All-optical control of high-purity trions in nanoscale waveguide

Creators: Lee, Hyeongwoo; Koo, Yeonjeong; Kumar, Shailabh; Jeong, Yunjo; Heo, Dong Gwon; Choi, Soo Ho; Joo, Huitae; Kang, Mingu; Siddique, Radwanul Hasan; Kim, Ki Kang; Lee, Hong Seok; An, Sangmin; Choo, Hyuck; Park, Kyoung-Duck

Abstract

The generation of high-purity localized trions, dynamic exciton–trion interconversion, and their spatial modulation in two-dimensional (2D) semiconductors are building blocks for the realization of trion-based optoelectronic devices. Here, we present a method for the all-optical control of the exciton-to-trion conversion process and its spatial distributions in a MoS₂ monolayer. We induce a nanoscale strain gradient in a 2D crystal transferred on a lateral metal–insulator–metal (MIM) waveguide and exploit propagating surface plasmon polaritons (SPPs) to localize hot electrons. These significantly increase the electrons and efficiently funnel excitons in the lateral MIM waveguide, facilitating complete exciton-to-trion conversion even at ambient conditions. Additionally, we modulate the SPP mode using adaptive wavefront shaping, enabling all-optical control of the exciton-to-trion conversion rate and trion distribution in a reversible manner. Our work provides a platform for harnessing excitonic quasiparticles efficiently in the form of trions at ambient conditions, enabling high-efficiency photoconversion.

Additional Information

© The Author(s) 2023. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. This work was supported by the projects of 2020R1C1C101130113, (2022)ERIC_03_3, IITP-2022-RS-2022-00164799, ETRI_21YB2100, and 2021R1A6A1A10042944. We gratefully acknowledge the critical support and infrastructure provided for the fabrication of the waveguide by the Kavli Nanoscience Institute at Caltech and Samsung Advanced Institute of Technology. S.A. and H.S.L. acknowledge National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (2022R1A4A1033358). H.S.L. acknowledges 2021R1A2C1003074. S.H.C. and K.K.K. acknowledge the support by the Institute for Basic Science (IBS-R001-D1) and Advanced Facility Center for Quantum Technology. K.K.K. acknowledges the Basic Research Program (2020R1A4A3079710, 2022R1A2C2091475) and the Next-generation Intelligence Semiconductor Program (2022M3F3A2A01072215) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT. Contributions. H.L. and K.-D.P. conceived the experiments. H.L. performed PL spectroscopy and control experiments. H.L. and Y.K. performed the adaptive wavefront shaping experiments. S.K., R.H.S., and H.C. designed and fabricated the nanogap-based waveguide devices. H.L. and H.J. performed the theoretical calculations and modeling by analyzing the exciton-diffusion model. Y.J. and S.A. obtained the KPFM images. D.G.H. and H.S.L. performed the time-resolved PL measurements. S.H.C. and K.K.K. prepared and transferred MoS₂ ML onto the nanogap-based waveguide device. H.L., Y.K., M.K., and K.-D.P. analyzed the data, and all authors discussed the results. H.L. and K.-D.P. wrote the manuscript with contributions from all authors. K.-D.P. supervised the project. Data availability. The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. The authors declare no competing interests.

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