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Applied Physics Letters

Broadband sensitization of 1.53μm Er3+ luminescence in erbium-implanted alumina

Constantinos E. Chryssou, Anthony Joseph Kenyon, T. M. Smeeton, Colin John Humphreys, David E. Hole

Published Nov 29, 2004• 9 citations
Publisher

Abstract

Experimental evidence of an efficient broadband sensitization mechanism in erbium-implanted alumina is presented. Alumina thin films were deposited by plasma-enhanced chemical vapor deposition using trimethyl-amine alane and nitrous oxide. The as-grown films, together with sapphire crystals, were implanted with erbium. Photoluminescence excitation spectra showed that erbium-implanted sapphire crystals exhibit characteristic Er3+ luminescence at 1.53μm only when pumped resonantly. In contrast, erbium-implanted alumina thin films exhibit 1.53μm luminescence even when pumped at wavelengths outside Er3+ absorption bands. We postulate that the sensitizing species is either small nanoclusters of aluminum or pairs of aluminum ions.

DOI
10.1063/1.1829139

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Journal of Applied Physics•Sep 26, 2024•12 citations
Experimental evidence of an efficient broadband sensitization mechanism in erbium-implanted alumina is presented. Alumina thin films were deposited by plasma-enhanced chemical vapor deposition using trimethyl-amine alane and nitrous oxide. The as-grown films, together with sapphire crystals, were implanted with erbium. Photoluminescence excitation spectra showed that erbium-implanted sapphire crystals exhibit characteristic Er3+ luminescence at 1.53μm only when pumped resonantly. In contrast, erbium-implanted alumina thin films exhibit 1.53μm luminescence even when pumped at wavelengths outside Er3+ absorption bands. We postulate that the sensitizing species is either small nanoclusters of aluminum or pairs of aluminum ions.
Successful incorporation of both erbium and ytterbium in alumina by ion implantation is reported. Some evidence for indirect pumping of erbium through the transfer of energy from ytterbium has been observed. Both plasma-enhanced CVD deposited alumina thin films and sapphire crystals were employed as substrates. Yb3+ and Er3+ concentrations ranged from 2.4 At% to 8 At% and from 0.4 At% to 0.8 At%, respectively. The samples show strong, broad, room-temperature photoluminescence at λ = 1.53 µm corresponding to the intra-4f transitions between the 4I13/2 (first excited) and the 4I15/2 (ground) state of Er3+. The full width at half maximum of the emission spectrum is as high as 67 nm for the Al2O3 thin films; for the sapphire crystals it is 45 nm. The fluorescence lifetime of the samples has been measured to be as high as 4.2 ms at 50 mW pump power.
The spectra and photoluminescence kinetics of Er 3+ ions embedded in amorphous fluorine- and chlorine-doped silica matrices synthesized by surface-plasma chemical vapor deposition were investigated at 27–300 K. Luminescence was excited with an Ar + laser at a wavelength of 514.5 nm and with a diode laser at a wavelength of 975 nm. Narrow and well-expressed components of Stark sublevels with a small contribution of inhomogeneous broadening intrinsic to Er 3+ ions in crystalline rather than amorphous matrices were revealed and identified in photoluminescence spectra. The structure of Stark sublevels was well-resolved at low temperatures. The presence of the well-resolved Stark structure in spectra was indicative of stable anion complex formation in Er 3+ environment presumably associated with halogen incorporation. This environment was formed at a stage of the low-temperature plasma-chemical synthesis and was destroyed at glass fusion.
The effects of Au thin layers on luminescence properties of Er and Yb co-doped Al2O3 films were studied. The 1.54μm emission of Er3+ excited by the energy transfer from Yb3+ is found to be strongly enhanced by placing a Au layer on top of the films. Photoluminescence excitation spectra of the 1.54μm PL of Er3+ and time transients of the 980nm emission of Yb3+ revealed that PL enhancement arises from two different mechanisms. The first one is the enhancement of local electric fields accompanied by the excitation of surface plasmons of rough Au surfaces. The other one is the enhancement of energy transfer rate from Yb3+ to Er3+ caused by the modification of the local photonic mode density at the position of the Yb–Er coupled system.
