Chemomechanical modification of quantum emission in monolayer WSe2

M. Iqbal Bakti Utama, Hongfei Zeng, Tumpa Sadhukhan, Anushka Dasgupta, S. Carin Gavin, Riddhi Ananth, Dmitry Lebedev, Wei Wang, Jia-Shiang Chen, Kenji Watanabe, Takashi Taniguchi, Tobin J. Marks, Xuedan Ma, Emily A. Weiss, George C. Schatz (), Nathaniel P. Stern () and Mark C. Hersam ()
Additional contact information
M. Iqbal Bakti Utama: Northwestern University
Hongfei Zeng: Northwestern University
Tumpa Sadhukhan: Northwestern University
Anushka Dasgupta: Northwestern University
S. Carin Gavin: Northwestern University
Riddhi Ananth: Northwestern University
Dmitry Lebedev: Northwestern University
Wei Wang: Argonne National Laboratory
Jia-Shiang Chen: Argonne National Laboratory
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Tobin J. Marks: Northwestern University
Xuedan Ma: Argonne National Laboratory
Emily A. Weiss: Northwestern University
George C. Schatz: Northwestern University
Nathaniel P. Stern: Northwestern University
Mark C. Hersam: Northwestern University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Two-dimensional (2D) materials have attracted attention for quantum information science due to their ability to host single-photon emitters (SPEs). Although the properties of atomically thin materials are highly sensitive to surface modification, chemical functionalization remains unexplored in the design and control of 2D material SPEs. Here, we report a chemomechanical approach to modify SPEs in monolayer WSe2 through the synergistic combination of localized mechanical strain and noncovalent surface functionalization with aryl diazonium chemistry. Following the deposition of an aryl oligomer adlayer, the spectrally complex defect-related emission of strained monolayer WSe2 is simplified into spectrally isolated SPEs with high single-photon purity. Density functional theory calculations reveal energetic alignment between WSe2 defect states and adsorbed aryl oligomer energy levels, thus providing insight into the observed chemomechanically modified quantum emission. By revealing conditions under which chemical functionalization tunes SPEs, this work broadens the parameter space for controlling quantum emission in 2D materials.

Date: 2023
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DOI: 10.1038/s41467-023-37892-0

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