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Nonlinear spectral hole-burning of the intraband transition at 1.55 μm in GaN/AlN quantum dots

D. T. Nguyen, Maria Tchernycheva, François Henri Julien, Eva Monroy, Bernard Gil, Guillaume Cassabois

Published Oct 15, 2012• 0 citations
OpenAlex

Abstract

GaN/AlN quantum dots are semiconductor nanostructures where the huge conduction band offset of 1.75 eV leads to intraband transitions at exceptionnaly short wavelengths compared to III-As semiconductor materials. For specific quantum dot dimensions, it was shown that the absorption spectrum covers the optical communication spectral range. The ultrafast relaxation dynamics observed for these materials motivates the development of opto-electronic devices, and especially ultrafast switches. However, a detailed insight into the microscopic processes governing the relaxation dynamics is still missing although of fundamental importance for the understanding and the optimization of the devices operation. In particular, there is no study of the homogeneous broadening which drives the saturation properties of GaN/AlN quantum dots-devices. In this paper, we present homogeneous linewidth measurements by means of the nonlinear optical technique of spectral hole-burning. Spectrally-resolved pump-probe experiments with cw-lasers allow us to characterize the coherence relaxation dynamics down to 5K by resolving the homogeneous linewidth in an ensemble of GaN/AlN quantum dots. The differential transmission measured at 5K for a TM-polarized pump shows a pronounced bleaching with an amplitude of 2x10-4 on a background signal of 5x10-5. According to the selection rules of the s-pz intraband transition in GaN/AlN QDs, we attribute the photoinduced increase of the probe transmission to the partial saturation of the quantum dots by the pump laser, and we deduce a homogeneous linewidth of 15 meV at 5K. We find that the differential transmission signal scales like the square-root of the incident pump power, thus revealing the importance of electron-electron scattering in the population relaxation dynamics. As a matter of fact, we find that the population relaxation from the pz excited state is predominantly governed by Auger-type processes whereas optical phonon emission only plays a minor role, even if it may contribute to secondary processes during the carrier cascade to the fundamental s state via intermediate confined states.

