Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy

Hyeongwoo Lee; Inki Kim; Chulho Park; Mingu Kang; Jinseong Choi; Kwang Yong Jeong; Jungho Mun; Yeseul Kim; Jeonghoon Park; Markus B. Raschke; Hong Gyu Park; Mun Seok Jeong; Junsuk Rho; Kyoung Duck Park

doi:10.1002/adfm.202102893

Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy

Hyeongwoo Lee, Inki Kim, Chulho Park, Mingu Kang, Jinseong Choi, Kwang Yong Jeong, Jungho Mun, Yeseul Kim, Jeonghoon Park, Markus B. Raschke, Hong Gyu Park, Mun Seok Jeong, Junsuk Rho, Kyoung Duck Park

Research output: Contribution to journal › Article › peer-review

20 Citations (Scopus)

Abstract

In atomically thin semiconductors, localized exciton (X_L) coupled to light provides a new class of optical sources for potential applications in quantum communication. However, in most studies, X_L photoluminescence (PL) from crystal defects has mainly been observed in cryogenic conditions because of their sub-wavelength emission region and low quantum yield at room temperature. Hybrid-modality of cavity-spectroscopy to induce and probe the X_L emissions at the nanoscale in atomically thin semiconductors is presented. By placing a WSe₂ monolayer on the two extremely sharp Au tips in a bowtie antenna with a radius of curvature of <1 nm, tensile strain of ≈0.3% is effectively induced in a <30 nm region to create robust X_L states. The Au tip then approaches the strained crystal region to enhance the X_L emissions and probe them with tip-enhanced photoluminescence (TEPL) spectroscopy at room temperature. Through this triple-sharp-tips cavity-spectroscopy with <15 nm spatial resolution, TEPL enhancement as high as ≈4.0 × 10⁴ by the Purcell effect is achieved, and peak energy shifts of X_L up to ≈40 meV are observed. This approach combining nano-cavity and -spectroscopy provides a systematic way to induce and probe the radiative emission of localized excitons in 2D semiconductors offering new strategies for dynamic quantum nano-optical devices.

Original language	English
Article number	2102893
Journal	Advanced Functional Materials
Volume	31
Issue number	33
DOIs	https://doi.org/10.1002/adfm.202102893
Publication status	Published - 2021 Aug 16
Externally published	Yes

Bibliographical note

Funding Information:
H.L. and I.K. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grants (2019K2A9A1A06099937 and 2020R1C1C1011301). J.R. acknowledges the NRF grants (2019R1A2C3003129, 2019M3A6B3030637, 2019R1A5A8080290) funded by the Ministry of Science and ICT (MSIT). I.K. acknowledges the NRF Sejong Science fellowship (NRF‐2021R1C1C2004291) funded by the MSIT of the Korean government. Y.K. acknowledges a fellowship from Hyundai Motor Chung Mong‐Koo Foundation and the POSTECHIAN fellowship from POSTECH. M.S.J. thanks the Creative Materials Discovery Program through NRF funded by the MSIT (2019M3D1A1078304). H.‐G.P. acknowledges the NRF grants (2021R1A2C3006781 and 2020R1A4A2002828) funded by the MSIT. M.B.R. acknowledges support from the National Science Foundation (NSF Grant CHE‐1709822). The authors thank D.S.L. and J.H.C. for the assistance of figure illustration.

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Keywords

cavity-spectroscopy
localized exciton
nano-cavity
plasmonic structures
purcell effect
tip-enhanced photoluminescence

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Condensed Matter Physics
Chemistry(all)
Materials Science(all)
Electrochemistry
Biomaterials

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10.1002/adfm.202102893

Cite this

Lee, H., Kim, I., Park, C., Kang, M., Choi, J., Jeong, K. Y., Mun, J., Kim, Y., Park, J., Raschke, M. B., Park, H. G., Jeong, M. S., Rho, J., & Park, K. D. (2021). Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy. Advanced Functional Materials, 31(33), Article 2102893. https://doi.org/10.1002/adfm.202102893

