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Effects of Direct Solvent-Quantum Dot Interaction on the Optical Properties of Colloidal Monolayer WS2 Quantum Dots

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Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States
Department of Materials Science and Engineering, Texas A&M University, College Station, Texas 77843, United States
§ Center for Nanomedicine, Institute for Basic Science (IBS), Seoul 03722, Republic of Korea
Yonsei-IBS Institute, Yonsei University, Seoul 03722, Republic of Korea
Department of Chemistry, Yonsei University, Seoul 03722, Republic of Korea
*E-mail: [email protected]. Tel: +1-979-458-2990.
Cite this: Nano Lett. 2017, 17, 12, 7471–7477
Publication Date (Web):October 27, 2017
https://doi.org/10.1021/acs.nanolett.7b03381
Copyright © 2017 American Chemical Society

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    Abstract

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    Because of the absence of native dangling bonds on the surface of the layered transition metal dichalcogenides (TMDCs), the surface of colloidal quantum dots (QDs) of TMDCs is exposed directly to the solvent environment. Therefore, the optical and electronic properties of TMDCS QDs are expected to have stronger influence from the solvent than usual surface-passivated QDs due to more direct solvent-QD interaction. Study of such solvent effect has been difficult in colloidal QDs of TMDC due to the large spectroscopic heterogeneity resulting from the heterogeneity of the lateral size or (and) thickness in ensemble. Here, we developed a new synthesis procedure producing the highly uniform colloidal monolayer WS2 QDs exhibiting well-defined photoluminescence (PL) spectrum free from ensemble heterogeneity. Using these newly synthesized monolayer WS2 QDs, we observed the strong influence of the aromatic solvents on the PL energy and intensity of monolayer WS2 QD beyond the simple dielectric screening effect, which is considered to result from the direct electronic interaction between the valence band of the QDs and molecular orbital of the solvent. We also observed the large effect of stacking/separation equilibrium on the PL spectrum dictated by the balance between inter QD and QD-solvent interactions. The new capability to probe the effect of the solvent molecules on the optical properties of colloidal TMDC QDs will be valuable for their applications in various liquid surrounding environments.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.7b03381.

    • Synthesis methods, STM measurement, NMR measurement, optical characterization, band edge calculation, additional PL spectra of WS2 QDs and MoS2 QDs in various solvents, FTIR spectra and NMR spectra of WS2 QDs (PDF)

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