A detailed analysis of the radiative recombination processes in CuxGaySe2 epitaxial layers is presented aiming at an investigation of the intrinsic defect levels as a function of chemical composition. CuxGaySe2 is grown by metalorganic vapor phase epitaxy to allow a precise control of composition. Temperature and excitation intensity dependent photoluminescence is used to identify different recombination mechanisms and to determine the ionization energies of the defect levels involved. Defect-correlated optical transitions in Cu-rich epilayers are described in a recombination model consisting of two acceptor and one donor levels showing ionization energies of (60±10) meV, (100±10) meV, and (12±5) meV, respectively. The identification of a shallow compensating donor in CuxGaySe2 and the assignment of the 100 meV state to an acceptor are the most important new aspects in this model. Photoluminescence properties of layers showing Ga-rich compositions are discussed in a model of highly doped and highly compensated semiconductors—the model of fluctuating potentials.
We present experimental results concerning optical transitions and carrier dynamics (capture and relaxation) in self assembled InAs/GaAs quantum dot structures grown by metalorganic vapor phase epitaxy. Photoluminescence (PL) measurements at high excitation level reveal optical transitions above the ground state emission. These transitions are found to originate from occupied hole states by solving the quantum dot eigenvalue problem. Time-resolved studies after non-resonant pulse excitation exhibit a relaxation ladder of the excited carriers from the GaAs barrier down to the ground state of the quantum dots. From both the continuous-wave measurements and the PL-decay curves we conclude that the carrier relaxation at non-resonant excitation is mediated by Coulomb interaction (Auger effect). PL-decay curves after resonant pulse excitation reveal a longer rise time compared to non-resonant excitation which is a clear indication of a relaxation bottleneck inside the quantum dots. We interpret the rise time (≊ 400 ps) in this case to originate from relaxation via scattering by acoustic phonons. The PL-decay time of the ground state emission ≊700 ps is interpreted as the excitonic lifetime of the quantum dot.
Excitonic line spectra from CuGaSe2 single crystals and epitaxial layers are investigated as a function of temperature. Near band edge luminescence from free and bound excitons is observed at 10 K. The identification of both, free exciton ground and first excited state allows to determine the free exciton binding energy, which is found to be (13±2) meV. The bound exciton line is attributed to the recombination of an exciton bound to a neutral acceptor (A0, X). The widely discussed phenomenon of an anomalous temperature dependence of the band gap energies in different chalcopyrite-type I-III-VI2 compounds is reconsidered for CuGaSe2 on the basis of temperature dependent photoluminescence studies. No anomalous behaviour of the band gap energy as a function of temperature is found in CuGaSe2.
The energy structure and the carrier relaxation in self-assembled InAs/GaAs quantum dots (SADs) is investigated by photoluminescence excitation spectroscopy (PLE) and photoluminescence (PL) at resonant excitation (below the GaAs and the wetting layer bandgap). In PLE measurements we find a clear resonance from the first excited hole state as well as resonances from a relaxation via different phonons. From a comparison of the PL-rise times in time resolved spectroscopy, we conclude on a fast electron relaxation (⩽50 ps) and a slow hole relaxation with a time constant of about 400 ps. Different relaxation paths are observed in the InAs/GaAs quantum dot system and allow us to identify the hole relaxation in the SADs as multiphonon assisted tunneling. The PL-decay time in the SADs after resonant excitation (about 600 ps) is attributed to the lifetime of the quantum dot exciton. In agreement with theoretical predictions, we find a constant lifetime of about 600 ps for temperatures below 50 K and a linear increase of the lifetime between 50 and 100 K with a slope of 26 ps/K.
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