Correlated fluorescence blinking in two-dimensional semiconductor heterostructures

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2016
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Xu, Weigao
Liu, Weiwei
Zhao, Weijie
Lu, Xin
Diederichs, Carole
Gao, Weibo
Xiong, Qihua
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Nature. 2016, 541(7635), pp. 62-67. ISSN 0028-0836. eISSN 1476-4687. Available under: doi: 10.1038/nature20601
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'Blinking', or 'fluorescence intermittency', refers to a random switching between 'ON' (bright) and 'OFF' (dark) states of an emitter; it has been studied widely in zero-dimensional quantum dots and molecules, and scarcely in one-dimensional systems. A generally accepted mechanism for blinking in quantum dots involves random switching between neutral and charged states (or is accompanied by fluctuations in charge-carrier traps), which substantially alters the dynamics of radiative and non-radiative decay. Here, we uncover a new type of blinking effect in vertically stacked, two-dimensional semiconductor heterostructures, which consist of two distinct monolayers of transition metal dichalcogenides (TMDs) that are weakly coupled by van der Waals forces. Unlike zero-dimensional or one-dimensional systems, two-dimensional TMD heterostructures show a correlated blinking effect, comprising randomly switching bright, neutral and dark states. Fluorescence cross-correlation spectroscopy analyses show that a bright state occurring in one monolayer will simultaneously lead to a dark state in the other monolayer, owing to an intermittent interlayer carrier-transfer process. Our findings suggest that bilayer van der Waals heterostructures provide unique platforms for the study of charge-transfer dynamics and non-equilibrium-state physics, and could see application as correlated light emitters in quantum technology.

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ISO 690XU, Weigao, Weiwei LIU, Jan SCHMIDT, Weijie ZHAO, Xin LU, Timo RAAB, Carole DIEDERICHS, Weibo GAO, Denis V. SELETSKIY, Qihua XIONG, 2016. Correlated fluorescence blinking in two-dimensional semiconductor heterostructures. In: Nature. 2016, 541(7635), pp. 62-67. ISSN 0028-0836. eISSN 1476-4687. Available under: doi: 10.1038/nature20601
BibTex
@article{Xu2016Corre-38709,
  year={2016},
  doi={10.1038/nature20601},
  title={Correlated fluorescence blinking in two-dimensional semiconductor heterostructures},
  number={7635},
  volume={541},
  issn={0028-0836},
  journal={Nature},
  pages={62--67},
  author={Xu, Weigao and Liu, Weiwei and Schmidt, Jan and Zhao, Weijie and Lu, Xin and Raab, Timo and Diederichs, Carole and Gao, Weibo and Seletskiy, Denis V. and Xiong, Qihua}
}
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