{"title":"反应气体预热加速类金刚石膜低温MW-CVD生长纳米晶金刚石成核","authors":"Brijmohan Paramanik, Debajyoti Das","doi":"10.1016/j.jpcs.2025.112554","DOIUrl":null,"url":null,"abstract":"<div><div>The reacting gas pre-heating is presented as a means to enhance the diamond nucleation density in the diamond-like carbon (DLC) films with embedded nanocrystallinity (NCD). Utilizing C<sub>2</sub>H<sub>2</sub> as the precursor gas having low ionization potential, allows for faster NCD-embedded DLC growth. The additions of H<sub>2</sub>, a conventional dilution gas, along with CO<sub>2</sub>, a weak oxidant, increase the chemical activity of the growth precursors and aids in the removal of a-C phase from the growth site. Notably, the bandgap widens from 3.40 to 3.48 eV, while the <em>sp</em><sup>3</sup>/<em>sp</em><sup>2</sup> ratio increases from 1.9 to 2.38. Raman spectroscopy reveals higher I<sub>Dia</sub>/I<sub>G</sub> (0.85), I<sub>Dia</sub>/I<sub>D</sub> (0.94), alongside a lower I<sub>D</sub>/I<sub>G</sub> ratio (0.90) for the film grown at the optimum gas-pre-heating temperature (T<sub>G</sub> = 250 °C) demonstrate the superiority of the less-stressed DLC network, with higher optical transmittance of ∼93% at 600 nm. The DLC matrix developed at a substrate-temperature (T<sub>S</sub>) ∼300 °C holds a good quality nano-diamond phase (grain size ∼8–10 nm), containing distinct <em>trans</em>-PA peaks (1171 and 1497 cm<sup>−1</sup>) and diamond peaks (1333 cm<sup>−1</sup>) as the signature. The preheating of the source gas mixture elevates the precursor gas molecules’ vibrational energy states, facilitating the conversion of C<sub>2</sub>H<sub>2</sub> to CH<sub>3</sub>, which is energetically favorable for diamond nucleation.</div></div>","PeriodicalId":16811,"journal":{"name":"Journal of Physics and Chemistry of Solids","volume":"199 ","pages":"Article 112554"},"PeriodicalIF":4.9000,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Accelerating nanocrystalline-diamond nucleation in the low-temperature MW-CVD growth of diamond-like carbon films via reacting-gas pre-heating\",\"authors\":\"Brijmohan Paramanik, Debajyoti Das\",\"doi\":\"10.1016/j.jpcs.2025.112554\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The reacting gas pre-heating is presented as a means to enhance the diamond nucleation density in the diamond-like carbon (DLC) films with embedded nanocrystallinity (NCD). Utilizing C<sub>2</sub>H<sub>2</sub> as the precursor gas having low ionization potential, allows for faster NCD-embedded DLC growth. The additions of H<sub>2</sub>, a conventional dilution gas, along with CO<sub>2</sub>, a weak oxidant, increase the chemical activity of the growth precursors and aids in the removal of a-C phase from the growth site. Notably, the bandgap widens from 3.40 to 3.48 eV, while the <em>sp</em><sup>3</sup>/<em>sp</em><sup>2</sup> ratio increases from 1.9 to 2.38. Raman spectroscopy reveals higher I<sub>Dia</sub>/I<sub>G</sub> (0.85), I<sub>Dia</sub>/I<sub>D</sub> (0.94), alongside a lower I<sub>D</sub>/I<sub>G</sub> ratio (0.90) for the film grown at the optimum gas-pre-heating temperature (T<sub>G</sub> = 250 °C) demonstrate the superiority of the less-stressed DLC network, with higher optical transmittance of ∼93% at 600 nm. The DLC matrix developed at a substrate-temperature (T<sub>S</sub>) ∼300 °C holds a good quality nano-diamond phase (grain size ∼8–10 nm), containing distinct <em>trans</em>-PA peaks (1171 and 1497 cm<sup>−1</sup>) and diamond peaks (1333 cm<sup>−1</sup>) as the signature. The preheating of the source gas mixture elevates the precursor gas molecules’ vibrational energy states, facilitating the conversion of C<sub>2</sub>H<sub>2</sub> to CH<sub>3</sub>, which is energetically favorable for diamond nucleation.</div></div>\",\"PeriodicalId\":16811,\"journal\":{\"name\":\"Journal of Physics and Chemistry of Solids\",\"volume\":\"199 \",\"pages\":\"Article 112554\"},\"PeriodicalIF\":4.9000,\"publicationDate\":\"2025-04-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Physics and Chemistry of Solids\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0022369725000058\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/1/2 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Physics and Chemistry of Solids","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022369725000058","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/1/2 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Accelerating nanocrystalline-diamond nucleation in the low-temperature MW-CVD growth of diamond-like carbon films via reacting-gas pre-heating
The reacting gas pre-heating is presented as a means to enhance the diamond nucleation density in the diamond-like carbon (DLC) films with embedded nanocrystallinity (NCD). Utilizing C2H2 as the precursor gas having low ionization potential, allows for faster NCD-embedded DLC growth. The additions of H2, a conventional dilution gas, along with CO2, a weak oxidant, increase the chemical activity of the growth precursors and aids in the removal of a-C phase from the growth site. Notably, the bandgap widens from 3.40 to 3.48 eV, while the sp3/sp2 ratio increases from 1.9 to 2.38. Raman spectroscopy reveals higher IDia/IG (0.85), IDia/ID (0.94), alongside a lower ID/IG ratio (0.90) for the film grown at the optimum gas-pre-heating temperature (TG = 250 °C) demonstrate the superiority of the less-stressed DLC network, with higher optical transmittance of ∼93% at 600 nm. The DLC matrix developed at a substrate-temperature (TS) ∼300 °C holds a good quality nano-diamond phase (grain size ∼8–10 nm), containing distinct trans-PA peaks (1171 and 1497 cm−1) and diamond peaks (1333 cm−1) as the signature. The preheating of the source gas mixture elevates the precursor gas molecules’ vibrational energy states, facilitating the conversion of C2H2 to CH3, which is energetically favorable for diamond nucleation.
期刊介绍:
The Journal of Physics and Chemistry of Solids is a well-established international medium for publication of archival research in condensed matter and materials sciences. Areas of interest broadly include experimental and theoretical research on electronic, magnetic, spectroscopic and structural properties as well as the statistical mechanics and thermodynamics of materials. The focus is on gaining physical and chemical insight into the properties and potential applications of condensed matter systems.
Within the broad scope of the journal, beyond regular contributions, the editors have identified submissions in the following areas of physics and chemistry of solids to be of special current interest to the journal:
Low-dimensional systems
Exotic states of quantum electron matter including topological phases
Energy conversion and storage
Interfaces, nanoparticles and catalysts.