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arXiv:2006.07337 · Physical review. B./Physical review. B

Four-wave mixing dynamics of a strongly coupled quantum-dot–microcavity system driven by up to 20 photons

Daniel Groll, Daniel Wigger, Kevin Jürgens, Thilo Hahn, Christian Schneider, Martin Kamp, Sven Höfling, Jacek Kasprzak, T. Kühn

Published Jun 4, 2020• 13 citations
arXivHTMLPDF

Abstract

The Jaynes-Cummings (JC) model is at the heart of cavity QED and suitable to describe many different systems. Here, the authors use it to investigate a quantum dot strongly coupled to a micropillar cavity. Supported by experiments, they apply four-wave mixing spectroscopy to study the system's dynamics. They push the limits of JC physics by injecting up to $\ensuremath{\sim}20$ photons using ultrashort laser pulses. Starting with complicated dynamics, the signal evolves into a single-frequency oscillation monitoring the relaxation down the JC ladder.

DOI
10.1103/physrevb.101.245301

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The Jaynes-Cummings (JC) model is at the heart of cavity QED and suitable to describe many different systems. Here, the authors use it to investigate a quantum dot strongly coupled to a micropillar cavity. Supported by experiments, they apply four-wave mixing spectroscopy to study the system's dynamics. They push the limits of JC physics by injecting up to \ensuremath∼20\ensuremath{\sim}20\ensuremath∼20 photons using ultrashort laser pulses. Starting with complicated dynamics, the signal evolves into a single-frequency oscillation monitoring the relaxation down the JC ladder.
Light and matter can be unified under the strong coupling regime, creating superpositions of both, called dressed states or polaritons. After initially being demonstrated in bulk semiconductors and atomic systems ,strong coupling phenomena have been realized in solid state optical microcavities. They form an essential ingredient in the exciting physics spanning from many-body quantum coherence phenomena, like Bose-Einstein condensation and superfluidity, to cavity quantum electrodynamics (cQED). A widely used approach within cQED is the Jaynes-Cummings (JC) model that describes the interaction of a single fermionic two-level system with a single bosonic photon mode. For a photon number larger than one, known as quantum strong coupling (QSC), a significant anharmonicity is predicted for the ladder-like spectrum of dressed states. For optical transitions in semiconductor nanostructures, first signatures of the quantum strong coupling were recently published. In our latest report we applied advanced coherent nonlinear spectroscopy to explore a strongly coupled exciton-cavity system. Specifically, we measured and simulated its four-wave mixing (FWM) response, granting direct access to the first two rungs of the JC ladder. This paper summarizes the main results of Ref. 15 and adds FWM experiments obtained on a micropillar cavity in which a doublet of quantum dot (QD) excitons interacts with the cavity mode in the limit of weak to strong coupling.
We develop an exact analytical approach to four-wave mixing and higher-order optical nonlinearities of a quantum dot-microcavity system. This approach allows us \nto analyse the non-linear response in terms of coherent transitions between rungs \nof the Jaynes-Cummings ladder, finding their complex amplitudes and frequencies. \nIncreasing the pulse area of the excitation field, a transition from quantum strong \ncoupling to coherent classical regime is observed, which manifests itself in a formation of the famous Mollow triplet, with the observation in the three-level model \nof a quantum dot, including a biexciton, to predict two new effects: One is the \nexistence of a Mollow-like quintuplet, the other is a complete elimination of the \nfour-wave-mixing optical non-linearity under certain parameter constraints. We further develop a simple and accurate approximation in the low-damping limit of the \nJaynes-Cummings model of the quantum dot-microcavity system, for nonlinear response of any order in a closed analytic form, predicting the positions and widths \nof the spectral lines. For higher damping, we demonstrate a strong relaxation down \nthe ladder, shown by both numerical and analytic calculation.
Interaction between light and matter generates optical nonlinearities, which are particularly pronounced in the quantum strong coupling regime. When a single bosonic mode couples to a single fermionic mode, a Jaynes–Cummings (JC) ladder is formed, which we realize here using cavity photons and quantum dot excitons. We measure and model the coherent anharmonic response of this strongly coupled exciton–cavity system at resonance. Injecting two photons into the cavity, we demonstrate a larger polariton splitting with respect to the vacuum Rabi splitting. This is achieved using coherent nonlinear spectroscopy, specifically four-wave mixing, where the coherence between the ground state and the first (second) rung of the JC ladder can be interrogated for positive (negative) delays. With increasing excitation intensity and thus rising average number of injected photons, we observe spectral signatures of the quantum-to-classical crossover of the strong coupling regime.
The nonlinear optical response of an ensemble of semiconductor quantum dots is analyzed by wave-mixing processes, where we focus on four-wave mixing with two incident pulses. Wave-mixing experiments are often described with semiclassical models, where the light is modeled classically and the material quantum mechanically. Here, however, we use a fully quantized model, where the light is given by a quantum state of light. Quantum light involves more degrees of freedom than classical light as e.g., its photon statistics and quantum correlations, which is a promising resource for quantum devices, such as quantum memories. The light-matter interaction is treated with a Jaynes-Cummings type model and the quantum field is given by a single mode since the quantum dots are embedded in a microcavity. We present numerical simulations of the four-wave-mixing response of a homogeneous system for pulse sequences and find a significant dependence of the result on the photon statistics of the incident pulses. The model constitutes a problem with a large state space which arises from the frequency distribution of the transition energies of the inhomogeneously broadened quantum dot ensemble that is coupled with a quantum light mode. Here we approximate the dynamics by summing over individual quantum dot-microcavity systems. Photon echoes arising from the excitation with different quantum states of light are simulated and compared.
We measure the detuning-dependent dynamics of a quasiresonantly excited single quantum dot coupled to a micropillar cavity. The system is modeled with the dissipative Jaynes-Cummings model where all experimental parameters are determined by explicit measurements. We observe non-Markovian dynamics when the quantum dot is tuned into resonance with the cavity leading to a nonexponential decay in time. Excellent agreement between experiment and theory is observed with no free parameters providing the first quantitative description of an all-solid-state cavity QED system based on quantum dot emitters.