Generating ultrabroadband deep-UV radiation and sub-10 nm gap by hybrid-morphology gold antennas

Liping Shi, Jose R. C. Andrade, Ayhan Tajalli, Jiao Geng, Jue-min Yi, Torsten Heidenblut, Frans Segerink, Ihar Babushkin, Maria Kholodtsova, Hamed Merdji, Bert Bastiaens, Uwe Morgner, Milutin Kovacev

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Abstract

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

Original languageEnglish
Pages (from-to)4779-4786
Number of pages8
JournalNano letters
Volume19
Issue number7
DOIs
Publication statusPublished - 10 Jul 2019

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Ultraviolet radiation
Gold
antennas
Antennas
gold
Lasers
Aluminum Oxide
radiation
harmonics
Sapphire
lasers
resonant frequencies
Natural frequencies
sapphire
apertures
Magnetic fields
Wavelength
nanofabrication
Laser ablation
Nanotechnology

Keywords

  • Nonlinear plasmonics
  • broadband deep-ultraviolet
  • laser ablation
  • nanoscale gaps
  • near-field mapping

Cite this

Shi, L., Andrade, J. R. C., Tajalli, A., Geng, J., Yi, J., Heidenblut, T., ... Kovacev, M. (2019). Generating ultrabroadband deep-UV radiation and sub-10 nm gap by hybrid-morphology gold antennas. Nano letters, 19(7), 4779-4786. https://doi.org/10.1021/acs.nanolett.9b02100
Shi, Liping ; Andrade, Jose R. C. ; Tajalli, Ayhan ; Geng, Jiao ; Yi, Jue-min ; Heidenblut, Torsten ; Segerink, Frans ; Babushkin, Ihar ; Kholodtsova, Maria ; Merdji, Hamed ; Bastiaens, Bert ; Morgner, Uwe ; Kovacev, Milutin. / Generating ultrabroadband deep-UV radiation and sub-10 nm gap by hybrid-morphology gold antennas. In: Nano letters. 2019 ; Vol. 19, No. 7. pp. 4779-4786.
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abstract = "We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a {"}plasmonic lens{"} and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.",
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author = "Liping Shi and Andrade, {Jose R. C.} and Ayhan Tajalli and Jiao Geng and Jue-min Yi and Torsten Heidenblut and Frans Segerink and Ihar Babushkin and Maria Kholodtsova and Hamed Merdji and Bert Bastiaens and Uwe Morgner and Milutin Kovacev",
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Shi, L, Andrade, JRC, Tajalli, A, Geng, J, Yi, J, Heidenblut, T, Segerink, F, Babushkin, I, Kholodtsova, M, Merdji, H, Bastiaens, B, Morgner, U & Kovacev, M 2019, 'Generating ultrabroadband deep-UV radiation and sub-10 nm gap by hybrid-morphology gold antennas' Nano letters, vol. 19, no. 7, pp. 4779-4786. https://doi.org/10.1021/acs.nanolett.9b02100

Generating ultrabroadband deep-UV radiation and sub-10 nm gap by hybrid-morphology gold antennas. / Shi, Liping; Andrade, Jose R. C.; Tajalli, Ayhan; Geng, Jiao; Yi, Jue-min; Heidenblut, Torsten; Segerink, Frans; Babushkin, Ihar; Kholodtsova, Maria; Merdji, Hamed; Bastiaens, Bert; Morgner, Uwe; Kovacev, Milutin.

In: Nano letters, Vol. 19, No. 7, 10.07.2019, p. 4779-4786.

Research output: Contribution to journalArticleAcademicpeer-review

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AU - Shi, Liping

AU - Andrade, Jose R. C.

AU - Tajalli, Ayhan

AU - Geng, Jiao

AU - Yi, Jue-min

AU - Heidenblut, Torsten

AU - Segerink, Frans

AU - Babushkin, Ihar

AU - Kholodtsova, Maria

AU - Merdji, Hamed

AU - Bastiaens, Bert

AU - Morgner, Uwe

AU - Kovacev, Milutin

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AB - We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

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