Effect of Nitrogen on the Growth of (100)-, (110)-, and (111)-Oriented Diamond Films

Abstract

The aim of this research is the study of hydrogen abstraction reactions and methyl adsorption reactions on the surfaces of (100), (110), and (111) oriented nitrogen-doped diamond through first-principles density-functional calculations. The three steps of the growth mechanism for diamond thin films are hydrogen abstraction from the diamond surface, methyl adsorption on the diamond surface, and hydrogen abstraction from the methylated diamond surface. The activation energies for hydrogen abstraction from the surface of nitrogen-undoped and nitrogen-doped diamond (111) films were −0.64 and −2.95 eV, respectively. The results revealed that nitrogen substitution was beneficial for hydrogen abstraction and the subsequent adsorption of methyl molecules on the diamond (111) surface. The adsorption energy for methyl molecules on the diamond surface was generated during the growth of (100)-, (110)-, and (111)-oriented diamond films. Compared with nitrogen-doped diamond (100) films, adsorption energies for methyl molecule adsorption were by 0.14 and 0.69 eV higher for diamond (111) and (110) films, respectively. Moreover, compared with methylated diamond (100), the activation energies for hydrogen abstraction were by 0.36 and 1.25 eV higher from the surfaces of diamond (111) and (110), respectively. Growth mechanism simulations confirmed that nitrogen-doped diamond (100) films were preferred, which was in agreement with the experimental and theoretical observations of diamond film growth.

Rational design of diamond through microstructure engineering: From synthesis to applications

“…During the CVD growth process, 24,[157][158][159][160] the carboncontaining gas source (methane [CH 4 ], etc.) is activated into sp 2 or sp 3 species, which are grafted onto the dangling bonds on the vacancies to accumulate and form diamond.…”

Enhancing Luminescence Properties of Lab-Grown Diamond Films with Upconversion Nanoparticles for High-Performance Surface Temperature Sensing in Advanced Applications

“…Synthesis processes for obtaining luminescent diamonds of above type require strict control for impurity incorporation during diamond growth, and the processes can be hindered by factors like surface roughness, nonuniform crystal growth, etc. 10,11 Advanced techniques such as chemical vapor deposition (CVD) and high-pressure hightemperature (HPHT) methods circumvent the above-mentioned hindrances to a certain extent. 12,13 However, these techniques introduce additional complexities in maintaining a balance between crystal quality, defect concentration in different planes, 14 and fluorescence efficiency.…”

“…Furthermore, optimization of growth parameters, annealing cycles, and postsynthesis treatments is essential to ensure a desired level of fluorescence intensity. Synthesis processes for obtaining luminescent diamonds of above type require strict control for impurity incorporation during diamond growth, and the processes can be hindered by factors like surface roughness, nonuniform crystal growth, etc. , Advanced techniques such as chemical vapor deposition (CVD) and high-pressure high-temperature (HPHT) methods circumvent the above-mentioned hindrances to a certain extent. , However, these techniques introduce additional complexities in maintaining a balance between crystal quality, defect concentration in different planes, and fluorescence efficiency . Hence, the synthesis of luminescent diamonds with uniform and reproducible optical characteristics remains a challenge.…”