Tuning of solid-to-solid structural transitions in amorphous carbon films by optical pumping and chemical modification

Amorphous carbon (a-C) attracts great attention in tribology research and thin film technologies due to its versatile properties. However, high temperatures and mechanical stresses may cause significant changes in the structural ordering of the a-C network. We present an optical method to initiate structural ordering and to probe solid-to-solid structural transitions of element modified a-C films. A pulsed pump laser introduces heat into the film in a controlled manner, while a second laser probes confocally the first- and second-order Raman scattering signatures of the a-C network. For low pump power, the number of defects and non-sixfold aromatic rings is reduced. A further increase in the laser power leads to sharply evolved changes in the Raman scattering features, indicating a transition from a-C to defected graphite and an effusion of hydrogen. Moreover, graphite-dominant defect relaxation and an enhancement in hexagonal lattice areas occur and, in turn, activate second-order Raman scattering lines. A rising laser power subsequently results in progressive graphitization. Chemical modification of the films with Si or Cu enhances their thermal stability and even shifts the upper thermal limit of the film ablation, while the a-C:W film demonstrates a more efficient enrichment of nanocrystalline graphitic clusters.