General Physics Institute, Russian Academy of Sciences, 38 Vavilov Street, 119991 Moscow, Russia.
Small. 2010 Mar 8;6(5):687-94. doi: 10.1002/smll.200901587.
An efficient method to investigate the microstructure and spatial distribution of nitrogen and nitrogen-vacancy (N-V) defects in detonation nanodiamond (DND) with primary particle sizes ranging from approximately 3 to 50 nm is presented. Detailed analysis reveals atomic nitrogen concentrations as high as 3 at% in 50% of diamond primary particles with sizes smaller than 6 nm. A non-uniform distribution of nitrogen within larger primary DND particles is also presented, indicating a preference for location within the defective central part or at twin boundaries. A photoluminescence (PL) spectrum with well-pronounced zero-phonon lines related to the N-V centers is demonstrated for the first time for electron-irradiated and annealed DND particles at continuous laser excitation. Combined Raman and PL analysis of DND crystallites dispersed on a Si substrate leads to the conclusion that the observed N-V luminescence originates from primary particles with sizes exceeding 30 nm. These findings demonstrate that by manipulation of the size/nitrogen content in DND there are prospects for mass production of nanodiamond photoemitters based on bright and stable luminescence from nitrogen-related defects.
本文提出了一种高效的方法,用于研究粒径约为 3 至 50nm 的爆轰纳米金刚石(DND)中的氮和氮空位(N-V)缺陷的微观结构和空间分布。详细分析表明,在粒径小于 6nm 的 50%金刚石初级颗粒中,原子氮浓度高达 3at%。较大的 DND 初级颗粒中氮的分布也不均匀,表明氮优先位于有缺陷的中心部分或孪晶边界处。首次在连续激光激发下,对电子辐照和退火后的 DND 颗粒进行了光致发光(PL)光谱测试,结果表明存在与 N-V 中心相关的零声子线。通过对分散在 Si 衬底上的 DND 纳米晶的 Raman 和 PL 分析,得出结论:观察到的 N-V 发光源自粒径大于 30nm 的初级颗粒。这些发现表明,通过对 DND 的尺寸/氮含量进行调控,有望大规模生产基于氮相关缺陷的明亮、稳定发光的纳米金刚石光发射器。