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Applied Physics Letters•Feb 6, 2006•26 citations
GaN/AlN quantum dots are semiconductor nanostructures where the huge conduction band offset of 1.75 eV leads to intraband transitions at exceptionnaly short wavelengths compared to III-As semiconductor materials. For specific quantum dot dimensions, it was shown that the absorption spectrum covers the optical communication spectral range. The ultrafast relaxation dynamics observed for these materials motivates the development of opto-electronic devices, and especially ultrafast switches. However, a detailed insight into the microscopic processes governing the relaxation dynamics is still missing although of fundamental importance for the understanding and the optimization of the devices operation. In particular, there is no study of the homogeneous broadening which drives the saturation properties of GaN/AlN quantum dots-devices. In this paper, we present homogeneous linewidth measurements by means of the nonlinear optical technique of spectral hole-burning. Spectrally-resolved pump-probe experiments with cw-lasers allow us to characterize the coherence relaxation dynamics down to 5K by resolving the homogeneous linewidth in an ensemble of GaN/AlN quantum dots. The differential transmission measured at 5K for a TM-polarized pump shows a pronounced bleaching with an amplitude of 2x10-4 on a background signal of 5x10-5. According to the selection rules of the s-pz intraband transition in GaN/AlN QDs, we attribute the photoinduced increase of the probe transmission to the partial saturation of the quantum dots by the pump laser, and we deduce a homogeneous linewidth of 15 meV at 5K. We find that the differential transmission signal scales like the square-root of the incident pump power, thus revealing the importance of electron-electron scattering in the population relaxation dynamics. As a matter of fact, we find that the population relaxation from the pz excited state is predominantly governed by Auger-type processes whereas optical phonon emission only plays a minor role, even if it may contribute to secondary processes during the carrier cascade to the fundamental s state via intermediate confined states.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
This study explores the potential for coherent control of the quantum state of quantum confined InGaN nanostructures, known for large exciton binding energies, using optical fields for future applications such as quantum information processing up to room temperature. Here we specifically report on the coherent nonlinear optical spectrum of InGaN disks grown in GaN nanowires at both cryogenic temperatures and room temperature. Two different samples are featured in this study: a self-assembled nanowire sample grown on a silicon substrate and a selective area sample grown on GaN/sapphire. Self-assembled DINWs grown on silicon are important for on-chip silicon photonics applications, however the morphological properties of the nanowires are much more difficult to control compared to selective area samples. Using frequency domain nonlinear spectroscopy methods, we find resonances in an ensemble of self-assembled InGaN disks in GaN nanowires that persist without significant broadening up to room temperature that we assign to quantum-confined excitons. Furthermore, the nonlinear optical spectrum as a function of excitation frequency depends only on the disorder state dominated photoluminescence excitation spectrum. Under these growth conditions, we find that the kinetics are dominated by metastable traps with strongly temperature dependent lifetimes corresponding to an activation energy between 5 and 12 meV. The metastable traps are mostly likely formed due to the coalescence of multiple nanowires during growth. The selective area sample is grown free of nanowire coalescence; therefore we do not observe effects from metastable states in the system. The nonlinear optical spectrum in the selective area shows some evidence of spectral hole burning from exciton states without significant additional broadening at room temperature, where the spectral holes have homogeneous linewidths ~20-30 meV at both low temperature and room temperature corresponding to ultrafast decoherence processes. The ultrafast decoherence could be associated with fast electron-hole transfer within a large density of background disorder states that is observed in the nondegenerate nonlinear absorption spectrum. In summary, although the samples show evidence of excitons with high temperature stability, the presence of material disorder and metastable trap states severely limits the use of InGaN disks-in-nanowires for coherent control applications without further material engineering.
Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.
Persistent spectral-hole-burning (PSHB) phenomena have been observed in many kinds of semiconductor quantum dots (QDs). Luminescence hole burning and charged excitons have been observed in CuCl QDs in NaCl crystals. The observed PSHB phenomena are explained by the ionization of QDs. The energy of photoionized QDs is changed from the original energy and their new energies depend on the spatial arrangement of trapped carriers. Quantum confinement of carriers and the resulting strong Coulomb interaction between confined carriers and trapped carriers cause the energy change. PSHB has been widely applied to site-selective spectroscopy of QDs. Size-dependent excited exciton quantum states in CuCl quantum cubes, size-dependent excited electron-hole quantum states in CdTe QDs and renormalization of longitudinal optical phonons confined in CuCl QDs have been revealed by studying sideband holes. This also allowed the measurement of accumulated photon echo, which clarified the very sharp homogeneous spectral linewidth of QDs under weak excitation conditions.
We study CuBr nanocrystals embedded in a borosilicate matrix. The excitonic absorption line is strongly inhomogeneously broadened by the size dispersion of the quantum dots. We explore two ways in order to study the dephasing processes of the transition. The homogeneous absorption linewidth is first determined by spectral hole-burning (SHB) measurements, using a nanosecond dye laser excitation. We then perform degenerate four-wave-mixing experiments (FWM), using 100 fs pulses from a frequency-doubled Ti:sapphire laser. Due to the inhomogeneous broadening, we observe a so-called photon-echo signal and we measure its dynamics. From SHB experiments, we obtain homogeneous linewidths larger than 0.3 meV. From the FWM experiment, we obtain values smaller than 0.2 meV. These discrepancies between SHB and FWM measurements can be explained if we take into account the high excitation intensity necessary to induce absorption saturation in SHB experiments. Moreover, during the 20 ns pulses used, spectral diffusion may occur due to interactions between the nanocrystals and their matrix. Spectrally resolved four-wave-mixing experiments (SR-FWM) are also performed. The oscillations with a 250 fs period we observe at short time delays could be interpreted in terms of quantum beats between two-exciton and one-exciton states.
We report the use of continuous wave spectral hole burning to perform high-resolution spectroscopy of the homogeneous linewidth of self-assembled InGaAs-GaAs quantum dots at low temperature. We use this technique to examine the power broadening behavior of the homogeneous InGaAs-GaAs quantum dot line. We find that at a temperature of 9.8 K and over the majority of the pump powers considered, the spectral hole signal is well fit by a single Lorentizian line shape. Analysis of the power broadening yields a full width at half maximum of 0.74μeV for the homogeneous linewidth and a corresponding coherence time T2 of 1.76 ns.