Establishment of innovational materials surface treatment / modification technology with using supercritical cluster plasma fluid

(A)我们在高压H2O和Xe直到超临界条件下产生了微米级的放电等离子体。在我们以前的论文中，我们报道了高压CO_2下击穿电压的两个特殊特征，第一个特征是在2.5 Mpa以上的巴氏曲线右手边的下移，第二个特征是在临界点附近击穿电压的急剧下降。我们已经从实验上证实了在H2O和Xe中也观察到了这些特征，尽管这两种材料之间有一些不同。考虑密度涨落项ED的理论拟合与实验结果符合得很好，特别是对Xe。我们认为这些独特的特征是由于电子-粒子截面、电离势-i和二次电子系数-‘的减小以及放电空间的变化所造成的。(B)我们诊断了超临界CO_2-DBD(介质棒…)的内态更多载流子放电)等离子体的微拉曼光谱。在等离子体内1388 cm‘附近的CO_2拉曼光谱中，没有观察到与CO_2浓度降低相对应的大波数移动。与其他高压条件相比，CO_2等离子体的拉曼光谱在临界点附近发生了局部移动。(C)在最佳条件下，用介质阻挡放电方法在Sc-CO_2和Ar气氛中成功地沉积了致密的铜碳复合膜。对SCCO_2产生的DBD和SCAR进行了诊断。根据V-I测量，我们的SCF等离子体的负电荷密度估计在10^&lt；18；cm^&lt；-3&gt；，这表明我们的SCF等离子体具有高密度的离子和电子，这是获得高活性等离子体所必需的。成功地制备了Cu/C薄膜，并研究了其与工频和外加电压的关系。在SCCO_2和SCAR中得到的薄膜的最大铜含量分别约为10%和60%。这一结果表明了Ar在合成材料细度方面的优势。在SCCO_2中沉积速率约为300 nm/min，在SCAR中沉积速率约为190 nm/min。这些结果表明，超临界流体等离子体工艺有可能实现金属薄膜的高速沉积。此外，还产生了带状微波微等离子体，其中衬底条件，如温度和与等离子体的距离，可以独立于等离子体控制。较少

(A) We generated micrometer-scale discharge plasma in high-pressure H_2O and Xe up to supercritical conditions. In our previous paper, we reported the existence of two peculiar features in the breakdown voltages under high-pressure CO_2. The first one was the downward shift at the right-hand side of Paschen's curve above about 2.5 MPa, and the second one was the drastic decrease in the breakdown voltages near the critical point. We have experimentally confirmed that these features are also observed in H_2O and Xe, even though there are some differences among these materials. Our theoretical fitting involving a density fluctuation term ED agrees well with the experimental results, especially for Xe. We suppose that these unique features are brought about by decreases in the electron-to-particle cross section □, ionization potential □_i, and secondary electron coefficient □', and changes in the discharge space.(B) We diagnosed the inner state of the supercritical CO_2-DBD (dielectric bar … More rier discharge) plasma by micro-Raman spectroscopy. From Raman band of CO_2 near 1388 cm' inside the plasma, the large-wavenumber shift, which correspond to a decrease of CO_2 density was not observed. It was also found that the Raman band obtained from CO_2 with the plasma showed a local shift near the critical point, comparing with other high-pressure condition.(C) Under an optimal condition, dense Cu-carbon composite films were successfully deposited by dielectric barrier discharge method in sc-CO_2 and Ar. Diagnostics of DBD generated in scCO_2 and scAr was conducted. From V-I measurement, the negative charge density of our SCF plasma was estimated to be more than 10^<18> cm^<-3>, which shows that our SCF plasma has a high density of ions and electrons, which are required for obtaining a highly reactive plasma. Cu/C films were successfully obtained and its dependence on power frequency and applied voltage was studied. Cu content of films obtained in an scCO_2 and scAr was about 10 % and 60 % maximum, respectively. This result suggests the advantage of Ar in terms of the fineness of synthesized materials. The deposition rate was about 300 nm/min in scCO_2 and 190 nm/min in scAr. These results suggest the potential of an SCF plasma processing for realization of high-speed metal film deposition. Moreover, strip-line microwave micro plasma was also generated, in which substrate conditions, such as temperature and distance from plasma, can be controlled independently of plasma. Less