Probing Alloy Formation Using Different Excitonic Species: The Particular Case of InGaN

Abstract

Since the early 1960s, alloys are commonly grouped into two classes that feature either bound states in the band gap (I) or additional, nondiscrete band states (II). Consequently, one can observe either excitons bound to isoelectronic impurities or the typical band edge emission of a semiconductor that shifts and broadens with rising isoelectronic doping concentration. Microscopic parameters for class I alloys can directly be extracted from photoluminescence (PL) spectra, whereas any conclusions drawn for class II alloys usually remain limited to macroscopic assertions. Nonetheless, we present a spectroscopic study on exciton localization in a mixed-crystal alloy (class II) that allows us to access microscopic alloy parameters. In order to illustrate our approach, we study bulk In x Ga 1−x N epilayers at the onset of alloying (0 ≤ x ≤ 2.4%) in order to understand their robustness to point and structural defects. Through an indepth PL analysis it is demonstrated how different excitonic complexes (free, bound, and complex bound excitons) can serve as a probe to monitor the dilute limit of class II alloys. From an x-dependent linewidth analysis we extract the length scales at which excitons become increasingly localized, i.e., their conversion from a free to a bound particle upon alloy formation. Already at x ¼ 2.4% the exciton diffusion length is reduced to 5.7 AE 1.3 nm at a temperature of 12 K; hence, detrimental exciton transfer mechanisms toward nonradiative defects are suppressed. In addition, the associated low-temperature PL data suggest that a single indium atom cannot permanently capture an exciton. The low density of silicon impurities in our samples even allows studying their local indium-enriched environment at the scale of the exciton Bohr radius based on impurity bound excitons. The associated temperature-dependent PL data reveal an alloying dependence for the exciton-phonon coupling. Thus, the formation of the random alloy can not only be monitored by the emission of various excitonic complexes, but also more indirectly via the associated coupling(s) to the phonon bath. Micro-PL spectra even give access to a probing of silicon bound excitons embedded in a particular environment of indium atoms thanks to the emergence of a series of individual and energetically sharp emission lines (full width at half maximum ≈300 μeV). Consequently, the present study allows us to extract microscopic properties formerly mostly only accessible for class I alloys.

Disorder effects in nitride semiconductors: impact on fundamental and device properties

“…The indirect impact of nm-scale disorder can however be observed at the macroscopic level, through spatially averaged observations. For instance, the increase in emission linewidth compared with pure compounds reflects the variations in local composition, as does the absorption edge broadening [20].…”

Superfluorescence of Sub-Band States in C-Plane In0.1Ga0.9N/GaN Multiple-QWs

“…C-plane InGaN/GaN quantum wells (QWs) as the prevailing active layer have been studied extensively due to their promising applications in group-III nitride semiconductor optoelectronic devices [ 1 , 2 , 3 , 4 ]. Commonly accepted explanations for emission features are the spatial localization of carriers due to random alloy fluctuations, indium compositional fluctuations and well width fluctuations [ 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 ], the quantum-confined Stark effect (QCSE) because it spatially separates electron and hole wave functions and reduces the wave function overlap in the QWs [ 19 , 20 , 21 , 22 , 23 , 24 , 25 ] and the screening of the QCSE under a high excitation that affects the excitation density-dependent emission energy of InGaN/GaN MQWs, for example, a very strong emission from quantum-dot-like states [ 26 ], high energy emission band [ 27 , 28 , 29 ] and stimulated emission on the high-energy side in thick QWs [ 30 , 31 , 32 ].…”

Evidence of localization effect on photoelectron transport induced by alloy disorder in nitride semiconductor compounds

“…The effects of disorder on absorption [14,17,18] and recombination [19][20][21][22] in InGaN have been reported down to the intrinsic alloy disorder scale [23]. However, evidencing electron localization requires electron transport measurements as a function of temperature.…”