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arXiv:1704.03290 · Physical review. B./Physical review. B

Exploring coherence of individual excitons in InAs quantum dots embedded in natural photonic defects: Influence of the excitation intensity

Daniel Wigger, Quentin Mermillod, Tomasz Jakubczyk, F. Fras, Simon Le Denmat, Doris E. Reiter, Sven Höfling, Martin Kamp, Gilles Nogues, Christian Schneider, T. Kühn, Jacek Kasprzak

Published Oct 24, 2017• 12 citations
arXivHTMLPDF

Abstract

The exact optical response of quantum few-level systems depends crucially on the exact choice of the incoming pulse areas. We use four-wave mixing (FWM) spectroscopy to infer the coherent response and dynamics of single InAs quantum dots (QDs) and study their pulse area dependence. By combining atomic force microscopy with FWM hyperspectral imaging, we show that the retrieved FWM signals originate from individual QDs enclosed in natural photonic defects. The optimized light-matter coupling in these defects allows us to perform our studies in a wide range of driving field amplitudes. When varying the pulse areas of the exciting laser pulses, Rabi rotations of microscopic interband coherences can be resolved by the two-pulse FWM technique. We investigate these Rabi coherence rotations within two- and three-level systems, both theoretically and experimentally, and explain their damping by the coupling to acoustic phonons. To highlight the importance of the pulse area influence, we show that the phonon-induced dephasing of QD excitons depends on the pulse intensity.

DOI
10.1103/physrevb.96.165311

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A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.
While the advanced coherent control of qubits is now routinely carried out in low frequency (GHz) systems like single spins, it is far more challenging to achieve for two-level systems in the optical domain. This is because the latter evolve typically in the THz range, calling for tools of ultrafast, coherent, nonlinear optics. Using four-wave mixing micro-spectroscopy, we here measure the optically driven dynamics of a single exciton quantum state confined in a semiconductor quantum dot. In a combined experimental and theoretical approach, we reveal the intrinsic Rabi oscillation dynamics by monitoring both central exciton quantities, i.e., its occupation and the microscopic coherence, as resolved by the four-wave mixing technique. In the frequency domain this oscillation generates the Autler-Townes splitting of the light-exciton dressed states, directly seen in the four-wave mixing spectra. We further demonstrate that the coupling to acoustic phonons strongly influences the FWM dynamics on the picosecond timescale, because it leads to transitions between the dressed states.
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We employ two-dimensional (2D) coherent, nonlinear spectroscopy to investigate couplings within individual InAs quantum dots (QDs) and QD molecules. Swapping pulse ordering in a two-beam sequence permits one to distinguish between rephasing and nonrephasing four-wave mixing (FWM) configurations. We emphasize the nonrephasing case, allowing one to monitor two-photon coherence dynamics. Respective Fourier transform yields a double quantum 2D FWM map, which is corroborated with its single quantum counterpart, originating from the rephasing sequence. We introduce referencing of the FWM phase with the one carried by the driving pulses, overcoming the necessity of its active stabilization, as required in 2D spectroscopy. Combining single and double quantum 2D FWM provides a pertinent tool in detecting and ascertaining coherent coupling mechanisms between individual quantum systems, as exemplified experimentally.