@article{f1d67529e9f544c7a3a4e9705da70bf5,

title = "Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy",

abstract = "In atomically thin semiconductors, localized exciton (XL) coupled to light provides a new class of optical sources for potential applications in quantum communication. However, in most studies, XL photoluminescence (PL) from crystal defects has mainly been observed in cryogenic conditions because of their sub-wavelength emission region and low quantum yield at room temperature. Hybrid-modality of cavity-spectroscopy to induce and probe the XL emissions at the nanoscale in atomically thin semiconductors is presented. By placing a WSe2 monolayer on the two extremely sharp Au tips in a bowtie antenna with a radius of curvature of <1 nm, tensile strain of ≈0.3% is effectively induced in a <30 nm region to create robust XL states. The Au tip then approaches the strained crystal region to enhance the XL emissions and probe them with tip-enhanced photoluminescence (TEPL) spectroscopy at room temperature. Through this triple-sharp-tips cavity-spectroscopy with <15 nm spatial resolution, TEPL enhancement as high as ≈4.0 × 104 by the Purcell effect is achieved, and peak energy shifts of XL up to ≈40 meV are observed. This approach combining nano-cavity and -spectroscopy provides a systematic way to induce and probe the radiative emission of localized excitons in 2D semiconductors offering new strategies for dynamic quantum nano-optical devices.",

keywords = "cavity-spectroscopy, localized exciton, nano-cavity, plasmonic structures, purcell effect, tip-enhanced photoluminescence",

author = "Hyeongwoo Lee and Inki Kim and Chulho Park and Mingu Kang and Jinseong Choi and Jeong, {Kwang Yong} and Jungho Mun and Yeseul Kim and Jeonghoon Park and Raschke, {Markus B.} and Park, {Hong Gyu} and Jeong, {Mun Seok} and Junsuk Rho and Park, {Kyoung Duck}",

note = "Funding Information: H.L. and I.K. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grants (2019K2A9A1A06099937 and 2020R1C1C1011301). J.R. acknowledges the NRF grants (2019R1A2C3003129, 2019M3A6B3030637, 2019R1A5A8080290) funded by the Ministry of Science and ICT (MSIT). I.K. acknowledges the NRF Sejong Science fellowship (NRF‐2021R1C1C2004291) funded by the MSIT of the Korean government. Y.K. acknowledges a fellowship from Hyundai Motor Chung Mong‐Koo Foundation and the POSTECHIAN fellowship from POSTECH. M.S.J. thanks the Creative Materials Discovery Program through NRF funded by the MSIT (2019M3D1A1078304). H.‐G.P. acknowledges the NRF grants (2021R1A2C3006781 and 2020R1A4A2002828) funded by the MSIT. M.B.R. acknowledges support from the National Science Foundation (NSF Grant CHE‐1709822). The authors thank D.S.L. and J.H.C. for the assistance of figure illustration. Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

month = aug,

day = "16",

doi = "10.1002/adfm.202102893",

language = "English",

volume = "31",

journal = "Advanced Functional Materials",

issn = "1616-301X",

publisher = "Wiley-VCH Verlag",

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T1 - Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy

AU - Lee, Hyeongwoo

AU - Kim, Inki

AU - Park, Chulho

AU - Kang, Mingu

AU - Choi, Jinseong

AU - Jeong, Kwang Yong

AU - Mun, Jungho

AU - Kim, Yeseul

AU - Park, Jeonghoon

AU - Raschke, Markus B.

