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Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics

Study of the atomic dynamics of nanoclusters Y2SiO5:Pr3+by the confocal fluorescent microscopy

Yu. V. Malyukin, P.N. Zhmurin, Е. С. Сыркин, S. B. Feodosyev, M. A. Mamaluı̆

Published Nov 1, 2004• 0 citations

Abstract

The system under consideration consists of a Pr3+ ion placed into a nanodimensional Y2SiO5 crystal (∼20 nm), which rests on a glass substrate. The spectrum and attenuation of the fluorescence of the Pr3+ ion have been studied by the method of confocal fluorescent microscopy. The rapid electron relaxation in J-multiplets of rare earth impurity ions split by the crystal field (for a usual bulk crystal τ∼10–9–10–12 sec) is shown to be suppressed in the nanodimensional crystal of Y2SiO5:Pr3+. For the excited Stark components of 1D2 multiplet, the electron relaxation appears to be more than 104 times suppressed, while an average splitting of the 1D2 multiplet by the crystal field of ligands is 200 cm–1. The observed phenomena strongly depends on the interaction of the Y2SiO5:Pr3+ cluster with the substrate and the surrounding (‘matrix’). Experimental results and theoretical calculations show the noticeble changes in the structure of vibrational spectrum and the density of vibrational states of the nanodimensional Y2SiO5:Pr3+ crystal. (© 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

DOI: 10.1002/pssc.200405311

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The system under consideration consists of a Pr3+ ion placed into a nanodimensional Y2SiO5 crystal (∼20 nm), which rests on a glass substrate. The spectrum and attenuation of the fluorescence of the Pr3+ ion have been studied by the method of confocal fluorescent microscopy. The rapid electron relaxation in J-multiplets of rare earth impurity ions split by the crystal field (for a usual bulk crystal τ∼10–9–10–12 sec) is shown to be suppressed in the nanodimensional crystal of Y2SiO5:Pr3+. For the excited Stark components of 1D2 multiplet, the electron relaxation appears to be more than 104 times suppressed, while an average splitting of the 1D2 multiplet by the crystal field of ligands is 200 cm–1. The observed phenomena strongly depends on the interaction of the Y2SiO5:Pr3+ cluster with the substrate and the surrounding (‘matrix’). Experimental results and theoretical calculations show the noticeble changes in the structure of vibrational spectrum and the density of vibrational states of the nanodimensional Y2SiO5:Pr3+ crystal. (© 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Optical read-out and manipulation of the nuclear spin state of single rare-earth ions doped in a crystal enable the large-scale storage and the transport of quantum information. Here, we report the photo-luminescence excitation spectroscopy results of single Pr3+ ions in a bulk crystal of LaF3 at 1.5 K. In a bulk sample, the signal from a single ion at the focus is often hidden under the background signal originating from numerous out-of-focus ions in the entire sample. To combine with a homemade cryogenic confocal microscope, we developed a reflecting objective that works in superfluid helium with a numerical aperture of 0.99, which increases the signal by increasing the solid angle of collection to 1.16π and reduces the background by decreasing the focal volume. The photo-luminescence excitation spectrum of single Pr3+ was measured at a wing of the spectral line of the 3H4 right arrow 3P0 transition at 627.33 THz (477.89 nm). The spectrum of individual Pr3+ ions appears on top of the background of 60 cps as isolated peaks with intensities of 20–30 cps and full-width at half-maximum widths of approximately 3 MHz at an excitation intensity of 80 W cm−2.

Rare earth ions in crystals exhibit narrow spectral features and hyperfine-split ground states with exceptionally long coherence times. These features make them ideal platforms for quantum information processing in the solid state. Recently, we reported on the first high-resolution spectroscopy of single ions in yttrium orthosilicate nanocrystals via the transition at a wavelength of 488 nm. Here we show that individual praseodymium ions can also be detected on the more commonly studied transition at 606 nm. In addition, we present the first measurements of the second-order autocorrelation function, fluorescence lifetime, and emission spectra of single ions in this system as well as their polarization dependencies on both transitions. Furthermore, we demonstrate that by a proper choice of the crystallite, one can obtain narrower spectral lines and, thus, resolve the hyperfine levels of the excited state. We expect our results to make single-ion spectroscopy accessible to a larger scientific community.

Optical read-out and manipulation of the nuclear spin state of single rare-earth ions doped in a crystal enable the large-scale storage and the transport of quantum information. Here, we report the photo-luminescence excitation spectroscopy results of single Pr(3+) ions in a bulk crystal of LaF3 at 1.5 K. In a bulk sample, the signal from a single ion at the focus is often hidden under the background signal originating from numerous out-of-focus ions in the entire sample. To combine with a homemade cryogenic confocal microscope, we developed a reflecting objective that works in superfluid helium with a numerical aperture of 0.99, which increases the signal by increasing the solid angle of collection to 1.16π and reduces the background by decreasing the focal volume. The photo-luminescence excitation spectrum of single Pr(3+) was measured at a wing of the spectral line of the (3)H4 → (3)P0 transition at 627.33 THz (477.89 nm). The spectrum of individual Pr(3+) ions appears on top of the background of 60 cps as isolated peaks with intensities of 20-30 cps and full-width at half-maximum widths of approximately 3 MHz at an excitation intensity of 80 W cm(-2).

Quantum computing with single instances of rare earth-ions doped into inorganic crystals shows great promise as a scalable design in the field of quantum information. A detectable and controllable single readout ion is necessary for the scheme proposed in Lund to work. Due to its short excited state lifetime and its cyclable 4f-5d transition, cerium has been deemed suitable for just this purpose. The approach taken in Lund for this single cerium detection is to use a homemade confocal microscopy setup. In previous work using this setup on bulk crystals, it has been assumed that the undetectability of single cerium is due to out of focus ions contributing to a noise floor that is higher than the fluorescence signal from a single one. Hence single ion detection is being attempted in microcrystals. This thesis outlines the process behind converting the confocal microscope into a microcrystal detection setup. Subsequently, Ce3+:Y2SiO5 microcrystal spectroscopy experiments were performed. The energy level structure of cerium is reported to be identical to bulk, with a slight shift in wavelength, and the inhomogenous linewidth has proven to be inconclusive, although it hints towards being much wider than in bulk. Quantifying the homogenous linewidth of the cerium ions using Zeeman hole burning techniques was impervious to our attempts.