Multilayer graphene (MLG) is expected to be a low-resistance and high-reliability interconnect material replacing copper (Cu) in nanoscale interconnects. Chemical vapor deposition (CVD) on catalytic metals is expected as a practical method for MLG deposition. To obtain high-quality MLG films without catalyst agglomeration by CVD, heat-resistant Co-W catalytic metals were investigated. The agglomeration of the Co-W catalytic metals was suppressed by increasing the W composition; however, MLG deposition was suppressed at the same time. The effects of W addition on the MLG growth were discussed from the viewpoints of the crystallographic change of the Co-W catalysts and chemical reactions. It was found that the Co grain size was reduced and the fcc Co formation was suppressed by W addition. In addition, graphite formation was supposed to be suppressed by W addition owing to the formation of phases other than fcc Co according to the Co-W-C phase diagram. With the optimum W concentration, MLG crystallinity was improved by high-temperature CVD using the heat-resistant Co-W catalytic metals (0.7 at. %) without agglomeration, compared with that in the case of using pure-Co catalysts.
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