Zhang Xiao-Xiao, Cao Ting, Lu Zhengguang, Lin Yu-Chuan, Zhang Fan, Wang Ying, Li Zhiqiang, Hone James C, Robinson Joshua A, Smirnov Dmitry, Louie Steven G, Heinz Tony F
Department of Physics, Columbia University, New York, New York 10027, USA.
Department of Applied Physics, Stanford University, Stanford, California 94305, USA.
Nat Nanotechnol. 2017 Sep;12(9):883-888. doi: 10.1038/nnano.2017.105. Epub 2017 Jun 26.
Monolayer transition metal dichalcogenide crystals, as direct-gap materials with strong light-matter interactions, have attracted much recent attention. Because of their spin-polarized valence bands and a predicted spin splitting at the conduction band edges, the lowest-lying excitons in WX (X = S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark excitons. Here, we show how an in-plane magnetic field can brighten the dark excitons in monolayer WSe and permit their properties to be observed experimentally. Precise energy levels for both the neutral and charged dark excitons are obtained and compared with ab initio calculations using the GW-BSE approach. As a result of their spin configuration, the brightened dark excitons exhibit much-increased emission and valley lifetimes. These studies directly probe the excitonic spin manifold and reveal the fine spin-splitting at the conduction band edges.
单层过渡金属二硫属化物晶体作为具有强光-物质相互作用的直接带隙材料,最近备受关注。由于其自旋极化价带以及在导带边缘预测的自旋分裂,预计WX(X = S,Se)中能量最低的激子是自旋禁戒且光学暗的。然而,迄今为止,尚未对这些暗激子进行直接的实验探测。在此,我们展示了面内磁场如何使单层WSe中的暗激子变亮,并使其性质能够通过实验观测到。我们获得了中性和带电暗激子的精确能级,并与使用GW-BSE方法的从头算计算结果进行比较。由于其自旋构型,变亮的暗激子表现出大大增加的发射和谷寿命。这些研究直接探测了激子自旋多重态,并揭示了导带边缘精细的自旋分裂。