Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride
Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride
复制标题
DOI：
10.1103/prxquantum.3.030331
复制
发表时间：
2022-01
期刊：
影响因子：
9.7
通讯作者：
Raj N. Patel;David A. Hopper;Jordan A. Gusdorff;M. Turiansky;Tzu-Yung Huang;Rebecca E. K. Fishman;Benjamin Porat;C. G. Van de Walle;L. Bassett
中科院分区：
文献类型：
--
作者：
Raj N. Patel;David A. Hopper;Jordan A. Gusdorff;M. Turiansky;Tzu-Yung Huang;Rebecca E. K. Fishman;Benjamin Porat;C. G. Van de Walle;L. Bassett
六方氮化硼是一种在室温下具有可见波长量子发射体的范德华材料。然而，缺乏对量子发射体电子结构的实验鉴定，并且它们的电荷和自旋性质的关键细节仍然未知。本文利用光子发射相关光谱研究了六方氮化硼中量子发射体的光学动力学。一些量子发射体表现出理想的单光子发射，具有噪声限制的光子反束，$g^{(2)}(0)=0$。光致发光发射线形状与单个振动跃迁一致。然而，偏振分辨激发和发射表明了多重光学跃迁的作用，光子发射相关光谱揭示了通过多个电子激发态与激发和弛豫相关的复杂光学动力学。我们将实验结果与定量光学动力学模拟进行了比较，建立了与观测结果一致的电子结构模型，并在从头算理论计算的背景下讨论了结果。
Hexagonal boron nitride is a van der Waals material that hosts visible-wavelength quantum emitters at room temperature. However, experimental identification of the quantum emitters' electronic structure is lacking, and key details of their charge and spin properties remain unknown. Here, we probe the optical dynamics of quantum emitters in hexagonal boron nitride using photon emission correlation spectroscopy. Several quantum emitters exhibit ideal single-photon emission with noise-limited photon antibunching, $g^{(2)}(0)=0$. The photoluminescence emission lineshapes are consistent with individual vibronic transitions. However, polarization-resolved excitation and emission suggests the role of multiple optical transitions, and photon emission correlation spectroscopy reveals complicated optical dynamics associated with excitation and relaxation through multiple electronic excited states. We compare the experimental results to quantitative optical dynamics simulations, develop electronic structure models that are consistent with the observations, and discuss the results in the context of ab initio theoretical calculations.