The microscopic effect of electronic excitations on the transformation of few-layer graphene into sp³-bonded carbon nanofilm is examined through static and real-time propagation of time-dependent density-functional theory. Statically, presence of holes in high-lying valence bands is shown to reduce the energy barrier substantially. Dynamics of excited state electrons combined with Ehrenfest atomic motions reveals that non-thermal fast transformation from sp² to sp³ can happen within a few hundreds femtoseconds. We suggest that once the efficient path of sp³ carbon surface passivation is provided, the excitation from π$\pi$ to π$\pi$ bands of few-layer graphenes can be utilized to achieve the transformation into nanoscale sp³-bonded carbon film without heating process.

通过基于时间的密度泛函理论的静态和实时传播，研究了电子激发对几层石墨烯向sp ³键合的碳纳米膜转化的微观影响。静态地，高价价带中的空穴的存在显示出显着降低了能垒。激发态电子的动力学结合埃伦菲斯特原子运动揭示了从sp ²到sp ^3的非热快速转变可以在几百飞秒内发生。我们建议，一旦提供了sp ³碳表面钝化的有效路径，就可以从π激发。$\pi$到π$\pi$可以利用几层石墨烯的能带在不进行加热的情况下实现向纳米级sp ³键合碳膜的转化。