Vogl Tobias, Doherty Marcus W, Buchler Ben C, Lu Yuerui, Lam Ping Koy
Centre for Quantum Computation and Communication Technology, Department of Quantum Science, Research School of Physics and Engineering, The Australian National University, Acton ACT 2601, Australia.
Nanoscale. 2019 Aug 1;11(30):14362-14371. doi: 10.1039/c9nr04269e.
The recent discovery of single-photon emitting defects hosted by the two-dimensional wide band gap semiconductor hexagonal boron nitride (hBN) has inspired a great number of experiments. Key characteristics of these quantum emitters are their capability to operate at room temperature with a high luminosity. In spite of large theoretical and experimental research efforts, the exact nature of the emission remains unresolved. In this work we utilize layer-by-layer etching of multilayer hBN to localize the quantum emitters with atomic precision. Our results suggest the position of the emitters correlates with the fabrication method: emitters formed under plasma treatment are always in close proximity to the crystal surface, while emitters created under electron irradiation are distributed randomly throughout the entire crystal. This disparity could be traced back to the lower kinetic energy of the ions in the plasma compared to the kinetic energy of the electrons in the particle accelerator. The emitter distance to the surface also correlates with the excited state lifetime: near-surface emitters have a shorter one compared to emitters deep within the crystal. Finite-difference time-domain and density functional theory simulations show that optical and electronic effects are not responsible for this difference, indicating effects such as coupling to surface defects or phonons might cause the reduced lifetime. Our results pave a way toward identification of the defect, as well as engineering the emitter properties.
二维宽带隙半导体六方氮化硼(hBN)中存在的单光子发射缺陷的最新发现激发了大量实验。这些量子发射器的关键特性是它们能够在室温下以高发光度运行。尽管进行了大量的理论和实验研究工作,但发射的确切性质仍未得到解决。在这项工作中,我们利用多层hBN的逐层蚀刻以原子精度定位量子发射器。我们的结果表明,发射器的位置与制造方法相关:在等离子体处理下形成的发射器总是靠近晶体表面,而在电子辐照下产生的发射器则随机分布在整个晶体中。这种差异可以追溯到与粒子加速器中电子的动能相比,等离子体中离子的动能较低。发射器到表面的距离也与激发态寿命相关:与晶体深处的发射器相比,近表面发射器的激发态寿命更短。时域有限差分法和密度泛函理论模拟表明,光学和电子效应并非造成这种差异的原因,这表明诸如与表面缺陷或声子耦合等效应可能导致寿命缩短。我们的结果为识别缺陷以及设计发射器特性铺平了道路。