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<p>When disassembled into monolayers from their bulk crystals, two-dimensional (2D) transition metal dichalcogenides (TMDCs) exhibit exotic optical properties dominated by strong excitonic effects. Reassembling 2D TMDC layers to build bulk excitonic crystals can significantly boost their optical performance and introduce emerging functionalities toward optoelectronic and valleytronic applications. However, maintaining&#xa0;or manipulating 2D excitonic properties in bulk structures or superlattices is challenging. Herein, we developed a method to precisely construct <i>m</i>∙2<sup><i>N</i></sup>-layer artificial excitonic&#xa0;crystals with only a number <i>N</i> of stacking operations (m denotes the layer number of the initial material unit), referred to as the “2^N method”. We successfully fabricated a millimeter-scale weakly coupled 16-layer MoS<sub>2</sub> single crystal with zero interlayer twist angle, which retains monolayer-like exciton properties and exhibits remarkable enhancements up to 643% and 646% in their absorption and photoluminescence (PL) features, respectively. Moreover, we created a WSe<sub>2</sub>/(MoS<sub>2</sub>/WSe<sub>2</sub>)<sub>3</sub>/MoS<sub>2</sub> superlattice starting from monolayer WSe<sub>2</sub> and MoS<sub>2</sub>, which demonstrated an intensity increase of up to 400% in quadrupolar interlayer exciton (IX) emission as compared to dipolar IXs in its bilayer counterpart. Our work shows a promising approach for the design and bottom-up fabrication of excitonic crystals, promoting the exploration of excitonic physics in complex van der Waals (vdW) structures and their applications in optoelectronic devices.</p>

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Designable excitonic effects in van der Waals artificial crystals with exponentially growing thickness

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月19日

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  • Qianlu Sun,
  • Jiamin Lin,
  • Pedro Ludwig Hernandez-Martine,
  • Taotao Li,
  • Yantong Li,
  • Li Li,
  • Changjin Wan,
  • Nannan Mao,
  • Huakang Yu,
  • Peng Wang,
  • Hilmi Volkan Demir,
  • Zehua Hu,
  • Rui Su,
  • Weigao Xu

摘要

When disassembled into monolayers from their bulk crystals, two-dimensional (2D) transition metal dichalcogenides (TMDCs) exhibit exotic optical properties dominated by strong excitonic effects. Reassembling 2D TMDC layers to build bulk excitonic crystals can significantly boost their optical performance and introduce emerging functionalities toward optoelectronic and valleytronic applications. However, maintaining or manipulating 2D excitonic properties in bulk structures or superlattices is challenging. Herein, we developed a method to precisely construct m∙2N-layer artificial excitonic crystals with only a number N of stacking operations (m denotes the layer number of the initial material unit), referred to as the “2^N method”. We successfully fabricated a millimeter-scale weakly coupled 16-layer MoS2 single crystal with zero interlayer twist angle, which retains monolayer-like exciton properties and exhibits remarkable enhancements up to 643% and 646% in their absorption and photoluminescence (PL) features, respectively. Moreover, we created a WSe2/(MoS2/WSe2)3/MoS2 superlattice starting from monolayer WSe2 and MoS2, which demonstrated an intensity increase of up to 400% in quadrupolar interlayer exciton (IX) emission as compared to dipolar IXs in its bilayer counterpart. Our work shows a promising approach for the design and bottom-up fabrication of excitonic crystals, promoting the exploration of excitonic physics in complex van der Waals (vdW) structures and their applications in optoelectronic devices.