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Measuring the Magnetic Dipole Transition of Single Nanorods by Spectroscopy and Fourier Microscopy

Reinaldo Chacon, Aymeric Leray, Jeongmo Kim, Khalid Lahlil, Sanro Mathew, Alexandre Bouhelier, Jong-Wook Kim, Thierry Gacoin, and Gérard Colas des Francs
Phys. Rev. Applied 14, 054010 – Published 5 November 2020

Abstract

Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the 5D07F1 transition dipole vector in individual NaYF4:Eu3+ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of NaYF4:Eu3+ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.

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  • Received 16 March 2020
  • Revised 11 September 2020
  • Accepted 5 October 2020

DOI:https://doi.org/10.1103/PhysRevApplied.14.054010

© 2020 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Reinaldo Chacon1, Aymeric Leray1, Jeongmo Kim2, Khalid Lahlil2, Sanro Mathew1, Alexandre Bouhelier1, Jong-Wook Kim2, Thierry Gacoin2, and Gérard Colas des Francs1,*

  • 1Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB), UMR 6303, CNRS, Université Bourgogne Franche-Comté, 9 Avenue Savary, BP 47870, Dijon Cedex 21078, France
  • 2Physique de la Matière Condensée, CNRS UMR 7643, Ecole Polytechnique, Palaiseau 91128, France

  • *gerard.colas-des-francs@u-bourgogne.fr

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Vol. 14, Iss. 5 — November 2020

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Images

  • Figure 1
    Figure 1

    Schematic representation of the confocal optical microscope. The europium ions are excited by a continuous-wave laser emitting at a wavelength of 392 nm and focused by a microscope objective (40×, NA=0.6 or 60×NA=1.49, Nikon). The luminescence is collected by the same objective and is separated from the excitation laser by a dichroic mirror and routed either to an avalanche photodiode (APD) for confocal imaging or to a spectrometer. The polarization of the emitted light is analyzed placing a polarizer after the sample (“analyzer”).

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  • Figure 2
    Figure 2

    (a) SEM image of a NaYF4:Eu3+ single nanorod with a diameter of 90 nm and a length of 1500 nm. (b) Confocal image of the luminescence emitted by the same rod.

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  • Figure 3
    Figure 3

    (a) Spectrum of a single NaYF4:Eu3+ nanorod (obtained without the analyzer, and with an objective NA=0.6). (b) Energy diagram of trivalent europium. The ion has a 4f6 configuration with optical transitions occurring between the levels 5D1 or 5D0 and 7FJ. Each level has a degeneracy of 2J+1 split by the crystalline field into different Stark levels.

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  • Figure 4
    Figure 4

    Orientation of the dipole transition moment for a rod on the substrate. The emission is modeled by dipolar emitters oriented at a fixed angle with respect to the c axis (cone of semiangle α).

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  • Figure 5
    Figure 5

    (a) Luminescence spectra of single NaYF4:Eu3+ nanorod for different analyzer angles. The 5D07F1 magnetic transitions are highlighted in gray and enlarged in (b) for an analyzer angle of 0. Spectral unmixing is performed by the fitting experimental data with a sum of three Gaussians. Three magnetic dipoles can be isolated, they are noted MD1 (in red, Gaussian width 1.2 nm), MD2 (in green, Gaussian width 0.8 nm) and MD3 (in blue, Gaussian width 1.5 nm). The normalized polarization diagrams of MD1, MD2, and MD3 are shown with dots in the polar plots (c1)–(c3), respectively. For each dipole, a normalization is performed on the maximum emission of a single nanorod. The lines correspond to fits using the full model.

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  • Figure 6
    Figure 6

    Fourier imaging of a single NaYF4:Eu3+ nanorod for the 586.8–593.6 nm wavelength range. Experimental Fourier images acquired with analyzer angles of 0, 60, and 120 are shown, respectively, in (a1)–(a3). The white circle with larger diameter indicates the maximum collection angle corresponding to the numerical aperture of the objective (NA=1.49). We also represent the circle indicating the critical angle for an air-quartz interface (corresponding to NA=1.0). These experimental images are compared to the theoretical ones shown in (b1)–(b3) for an analyzer angle of, respectively, 0, 60, and 120. For each analyzer angle, we represent in (c1)–(c3), the experimental (in solid blue line) and theoretical (in dashed red line) intensity profiles corresponding to the white dashed lines in (a) and (b).

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  • Figure 7
    Figure 7

    Fourier imaging of single NaYF4:Eu3+ nanorod for 591.0–598.6 nm wavelength range. Experimental Fourier images acquired with analyzer angle of 0, 60, and 120 are shown, respectively, in (a1)–(a3). The white circle with larger diameter indicates the maximum collection angle corresponding to the numerical aperture of the objective (NA=1.49). We also represent the circle indicating the critical angle for an air-quartz interface (corresponding to NA=1.0). These experimental images are compared to the theoretical ones shown in (b1)–(b3) for an analyzer angle of, respectively, 0, 60, and 120. For each analyzer angle, we represent in (c1)–(c3), the experimental (in solid blue line) and theoretical (in dashed red line) intensity profiles corresponding to the white dashed lines in (a),(b).

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  • Figure 8
    Figure 8

    Notation for the scattered dipolar field.

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