AU - Park, Hong Gyu

AU - Jeong, Mun Seok

AU - Rho, Junsuk

AU - Park, Kyoung Duck

N1 - Funding Information: H.L. and I.K. contributed equally to this work. This work was supported by the National Research Foundation of Korea (NRF) grants (2019K2A9A1A06099937 and 2020R1C1C1011301). J.R. acknowledges the NRF grants (2019R1A2C3003129, 2019M3A6B3030637, 2019R1A5A8080290) funded by the Ministry of Science and ICT (MSIT). I.K. acknowledges the NRF Sejong Science fellowship (NRF‐2021R1C1C2004291) funded by the MSIT of the Korean government. Y.K. acknowledges a fellowship from Hyundai Motor Chung Mong‐Koo Foundation and the POSTECHIAN fellowship from POSTECH. M.S.J. thanks the Creative Materials Discovery Program through NRF funded by the MSIT (2019M3D1A1078304). H.‐G.P. acknowledges the NRF grants (2021R1A2C3006781 and 2020R1A4A2002828) funded by the MSIT. M.B.R. acknowledges support from the National Science Foundation (NSF Grant CHE‐1709822). The authors thank D.S.L. and J.H.C. for the assistance of figure illustration. Publisher Copyright: © 2021 Wiley-VCH GmbH

PY - 2021/8/16

Y1 - 2021/8/16

N2 - In atomically thin semiconductors, localized exciton (XL) coupled to light provides a new class of optical sources for potential applications in quantum communication. However, in most studies, XL photoluminescence (PL) from crystal defects has mainly been observed in cryogenic conditions because of their sub-wavelength emission region and low quantum yield at room temperature. Hybrid-modality of cavity-spectroscopy to induce and probe the XL emissions at the nanoscale in atomically thin semiconductors is presented. By placing a WSe2 monolayer on the two extremely sharp Au tips in a bowtie antenna with a radius of curvature of <1 nm, tensile strain of ≈0.3% is effectively induced in a <30 nm region to create robust XL states. The Au tip then approaches the strained crystal region to enhance the XL emissions and probe them with tip-enhanced photoluminescence (TEPL) spectroscopy at room temperature. Through this triple-sharp-tips cavity-spectroscopy with <15 nm spatial resolution, TEPL enhancement as high as ≈4.0 × 104 by the Purcell effect is achieved, and peak energy shifts of XL up to ≈40 meV are observed. This approach combining nano-cavity and -spectroscopy provides a systematic way to induce and probe the radiative emission of localized excitons in 2D semiconductors offering new strategies for dynamic quantum nano-optical devices.

AB - In atomically thin semiconductors, localized exciton (XL) coupled to light provides a new class of optical sources for potential applications in quantum communication. However, in most studies, XL photoluminescence (PL) from crystal defects has mainly been observed in cryogenic conditions because of their sub-wavelength emission region and low quantum yield at room temperature. Hybrid-modality of cavity-spectroscopy to induce and probe the XL emissions at the nanoscale in atomically thin semiconductors is presented. By placing a WSe2 monolayer on the two extremely sharp Au tips in a bowtie antenna with a radius of curvature of <1 nm, tensile strain of ≈0.3% is effectively induced in a <30 nm region to create robust XL states. The Au tip then approaches the strained crystal region to enhance the XL emissions and probe them with tip-enhanced photoluminescence (TEPL) spectroscopy at room temperature. Through this triple-sharp-tips cavity-spectroscopy with <15 nm spatial resolution, TEPL enhancement as high as ≈4.0 × 104 by the Purcell effect is achieved, and peak energy shifts of XL up to ≈40 meV are observed. This approach combining nano-cavity and -spectroscopy provides a systematic way to induce and probe the radiative emission of localized excitons in 2D semiconductors offering new strategies for dynamic quantum nano-optical devices.

KW - cavity-spectroscopy

KW - localized exciton

KW - nano-cavity

KW - plasmonic structures

KW - purcell effect

KW - tip-enhanced photoluminescence

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U2 - 10.1002/adfm.202102893

DO - 10.1002/adfm.202102893

M3 - Article

AN - SCOPUS:85108188395

SN - 1616-301X

VL - 31

JO - Advanced Functional Materials

JF - Advanced Functional Materials

IS - 33

M1 - 2102893

ER -

Inducing and Probing Localized Excitons in Atomically Thin Semiconductors via Tip-Enhanced Cavity-Spectroscopy

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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