Wragg Joseph, Bolzonello Luca, Donati Ludovica, Soundarapandian Karuppasamy Pandian, Bertini Riccardo, Tongay Seth Ariel, Watanabe Kenji, Taniguchi Takashi, Koppens Frank H L, van Hulst Niek F
ICFO - Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, Castelldefels, Barcelona 08860, Spain.
LENS, European Laboratory for Non-Linear Spectroscopy, 50019 Sesto Fiorentino FI, Italy.
Nano Lett. 2025 May 14;25(19):7658-7664. doi: 10.1021/acs.nanolett.4c06349. Epub 2025 Apr 4.
While it has long been accepted that the role of momentum dark excitons in the photoresponse of transition metal dichalcogenides (TMDs) is critical, their weak optical signature inhibits their study through conventional means. Here we expose the room-temperature contributions of both bright and dark excitons to the behavior of a TMD, WSe, from monolayer to multilayer to bulk. To do so, we present dual action spectroscopy, a photocurrent- and luminescence-detected Fourier-transform excitation spectroscopy scheme, to microscopically map the energy landscape of WSe. While bright excitons naturally dominate the luminescence response of the material, dark excitons dominate the current response. Notably, the dark exciton is more accessible than the ground state , while current maps reveal a disparity in the diffusivity of the two states. This work provides the basis for a new, current-detected approach to study the dynamics of dark exciton states across different materials.
虽然长期以来人们一直认为动量暗激子在过渡金属二硫属化物(TMD)的光响应中起着关键作用,但它们微弱的光学特征阻碍了通过传统方法对其进行研究。在此,我们揭示了从单层到多层再到体相的TMD材料WSe中,亮激子和暗激子在室温下对其行为的贡献。为此,我们提出了双作用光谱法,这是一种光电流和发光检测的傅里叶变换激发光谱方案,用于微观绘制WSe的能量分布图。虽然亮激子自然主导材料的发光响应,但暗激子主导电流响应。值得注意的是,暗激子比基态更容易被激发,而电流分布图显示这两种状态的扩散率存在差异。这项工作为一种新的、基于电流检测的方法提供了基础,用于研究不同材料中暗激子态的动力学。