Traditionally accepted design paradigms dictate that only optically isotropic (cubic) crystal structures with high equilibrium solubilities of optically active ions are suitable for polycrystalline laser gain media. The restriction of symmetry is due to light scattering caused by randomly oriented anisotropic crystals, whereas the solubility problem arises from the need for sufficient active dopants in the media. These criteria limit material choices and exclude materials that have superior thermo-mechanical properties than state-of-the-art laser materials. Alumina (Al2O3) is an ideal example; it has a higher fracture strength and thermal conductivity than today’s gain materials, which could lead to revolutionary laser performance. However, alumina has uniaxial optical proprieties, and the solubility of rare earths (REs) is two-to-three orders of magnitude lower than the dopant concentrations in typical RE-based gain media. We present new strategies to overcome these obstacles and demonstrate gain in a RE-doped alumina (Nd:Al2O3) for the first time. The key insight relies on tailoring the crystallite size to other important length scales—the wavelength of light and interatomic dopant distances, which minimize optical losses and allow successful Nd doping. The result is a laser gain medium with a thermo-mechanical figure of merit of Rs~19,500 Wm−1 a 24-fold and 19,500-fold improvements over the high-energy-laser leaders Nd:YAG (Rs~800 Wm−1) and Nd:Glass (Rs~1 Wm−1), respectively. Moreover, the emission bandwidth of Nd:Al2O3 is broad: ~13 THz. The successful demonstration of gain and high bandwidth in a medium with superior Rs can lead to the development of lasers with previously unobtainable high-peak powers, short pulses, tunability, and high-duty cycles.
Here we develop and characterize high thermal conductivity/high thermal shock resistant bulk Ce doped Al2O3 and propose it as a new phosphor converting capping layer for highpowered/high-brightness solid-state white lighting (SSWL). The bulk, dense Ce:Al2O3 ceramics have a 0.5 at.% Ce:Al concentration (significantly higher than the equilibrium solubility limit), and were produced using a simultaneous solid-state reactive Current Activated Pressure-Assisted Densification (CAPAD) approach. Ce:Al2O3 exhibits a broadband emission from 400-600nm, which encompasses the entire blue and green portions of the visible spectrum when pumped with ultra-violet (UV) light that is now commercially available in UV light emitting devices (LED) and laser diodes (LD). These broadband phosphors can be used in the commonly employed scheme of mixing with other UV converting capping layers that emit red light to produce white light.Alternatively, they can be used in a novel composite down converter approach that ensures improved thermal-mechanical properties of the converting phosphor capping layer. In this configuration Ce:Al2O3 is used with proven phosphor conversion materials such as Ce:YAG as an active encapsulant or as a capping layer to produce SSWL with an improved bandwidth in the blue portion of the visible spectrum. In order to study the effect of crystallinity on the Ce PL emission, we synthesize Ce:YAG ceramics using high-pressure CAPAD at moderate temperatures to obtain varying crystallinity (amorphous through fully -crystalline). We investigate the PL characteristics of Ce:Al2O3 and Ce:YAG from 295K to 4K, revealing unique crystal field effects from the matrix on the Ce-dopants. The unique PL properties in conjunction with the superior thermal-mechanical properties of Ce:Al2O3 can be used in high-powered/high-brightness integrated devices based on high-efficiency UV-LD that do not suffer from efficiency droop at high drive currents to pump the solid-state capping phosphors.
Producing bulk AlN with grain sizes in the nano regime and measuring its thermal conductivity is an important milestone in the development of materials for high energy optical applications. We present the synthesis and subsequent densification of nano-AlN powder to produce bulk nanocrystalline AlN. The nanopowder is synthesized by converting transition alumina (δ-Al2O3) with <40 nm grain size to AlN using a carbon free reduction/nitridation process. We consolidated the nano-AlN powder using current activated pressure assisted densification (CAPAD) and achieved a relative density of 98% at 1300 °C with average grain size, d¯~125 nm. By contrast, high quality commercially available AlN powder yields densities ~75% under the same CAPAD conditions. We used the 3-ω method to measure the thermal conductivity, κ of two nanocrystalline samples, 91% dense, d¯ = 110 nm and 99% dense, d¯ = 220 nm, respectively. The dense sample with 220 nm grains has a measured κ = 43 W/(m·K) at room temperature, which is relatively high for a nanocrystalline ceramic, but still low compared to single crystal and large grain sized polycrystalline AlN which can exceed 300 W/(m·K). The reduction in κ in both samples is understood as a combination of grain boundary scattering and porosity effects. We believe that these are finest d¯ reported in bulk dense AlN and is the first report of thermal conductivity for AlN with ≤220 nm grain size. The obtained κ values are higher than the vast majority of conventional optical materials, demonstrating the advantage of AlN for high-energy optical applications.
The middle initial of Matthew C. Wingert was omitted. (ii) Two in-text citations have been updated for the following sentences due to errors in the reference list: The behavior of Ce:Al 2 O 3 is consistent with the lowtemperature optical behavior of other rare earths doped into oxides, such as Nd-[38, 39] and Er-doped [31] YAG, that exhibit optical 4f to 4f transitions that are shielded from crystal-field interactions by the outer 5d shell. The bulk ceramic Ce:Al 2 O 3 phosphors were produced using an all-solid-state, one-step reaction-densification route using CAPAD [23, 31].
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