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The growth of InGaN alloys via Metal-Modulated Epitaxy has been investigated. Transient reflection high-energy electron diffraction intensities for several modulation schemes during the growth of 20% InGaN were analyzed, and signatures associated with the accumulation, consumption, and segregation of excess metal adlayers were identified. A model for shuttered, metal-rich growth of InGaN was then developed, and a mechanism for indium surface segregation was elucidated. It was found that indium surface segregation only occurs after a threshold of excess metal is accumulated, and a method of quantifying this indium surface segregation onset dose is presented. The onset dose of surface segregation was found to be indium-composition dependent and between 1 and 2 monolayers of excess metal. Below this surface threshold off excess metal, metal-rich growth can occur without indium surface segregation. Since at least 2 monolayers of excess metal will accumulate in the case of metal-rich, unshuttered growth of InGaN at the low temperatures required to suppress thermal and spinodal decomposition, this study reveals that some form of modulation must be employed to maintain this adlayer thickness. These theories were applied in the growth of InGaN with varying compositions using Metal-Modulated Epitaxy. Single-phase, high-quality InGaN films with compositions throughout the miscibility gap with root mean square roughnesses less than 0.8 nm were obtained, demonstrating the feasibility of shuttered, metal-rich InGaN growth.

The surface kinetics of InGaN alloys grown via metal-modulated epitaxy (MME) are explored in combination with transient reflection high-energy electron diffraction intensities. A method for monitoring and controlling indium segregation in situ is demonstrated. It is found that indium segregation is more accurately associated with the quantity of excess adsorbed metal, rather than the metal-rich growth regime in general. A modified form of MME is developed in which the excess metal dose is managed via shuttered growth, and high-quality InGaN films throughout the miscibility gap are grown.

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