Chen Feiyang, Ju Meng, Kuang Xiaoyu, Yeung Yauyuen
Institute of Atomic and Molecular Physics, Sichuan University , Chengdu 610065 , China.
Department of Science and Environmental Studies , The Education University of Hong Kong , 10 Lo Ping Road , Tai Po , NT, Hong Kong China.
Inorg Chem. 2018 Apr 16;57(8):4563-4570. doi: 10.1021/acs.inorgchem.8b00316. Epub 2018 Mar 27.
Due to its unusual optical properties, neodymium ion (Nd)-doped bismuth silicate (BiSiO, BSO) is widely used for its excellent medium laser amplification in physics, chemistry, biomedicine, and other research fields. Although the spectral transitions and luminescent mechanisms of Nd-doped BSO have been investigated experimentally, theoretical research is severely limited due to the lack of detailed information about the microstructure and the doping site of Nd-doped BSO, as well as the electric and magnetic dipole transition mechanisms. Herein, we systematically study the microstructure and doping site of Nd-doped BSO using an unbiased CALYPSO structure search method in conjunction with first-principles calculations. The result indicates that the Nd ion impurity occupies the host Bi ion site with trigonal symmetry, forming a unique semiconducting phase. Based on our newly developed WEPMD method, the electric dipole and magnetic dipole transition lines, including a large number of absorption and emission lines, in the region of visible and near-infrared spectra of Nd-doped BSO are calculated. It is found that the G → I, H → I, and F → I channels are promising laser actions of Nd-doped BSO. These findings indicate that Nd-doped BSO crystals can serve as a promising multifunctional material for optical laser devices.
由于其独特的光学性质，掺钕离子（Nd）的硅酸铋（BiSiO，BSO）因其在物理、化学、生物医学等研究领域中优异的激光放大介质性能而被广泛应用。尽管已通过实验研究了掺Nd的BSO的光谱跃迁和发光机制，但由于缺乏关于掺Nd的BSO的微观结构和掺杂位点以及电偶极和磁偶极跃迁机制的详细信息，理论研究受到严重限制。在此，我们使用无偏CALYPSO结构搜索方法结合第一性原理计算，系统地研究了掺Nd的BSO的微观结构和掺杂位点。结果表明，Nd离子杂质占据具有三角对称性的主体Bi离子位点，形成独特的半导体相。基于我们新开发的WEPMD方法，计算了掺Nd的BSO在可见和近红外光谱区域的电偶极和磁偶极跃迁线，包括大量的吸收和发射线。发现G→I、H→I和F→I通道是掺Nd的BSO有前景的激光作用通道。这些发现表明，掺Nd的BSO晶体可作为一种有前景的用于光学激光器件的多功能材料。