The obtention of quantum-grade rare-earth-doped oxide thin films that can be integrated with optical cavities and microwave resonators is of great interest for the development of scalable quantum devices. Among the different growth methods, chemical vapor deposition (CVD) offers high flexibility and has demonstrated the ability to produce oxide films hosting rare-earth ions with narrow linewidths. However, growing epitaxial films directly on silicon is challenging by CVD due to a native amorphous oxide layer formation at the interface. In this manuscript, we investigate the CVD growth of erbium-doped yttrium oxide (Er:Y2O3) thin films on different substrates, including silicon, sapphire, quartz, or yttria stabilized zirconia (YSZ). Alternatively, growth was also attempted on an epitaxial Y2O3 template layer on Si (111) prepared by molecular beam epitaxy (MBE) in order to circumvent the issue of the amorphous interlayer. We found that the substrate impacts the film morphology and the crystalline orientations, with different textures observed for the CVD film on the MBE-oxide/Si template (111) and epitaxial growth on YSZ (001). In terms of optical properties, Er3+ ions exhibit visible and IR emission features that are comparable for all samples, indicating a high-quality local crystalline environment regardless of the substrate. Our approach opens interesting prospects to integrate such films into scalable devices for optical quantum technologies.
As an active material with favorable linear and nonlinear optical properties, thin-film lithium niobate has demonstrated its potential in integrated photonics. Integration with rare-earth ions, which are promising candidates for quantum memories and transducers, will enrich the system with new applications in quantum information processing. Here, we investigate the optical properties at 1.5 μm wavelengths of rare-earth ions (Er3+) implanted in thin-film lithium niobate waveguides and micro-ring resonators. Optical quality factors near a million after post-annealing show that ion implantation damage can be repaired. The transition linewidth and fluorescence lifetime of erbium ions are characterized. The ion-cavity coupling is observed through a Purcell enhanced fluorescence from which a Purcell factor of 3.8 ± 0.5, compared with waveguide lifetime, is extracted. This platform is compatible with top-down lithography processes and leads to a scalable path for controlling spin-photon interfaces in photonic circuits.
Rare-earth ion doped oxide thin films integrated on silicon substrates provide a route toward scalable, chip-scale platforms for quantum coherent devices. Erbium-doped TiO2 is an attractive candidate: the Er3+ optical transition is compatible with C-band optical fiber communications, while TiO2 is an insulating dielectric compatible with silicon process technology. Through structural and optical studies of Er-doped TiO2 thin films grown via molecular beam deposition on silicon, SrTiO3, and sapphire substrates, we have explored the impact of polycrystallinity and microstructure on the optical properties of the Er emission. Comparing polycrystalline TiO2(rutile)/Si with single-crystalline TiO2(rutile)/r-sapphire and polycrystalline TiO2(anatase)/Si with single-crystalline TiO2(anatase)/SrTiO3, we observe that the inhomogeneous linewidth (Γinh) of the most prominent peak in the Er spectrum (the Y1–Z1 transition, 1520 and 1533 nm in rutile and anatase TiO2) is significantly narrower in the polycrystalline case. This implies a relative insensitivity to extended structural defects and grain boundaries in such films (as opposed to, e.g., point defects). We show that the growth of an undoped, underlying TiO2 buffer on Si can reduce Γinh by a factor of 4–5. Expectedly, Γinh also reduces with decreasing Er concentrations: we observe a ∼2 order of magnitude reduction from ∼1000 ppm Er to ∼10 ppm Er. Γinh then gets limited to a residual value of ∼5 GHz that is insensitive to further reduction in the Er concentration. Based upon the above results, we argue that the optical properties in these thin films are limited by the presence of high “grown-in” point defect concentrations.