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Applied Physics Letters

Two-photon spectral hole burning spectroscopy of InAs/GaAs quantum dots

Thomas Moldaschl, Wolfgang Parz, Thomas G. Muller, Sebastian Golka, G. Strasser, K. Unterrainer

Published Jul 5, 2010• 1 citation
Publisher

Abstract

Femtosecond spectral hole burning experiments were performed on InAs/GaAs quantum dots to investigate the influence of high excitation intensities. The observation of additional spectral holes, as well as distinct absorption line broadening are both attributed to two-photon absorption processes. These spectral holes can be unambiguously assigned to degenerate two-photon biexciton creation, whereas the absorption line broadening is a direct result of Coulomb renormalization, initiated by carriers created through two-photon absorption in the surrounding GaAs crystal matrix and the InAs wetting layer.

DOI
10.1063/1.3460527

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Femtosecond spectral hole burning experiments were performed on InAs/GaAs quantum dots to investigate the influence of high excitation intensities. The observation of additional spectral holes, as well as distinct absorption line broadening are both attributed to two-photon absorption processes. These spectral holes can be unambiguously assigned to degenerate two-photon biexciton creation, whereas the absorption line broadening is a direct result of Coulomb renormalization, initiated by carriers created through two-photon absorption in the surrounding GaAs crystal matrix and the InAs wetting layer.
The biexciton absorption spectrum of a pair of InAs/GaAs quantum dots is being studied by photoluminescence excitation spectroscopy. An absorption resonance with the characteristics of an instantaneous two-photon process reveals a coherent interdot two-photon transition. Pauli-selective tunneling is being used to demonstrate the transduction of the two-photon coherence into a nonlocal spin singlet state. The two-photon transition can be tuned spectrally by electric field, enabling amplification of its transition strength.
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 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.
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.
Abstract In this work femtosecond spectral hole burning spectroscopy is used to resonantly excite ground state excitons in an ensemble of self‐assembled InAs/GaAs quantum dots with a strong pump pulse. Two fundamental coherent nonlinear effects are observed with the aid of the intrinsic time‐ and frequency resolution of the setup: The low temperature Rabi oscillation of the two‐level system associated with the excitonic ground state transition and the observation of two‐photon absorption in the surrounding GaAs crystal matrix. The emergence of the latter effect also infers the existence of charged excitons in the nominally undoped QD sample, backed up by the observation of additional spectral holes next to the excitonic transitions. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)