Kim Younghee, Goupalov Serguei V, Weight Braden M, Gifford Brendan J, He Xiaowei, Saha Avishek, Kim Mijin, Ao Geyou, Wang YuHuang, Zheng Ming, Tretiak Sergei, Doorn Stephen K, Htoon Han
Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.
Department of Physics, Jackson State University, Jackson, Mississippi 39217, United States.
ACS Nano. 2020 Mar 24;14(3):3451-3460. doi: 10.1021/acsnano.9b09548. Epub 2020 Feb 19.
Organic color-center quantum defects in semiconducting carbon nanotube hosts are rapidly emerging as promising candidates for solid-state quantum information technologies. However, it is unclear whether these defect color-centers could support the spin or pseudospin-dependent excitonic fine structure required for spin manipulation and readout. Here we conducted magneto-photoluminescence spectroscopy on individual organic color-centers and observed the emergence of fine structure states under an 8.5 T magnetic field applied parallel to the nanotube axis. One to five fine structure states emerge depending on the chirality of the nanotube host, nature of chemical functional group, and chemical binding configuration, presenting an exciting opportunity toward developing chemical control of magnetic brightening. We attribute these hidden excitonic fine structure states to field-induced mixing of singlet excitons trapped at sp defects and delocalized band-edge triplet excitons. These findings provide opportunities for using organic color-centers for spintronics, spin-based quantum computing, and quantum sensing.
半导体碳纳米管主体中的有机色心量子缺陷正迅速成为固态量子信息技术的有前途的候选者。然而，尚不清楚这些缺陷色心是否能够支持自旋操纵和读出所需的自旋或赝自旋相关的激子精细结构。在这里，我们对单个有机色心进行了磁光致发光光谱研究，并观察到在平行于纳米管轴施加的8.5 T磁场下出现了精细结构态。根据纳米管主体的手性、化学官能团的性质和化学结合构型，会出现一到五个精细结构态，这为开发磁增强的化学控制提供了令人兴奋的机会。我们将这些隐藏的激子精细结构态归因于捕获在sp缺陷处的单重态激子与离域的带边三重态激子的场致混合。这些发现为将有机色心用于自旋电子学、基于自旋的量子计算和量子传感提供了机会。
