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.
Bibliographical noteFunding Information:
This work was supported by the Robert A. Welch Foundation (A-1639 to H.J.) and the National Science Foundation (DMR-1404457 to D.H.S. and CHE-1611119 to J.D.B.). We also acknowledge the support from Institute for Basic Science (IBS-R026-D1), the Asian Office of Aerospace Research and Development (FA2386-14-1-0014), S. J. Yoo for TEM analyses [KBSI-HVEM (JEM-ARM1300S)] and C. Hilty and J. Kim for NMR analyses (Bruker 400 MHz NMR).
© 2017 American Chemical Society.
All Science Journal Classification (ASJC) codes
- Materials Science(all)
- Condensed Matter Physics
- Mechanical Engineering