Optical investigations of InGaN heterostructures and GeSn nanocrystals for photonic and phononic applications: light emitting diodes and phonon cavities

InGaN heterostructures are at the core of blue light emitting diodes (LEDs) which are the basic building blocks for energy efficient and environment friendly modern white light generating sources. Through quantum confinement and electronic band structure tuning on the opposite end of the spectrum, Ge1−xSnx alloys have recently attracted significant interest due to its potential role as a silicon compatible infra-red (IR) optical material for photodetectors and LEDs owing to transition to direct bandgap with increasing Sn. This thesis is dedicated to establishing an understanding of the optical processes and carrier dynamics in InGaN heterostructures for achieving more efficient visible light emitters and terahertz generating nanocavities and in colloidal Ge1−xSnx quantum dots (QDs) for developing efficient silicon compatible optoelectronics. To alleviate the electron overflow, which through strong experimental evidence is revealed to be the dominating mechanism responsible for efficiency degradation at high injection in InGaN based blue LEDs, different strategies involving electron injectors and optimized active regions have been developed. Effectiveness of optimum electron injector (EI) layers in reducing electron overflow and increasing quantum efficiency of InGaN based LEDs was demonstrated by photoluminescence (PL) and electroluminescence spectroscopy along with numerical simulations. Increasing the two-layer EI thickness in double heterostructure LEDs substantially reduced the electron overflow and increased external quantum efficiency (EQE) by three fold. By incorporating δ p-doped InGaN barriers in multiple quantum well (MQW) LEDs, 20% enhancement in EQE was achieved due to improved hole injection without degrading the layer quality. Carrier diffusion length, an important physical parameter that directly affects the performance of optoelectronic devices, was measured in epitaxial GaN using PL spectroscopy. The obtained diffusion lengths at room temperature in p- and n-type GaN were 93±7 nm and 432±30 nm, respectively. Moreover, near field scanning optical microscopy was employed to investigate the spatial variations of extended defects and their effects on the optical quality of semipolar and InGaN heterostructures, which are promoted for higher efficiency light emitters owing to reduced internal polarization fields. The near-field PL from the c+ wings in heterostructures was found to be relatively strong and uniform across the sample but the emission from the c- wings was substantially weaker due to the presence of high density of threading dislocations and basal plane stacking faults. In case of heterostructures, striated regions had weaker PL intensities compared to other regions and the meeting fronts of different facets were characterized by higher Indium content due to the varying internal field. Apart from being the part and parcel of blue LEDs, InGaN heterostructures can be utilized in generation of coherent lattice vibrations at terahertz frequencies. In analogy to LASERs based on photon cavities where light intensity is amplified, acoustic nanocavity devices can be realized for sustaining terahertz phonon oscillations which could potentially be used in acoustic imaging at the nanoscale and ultrafast acousto-optic modulation. Using In0.03Ga0.97N/InxGa1-xN MQWs with varying x, coherent phonon oscillations at frequencies of 0.69-0.80 THz were generated, where changing the MQW period (11.5 nm -10 nm) provided frequency tuning. The magnitude of phonon oscillations was found to increase with indium content in quantum wells, as demonstrated by time resolved differential transmission spectroscopy. Design of an acoustic nanocavity structure was proposed based on the abovementioned experimental findings and also supported by full cavity simulations. Optical gap engineering and carrier dynamics in colloidal Ge1−xSnx QDs were investigated in order to explore their potential in optoelectronics. By changing the Sn content from 5% to 23% in 2 nm-QDs, band-gap tunability from 1.88 eV to 1.61 eV, respectively, was demonstrated at 15 K, consistent with theoretical calculations. At 15 K, time resolved PL spectroscopy revealed slow decay (3 − 27 μs) of luminescence, due to recombination of spin-forbidden dark excitons and effect of surface states. Increase in temperature to 295 K led to three orders of magnitude faster decay (9 − 28 ns) owing to the effects of thermal activation of bright excitons and carrier detrapping from surface states. These findings on the effect of Sn incorporation on optical properties and carrier relaxation and recombination processes are important for future design of efficient Ge1−xSnx QDs based optoelectronic devices. This thesis work represents a comprehensive optical study of InGaN heterostructures and colloidal Ge1−xSnx QDs which would pave the way for more efficient InGaN based LEDs, realization of terahertz generating nanocavities, and efficient Ge1−xSnx based silicon compatible optoelectronic devices