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Published May 7, 2024 | in press
Journal Article Open

Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS₂ Interfaces

Abstract

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr-ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge-transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr-ESFG especially sensitive to the trion formation dynamics. The presence of charge-transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers the potential for transferring unique electronic attributes of TMD to the molecular layers.

 

Copyright and License

© 2024 Wiley-VCH.

Acknowledgement

The authors thank Dr. Haochuan Mao, Dr. Wenfan Chen and Dr.Chun-Chieh Yu for their valuable discussion in the manuscript.The authors thank Alyssa F. Cavazos for her help in preparing themanuscript. Y.J., N.M., C.W. and W. X., and S.K.C. are supportedby a collaborative ground from Department of Energy DE-FOA-0002449. K.L., H.Z. and Z.L. and S.L. are supported by NSFunder the grant CHE-2303936 awarded to S.L. Z.S. wassupported by ERC-CZ program (project LL2101) from Ministry ofEducation Youth and Sports (MEYS) and by the project AdvancedFunctional Nanorobots (reg. No.CZ.02.1.01/0.0/0.0/15_003/0000444 financed by the EFRR). J.P. J.S. and C.P.K. are supported by NSF under the grant CHE-1853908 and CHE-2153757 awarded to C.P.K.

Data Availability

https://onlinelibrary.wiley.com/action/downloadSupplement?doi=10.1002%2Fanie.202405123&file=anie202405123-s1-Supporting_information.pdf

Files

Angew Chem Int Ed - 2024 - Jing - Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS2.pdf

Additional details

Created:
May 31, 2024
Modified:
May 31, 2024