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Applied Physics Letters

Enhancement of photoluminescence from Yb and Er co-doped Al2O3 films by an asymmetric metal cavity

Nobuto Managaki, Minoru Fujii, Toshihiro Nakamura, Yoshiko Usui, Shinji Hayashi

Published Jan 20, 2006• 13 citations
Publisher

Abstract

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.

DOI
10.1063/1.2166685

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Applied Physics Letters•Nov 29, 2004•9 citations
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.
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.
Considering cooperative up-conversion,cross-relaxation and excited state absorption,the rate equations of eight energy levels were founded for Yb-Er co-doped Al 2O 3 materials.The functions of coefficients of cooperative up-conversion,cross-relaxation and excited state absorption varied along with the concentrations of ytterbium and erbium were built phenomenologically.The relationship among 1.53 μm photoluminescence intensity,doped concentration,and pump power were numerically simulated for Yb-Er co-doped Al 2O 3 film.The results show that there is the optimum Yb-doped concentration when Er-doped concentration and pump power are constant.The optimal Yb∶Er ratio will decrease following with increase of pump power under the fixed Er-doped concentration,and the optimal Yb∶Er ratio will also decrease following with increase of Er-doped concentration when pump power is fixed.The computed results are in good agreement with the experiment surveys.
Sputter-deposited thin-film amorphous AlN:Er (1 at. %) emits at 554 and 561 nm as a result of (2)H(11/2)→(4)I(15/2) and (4)S(3/2)→(4)I(15/2) transitions. AlN:Yb (1 at. %) gives a weak emission peak at 966 nm as a result of (2)F(5/2)→(2)F(7/2). The codoping of Er and Yb in AlN results in energy transfer from Er(+3) to Yb(+3) and enhances the Yb(+3) emissions by an order of magnitude. Transfer of electrons occurs from the (4)S(3/2) state of Er(+3) to the (2)F(5/2) state of Yb(+3). The weak emission from Yb(+3), when excited by a 532 nm laser in the absence of Er(+3), confirms that the luminescence enhancement in ytterbium is due to energy transfer and not to direct green light excitation by the erbium emission. A possibility of population inversion and a four-level laser cavity formation exists in the Er(+3)-Yb(+3) system.
Atomic layer deposited (ALD) Y 2 O 3 thin films have been thoroughly investigated for optical or electronic applications. The coherent spectroscopy of lanthanide ions doped into this material has also recently attracted increasing interest in the field of quantum technologies for which they are considered promising candidates in quantum memories or as spin–photon interfaces. However, these most demanding applications require a deep control over the local positioning of the ions and their close environment in the crystalline matrix. This study focuses on the structural as well as optical properties of Eu 3+ and Er 3+ dopants in Y 2 O 3 using photoluminescence (PL), luminescence decay times, and inhomogeneous line width (Γ inh ) measurements within this particular context. While as-grown ALD films do not provide an ideal host for the emitters, we demonstrate that by optimizing the deposition conditions and using appropriate annealing post treatments narrow inhomogeneous lines can be obtained for the 7 F 0 ↔ 5 D 0 transition of Eu 3+ even for nanoscale films. Furthermore, about 1.5 ms lifetime has been measured for the infrared telecom transition of Er in ultrathin films (<10 nm), which is an order of magnitude higher than in nanoparticles of the same size. These results validate optimized rare-earth-doped ALD Y 2 O 3 films as a suitable platform for photonics applications where few-nanometer-thick films with well-localized emitters are mandatory. This approach provides the first building blocks toward the development of more complex devices for quantum sensing or hybrid structures coupled with other systems such as two-dimensional materials.
We fabricated ytterbium-doped yttrium aluminum oxide (Yb:Y–Al–O) thin films by radio-frequency magnetron sputtering and evaluated their crystallinity and anti-Stokes photoluminescence (PL) properties for optical refrigeration. The Yb:Y–Al–O films that were grown on c-sapphire substrates had better transparency than the films deposited on fused-quartz substrates. The better transparency is considered to be a result of the smaller mismatch between the thermal expansion coefficients of Yb:Y–Al–O and c-sapphire. We found that the thin films on the c-sapphire substrates consist of densely packed sub-micron columnar crystals that are aligned perpendicular to the substrate. In these films, we confirmed the existence of perovskite, garnet, and monoclinic phases despite using a single-phase sputtering target. The excitation wavelength dependence of anti-Stokes PL is used to investigate the energy transfer process between trivalent Yb ions in neighboring columnar crystals. The data indicate that the resonant energy transfer from Yb3+ ions at a specific seven-coordinated site of the monoclinic phase to Yb3+ ions in neighboring columnar crystals is faster than the radiative relaxation at the energy-donor site.
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.