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Optical transition between Stark levels in (ErSc)2O3 epitaxitial films

Takehiko Tawara, Hiroo Omi, Adel Najar, Reina Kaji, S. Adachi, Hideki Gotoh

Published Jan 1, 2014• 0 citations
Publisher

Abstract

Toward quantum information applications, we control the interactions between Er ions by alloying epitaxial Er2O3 with scandium and suppress energy transfer and inhomogeneous broadening of Stark levels in the intra-4f band of Er ions.
DOI
10.1364/cleo_at.2014.jw2a.56

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We grow single crystal erbium-oxide (Er2O3) epitaxially on a Si (111) substrate by using molecular beam epitaxy and investigate the population dynamics in Er3+ ions for the coherent manipulation of the population in Er2O3. Sharp and discrete Stark energy levels of the 4I13/2 manifold as small as 200 μeV are observed with inhomogeneous broadening caused by the uniform crystal field of the epitaxial Er2O3. We also experimentally determine the time constant of the resonant population transfer between spatially distant Er3+-ion sites, which is limited to the manipulation time of the population in the Er2O3 crystals. Using selective excitation of the Stark level in the 4I13/2 manifold, we obtain the energy transfer times between spatially distant Er3+ ions, and they are about 2 μs between sites whose crystallographic symmetry is different and 10 μs between sites whose symmetry is the same.
Rare-earth ions (REIs) have incomplete 4f shells and possess narrow optical intra-4f transitions due to shielding from electrons in the 5s and 5p orbitals, making them good candidates for solid-state optical quantum memory. The emission of Er3+ in the telecom C-band (1530 nm–1565 nm) makes it especially attractive for this application. In order to build practical, scalable devices, the REI needs to be embedded in a non-interacting host material, preferably one that can be integrated with silicon. In this paper, we show that Er3+ can be isovalently incorporated into epitaxial Y2O3 thin films on Si (111). We report on the synthesis of epitaxial, single-crystalline Er:Y2O3 on Si with a narrow inhomogeneous linewidth in the photoluminescence (PL) spectra, 5.1 GHz (<100 mK), and an optical excited state lifetime of 8.1 ms. The choice of Y2O3 was driven by its low nuclear spin and small lattice mismatch with Si. Using PL and electron paramagnetic resonance, we show that Er3+ substitutes for Y in the crystal lattice. The role of interfacial SiOx, diffusion of silicon into the film, and the effect of buffer layers on the inhomogeneous PL linewidth are examined. We also find that the linewidth decreased monotonically with film thickness but surprisingly exhibits no correlation with the film crystalline quality, as measured by the x-ray rocking curve scans, suggesting other factors at play that limit the inhomogeneous broadening in Y2O3 films.
We have investigated the energy transfers in the 1.54- μ m region of (Er,Sc) 2 O 3 epitaxial thin films grown on Si(111). The interplay of the energy transfers between Er ions in the different and the same symmetry sites makes the dynamics complicated. To suppress the energy transfer upconversion, low power and resonant excitation of the third crystal-field level ( 4 I 13 / 2 : Y 3 ′ ) of the Er 3 + site with C 3 i symmetry was employed. The time-resolved photoluminescence measurements of the Y 1 ′ - Z 1 ′ transition indicate the existence of two decay components having fast (10–100 μ s) and slow (0.1–1 ms) relaxation times in the range of 4–60 K. The model calculation including the inter-site energy transfers, the temperature-sensitive and -insensitive non-radiative relaxations fits the experimental results well. Moreover, the long averaged inter-Er 3 + distance obtained by decreasing Er concentration was found to reduce two kinds of non-radiative relaxation rates and the energy transfer rates between Er ions very effectively.