Jan Talbot

Development of White-Light Emitting Active Layers in Nitride Based Heterostructures for Phosphorless Solid State Lighting

This report provides a summary of research activities carried out at the University of California, San Diego and Central Research of OSRAM SYLVANIA in Beverly, MA partially supported by a research contract from US Department of Energy, DE-FC26-04NT422274. The main objective of this project was to develop III-V nitrides activated by rare earth ions, RE{sup 3+}, which could eliminate the need for phosphors in nitride-based solid state light sources. The main idea was to convert electron-hole pairs injected into the active layer in a LED die to white light directly through transitions within the energy levels of the 4f{sup n}-manifold of RE{sup 3+}. We focused on the following materials: Eu{sup 3+}(red), Tb{sup 3+}(green), Er{sup 3+}(green), Dy{sup 3+}(yellow) and Tm{sup 3+}(blue) in AlN, GaN and alloys of AlN and GaN. Our strategy was to explore candidate materials in powder form first, and then study their behavior in thin films. Thin films of these materials were to be deposited on sapphire substrates using pulsed laser deposition (PLD) and metal organic vapor phase epitaxy (MOVPE). The photo- and cathode-luminescence measurements of these materials were used to investigate their suitability for white light generation. The project proceeded along this route with minor modifications neededmorexa0» to produce better materials and to expedite our progress towards the final goal. The project made the following accomplishments: (1) red emission from Eu{sup 3+}, green from Tb{sup 3+}, yellow from Dy{sup 3+} and blue from Tm{sup 3+} in AlN powders; (2) red emission from Eu{sup 3+} and green emission from Tb{sup 3+} in GaN powder; (3) red emission from Eu{sup 3+} in alloys of GaN and AlN; (4) green emission from Tb{sup 3+} in GaN thin films by PLD; (5) red emission from Eu{sup 3+} and Tb{sup 3+} in GaN thin films deposited by MOVPE; (6) energy transfer from host to RE{sup 3+}; (7) energy transfer from Tb{sup 3+} to Eu{sup 3+} in AlN powders; (8) emission from AlN powder samples codoped with (Eu{sup 3+} ,Tb{sup 3+} ) and (Dy{sup 3+}, Tm{sup 3+}); and (9) white emission from AlN codoped with Dy{sup 3+} and Tm{sup 3+}. We also extensively studied the stabilities of rare earth ions in GaN, and the nature of oxygen defects in GaN and its impact on the optical properties of the host material, using first principles method. Results from these theoretical calculations together with fluorescence measurements from the materials essentially proved the underlying concepts for generating white light using RE{sup 3+}-activated nitrides. For this project, we successfully built a horizontal MOVPE reactor and used it to deposit thin films of undoped and doped nitrides of GaN and InGaN, which is a very significant achievement. Since this reactor was designed and built by in-house experts, it could be easily modified and reassembled for specific research purposes. During this study, it was successfully modified for homogeneous distribution of rare earth ions in a deposited film. It will be an ideal tool for future research involving novel thin film material concepts. We examined carefully the suitability of various metal organic precursors for incorporating RE{sup 3+}. In order to avoid oxygen contamination, several oxygen-free RE{sup 3+} precursors were identified. Both oxygen-free and oxygen- containing metal organic precursors were used for certain rare earth ions (Eu{sup 3+}, Tb{sup 3+} and Er{sup 3+}). However, the suitability of any particular type of precursor for MOVPE deposition was not established during this study, and further study is needed. More intensive research in the future is needed to improve the film quality, and eliminate the separation of rare earth oxide phases during the deposition of thin films by MOVPE. The literature in the area of the chemistry of rare earth ions in nitrides is almost nonexistent, in spite of the significant research on luminescence of RE{sup 3+} in nitrides. Consequently, MOVPE as a method of deposition of RE{sup 3+}-activated nitrides is relatively unexplored. In the following sections of this report, the outcomes from this study are described in detail. The present investigations have clearly validated the underlying concepts for generating white light within the LED die itself and its importance for fabricating a new generation of solid state light sources. Yet, significant research is still needed to transform these concepts into products.«xa0less