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arXiv 2102.10758cond-mat.mes-hall
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范德瓦尔斯反铁磁绝缘体中的强各向异性激子和多声子束缚态

Highly Anisotropic Excitons and Multiple Phonon Bound States in a Van der Waals Antiferromagnetic Insulator

Kyle Hwangbo, Qi Zhang, Qianni Jiang, Yong Wang, Jordan Fonseca, Chong Wang, Geoffrey M. Diederich, Daniel R. Gamelin, Di Xiao, Jiun-Haw Chu, Wang Yao, Xiaodong Xu

摘要:

二维半导体系统,如量子阱和过渡金属二硫属化物,是研究低维光-物质相互作用的基础。到目前为止,由于缺乏合适的材料平台,在具有内禀磁有序的二维半导体中的元光激发,即激子的研究仍然是一个挑战。在这里,我们报告的观察激子耦合到锯齿形反铁磁顺序在层状反铁磁绝缘体NiPS 3使用光致发光(PL)和光学反射光谱。激子在PL谱中具有窄至~350 μ eV的线宽,且具有接近1的线性偏振。随着样品的厚度从五层减少到双层,PL强度被大大抑制,并最终在单层中消失,这与双层和单层的计算带隙高度间接一致。我们观察到强的线性二向色性(LD)在一个广泛的光谱范围内,共享相同的光学各向异性轴,被锁定到锯齿形方向,作为激子PL。激子PL中的LD和线偏振度都随着温度的升高而降低,并且在高于Neel温度时变得可以忽略不计。这些观测结果表明,这两个光学量是对称破缺磁序参量的探针。此外,在激子PL附近的能量的LD光谱中观察到尖锐的共振。在其高能侧存在十多个激子-A1 g声子束缚态,这可能是由于强的电子-晶格相互作用对配体-金属电荷转移能量的强烈调制.我们的工作建立了NiPS 3作为一个新的二维平台,探索磁激子物理与强相关性,以及构建块的二维异质结构的工程物理现象与时间反演对称性破缺。

英文摘要:

Two-dimensional semiconducting systems, such as quantum wells and transition metal dichalcogenides, are the foundations to investigate low dimensional light-matter interactions. To date, the study of elementary photoexcitation, namely the exciton, in 2D semiconductors with intrinsic magnetic order remains a challenge due to the lack of suitable material platforms. Here, we report an observation of excitons coupled to zigzag antiferromagnetic order in the layered antiferromagnetic insulator NiPS3 using both photoluminescence (PL) and optical reflection spectroscopy. The exciton exhibits a linewidth as narrow as ~350 ueV with near unity linear polarization in the PL spectrum. As the thicknesses of samples is reduced from five layers to bilayers, the PL intensity is drastically suppressed and eventually vanishes in monolayers, consistent with the calculated bandgap being highly indirect for both bilayer and monolayer. We observed strong linear dichroism (LD) over a broad spectra range, which shares the same optical anisotropy axis, being locked to the zigzag direction, as the exciton PL. Both LD and the degree of linear polarization in the exciton PL decrease as the temperature increases and become negligible above the Neel temperature. These observations suggest both optical quantities are probes of the symmetry breaking magnetic order parameter. In addition, a sharp resonance in the LD spectrum is observed with an energy near the exciton PL. There exist over ten exciton-A1g phonon bound states on its high energy side, which likely result from the strong modulation of the ligand-to-metal charge transfer energy by strong electron-lattice interactions. Our work establishes NiPS3 as a new 2D platform for exploring magneto-exciton physics with strong correlations, as well as a building block for 2D heterostructures for engineering physical phenomena with time reversal symmetry breaking.

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