the PHDLC surface, during novel electrochemical process of hydrogenation of sp2 C=C into sp3 C-H.
In this work, we studied amorphous carbon ($a$-C) thin films deposited using direct current (dc) and high power impulse magnetron sputtering (HiPIMS) techniques. The microstructure and electronic properties reveal subtle differences in $a$-C thin films deposited by two techniques. While, films deposited with dcMS have a smooth texture typically found in $a$-C thin films, those deposited with HiPIMS consist of dense hillocks surrounded by a porous microstructure. The density of $a$-C thin films is a decisive parameter to judge their quality. Often, x-ray reflectivity (XRR) has been used to measure the density of carbon thin films. From the present work, we find that determination of density of carbon thin films, specially those with a thickness of few tens of nm, may not be accurate with XRR due to a poor scattering contrast between the film and substrate. By utilizing neutron reflectivity (NR) in the time of flight mode, a technique not commonly used for carbon thin films, we could accurately measure differences in the densities of $a$-C thin films deposited using dcMS and HiPIMS.
By using molecular dynamics simulation, formation mechanisms of amorphous carbon in particular sp${}^3$ rich structure was researched. The problem that reactive empirical bond order potential cannot represent amorphous carbon properly was cleared in the transition process from graphite to diamond by high pressure and the deposition process of amorphous carbon thin films. Moreover, the new potential model which is based on electron distribution simplified as a point charge was developed by using downfolding method. As a result, the molecular dynamics simulation with the new potential could demonstrate the transition from graphite to diamond at the pressure of 15 GPa corresponding to experiment and the deposition of sp${}^3$ rich amorphous carbon.
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