Gradual Carrier Filling Effect in "Green" InGaN/GaN Quantum Dots: Femtosecond Carrier Kinetics with Sequential Two-Photon Absorption.

Quantum dots (QDs) allow for a significant amount of strain relaxation, which is helpful in GaN systems where a large lattice mismatch needs to be accommodated. InGaN QDs with a large indium composition are intensively investigated for light emitters requiring longer wavelengths. These are especially important for developing high-efficiency white light sources. Understanding the carrier dynamics in this large lattice-mismatched system is essential to improving the radiative efficiency while circumventing high defect density. This work investigates femtosecond carrier and photon dynamics in self-organized In0.27Ga0.73N/GaN QDs grown by molecular beam epitaxy using transient differential absorption spectroscopy, which measures the differential absorption coefficient (Δα) with and without an optical pump. Due to 3D quantum confinement and the small effective mass of InGaN, the low density of states in the conduction band is easily filled with electrons. In contrast, the GaN barrier region is replete with a high density of electrons due to a large effective mass. This contrast in carrier density creates a unique phenomenon in the dynamics, showing a change in the differential absorption coefficient (Δα) sign from negative to positive with time. The ultrafast microscopic processes indicate that right after the optical pump and first photon absorption, the valence (conduction) band states are depleted (replete) of electrons. This ground-state bleaching process makes Δα negative, and the probe beam is not absorbed. The electrons are then gradually transferred from the GaN barrier into InGaN QDs, which absorb the second photon from the probe beam (excited-state absorption), making Δα positive. The presence of excited-state carriers with a long lifetime is indicative of the enhanced availability of carriers for radiative recombination. This effect also promotes stimulated emission and amplified spontaneous emission, which can be used to develop lasers and superluminescent LEDs, respectively. Measurements with multiple pump powers and temperatures further confirm that the efficacy of InGaN QDs is enhanced by this effective mass contrast and 3D reservoir of carriers from the GaN barrier. This effect can be used to improve the internal quantum efficiency of GaN-based light emitters.