Kim Bumseop, Park Noejung, Kim Jeongwoo
Department of Physics, Ulsan National Institute of Science and Technology, Ulsan, 689-798, Korea.
Department of Physics, Incheon National University, Incheon, 406-772, Korea.
Nat Commun. 2022 Jun 10;13(1):3237. doi: 10.1038/s41467-022-31018-8.
The intrinsic light-matter characteristics of transition-metal dichalcogenides have not only been of great scientific interest but have also provided novel opportunities for the development of advanced optoelectronic devices. Among the family of transition-metal dichalcogenide structures, the one-dimensional nanotube is particularly attractive because it produces a spontaneous photocurrent that is prohibited in its higher-dimensional counterparts. Here, we show that WS nanotubes exhibit a giant shift current near the infrared region, amounting to four times the previously reported values in the higher frequency range. The wall-to-wall charge shift constitutes a key advantage of the one-dimensional nanotube geometry, and we consider a Janus-type heteroatomic configuration that can maximize this interwall effect. To assess the nonlinear effect of a strong field and the nonadiabatic effect of atomic motion, we carried out direct real-time integration of the photoinduced current using time-dependent density functional theory. Our findings provide a solid basis for a complete quantum mechanical understanding of the unique light-matter interaction hidden in the geometric characteristics of the reduced dimension.
过渡金属二硫属化物的本征光与物质特性不仅具有重大的科学研究价值,还为先进光电器件的发展提供了新机遇。在过渡金属二硫属化物结构家族中,一维纳米管尤其引人注目,因为它能产生自发光电流,而其高维同类结构中则不存在这种现象。在此,我们表明WS纳米管在红外区域附近展现出巨大的位移电流,达到此前在高频范围所报道值的四倍。壁间电荷转移是一维纳米管几何结构的关键优势,我们考虑一种能使这种壁间效应最大化的Janus型杂原子构型。为评估强场的非线性效应和原子运动的非绝热效应,我们利用含时密度泛函理论对光致电流进行了直接实时积分。我们的研究结果为从量子力学角度全面理解隐藏在低维几何特征中的独特光与物质相互作用奠定了坚实基础。