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Annalen der Physik

2D optical photon echo spectroscopy of a self‐assembled quantum dot

Benjamin Philipp Fingerhut, Marten Richter, Jun‐Wei Luo, Alex Zunger, Shaul Mukamel

Published Dec 28, 2012• 11 citations
Publisher

Abstract

Simulations of two dimensional coherent photon echo (2D‐PE) spectra of self‐assembled InAs/GaAs quantum dots (QD) in different charged states are presented revealing the coupling between the individual mono‐exciton transitions and contributions of bi‐excitons . The information about the states is crucial for various application scenarios of QDs, like e.g. highly efficient solar cells. The simulations rely on a microscopic description of the electronic structure by high‐level atomistic many‐body pseudopotential calculations. It is shown that asymmetric diagonal peak shapes and double cross‐peaks are the result of state contributions to the PE signal by analyzing the contributions of the individual pathways excited state emission, ground state bleach and excited state absorption. The results show that from the detuned and contributions the bi‐exciton binding energies of the manifold are revealed in 2D‐PE signals.

DOI
10.1002/andp.201200204

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Simulations of two dimensional coherent photon echo (2D‐PE) spectra of self‐assembled InAs/GaAs quantum dots (QD) in different charged states are presented revealing the coupling between the individual mono‐exciton transitions and contributions of bi‐excitons . The information about the states is crucial for various application scenarios of QDs, like e.g. highly efficient solar cells. The simulations rely on a microscopic description of the electronic structure by high‐level atomistic many‐body pseudopotential calculations. It is shown that asymmetric diagonal peak shapes and double cross‐peaks are the result of state contributions to the PE signal by analyzing the contributions of the individual pathways excited state emission, ground state bleach and excited state absorption. The results show that from the detuned and contributions the bi‐exciton binding energies of the manifold are revealed in 2D‐PE signals.
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)
We investigate the dephasing mechanism of optically-induced exciton coherence in an ensemble of InAs self-assembled quantum dots (QDs) using a two-pulse photon-echo (PE) technique. The sample was fabricated on an InP (311)B substrate using strain compensation to control the emission wavelength. This technique also enabled us to fabricate a 150-layer stacked QD structure for enhancing the PE signal intensity. We show the measured decay time of PE signal intensity for resonant excitation of ground-state transition is extremely long, which corresponds to ultralong coherence times of excitons in our QDs. We confirmed that non-radiative population relaxation and pure dephasing are considerably smaller than the radiative relaxation at low temperature. Furthermore, we demonstrate the ultrafast coherent control of QD exciton polarization by changing the pulse areas (Rabi oscillations) in the PE experiment. We also propose a new scheme for implementing QD quantum memory by using the PE technique.
We study the photon echo spectrum of self-assembled semiconductor quantum dots using femtosecond light pulses. The spectrum shape changes from a single-peaked to a double-peaked structure as the time delay between the two excitation pulses is increased. The spectrum change is reproduced by numerical calculations, which include the depolarization field induced by the biexciton-exciton transition as well as the conventional local-field effect for the exciton--ground-state transition in a quantum dot. Our findings suggest that various optical transitions in tightly localized systems generate a depolarization field, which renormalizes the resonant frequency with a change in the polarization itself, leading to unique optical properties.
We report photon correlation measurements that reveal unique signatures of biexciton and charged exciton emissions in a single self-assembled InAs quantum dot. Biexciton emission exhibits both bunching and antibunching under continuous-wave excitation and only antibunching under pulsed excitation. Cross correlation between biexciton and single-exciton emissions reveals highly asymmetric features due to cascaded emission. Under our excitation conditions, no polarization correlations between the exciton and biexciton emissions were observed.
Abstract Techniques for coherent multidimensional optical spectroscopy have been developed and utilised to understand many different processes, including energy transfer in photosynthesis and many‐body effects in semiconductor nanostructures. Double‐quantum 2D spectroscopy is one variation that has been particularly useful for understanding many‐body effects. In condensed matter systems, however, there are often many competing signal pathways, which can make it difficult to isolate different contributions and retrieve quantitative information. Here, a means of separating overlapping pathways while maintaining the fidelity of the relevant peak/s is demonstrated. This selective approach is used to isolate the double‐quantum signal from a mixed two exciton state in a semiconductor quantum well. The removal of overlapping peaks allows analysis of the relevant peak‐shape and thus details of interactions with the environment and other carriers to be revealed. An alternative pulse ordering identifies a double‐quantum state associated only with GaAs defects, the signature of which has previously been confused with other interaction induced effects. The experimental approach described here provides access to otherwise hidden details of excitonic interactions and demonstrates that the manner in which the double‐quantum coherence is generated can be important and provide an additional control to help understand the many‐body physics in complex systems. image